<<

THE ROLE OF ABCG5/G8 IN STEROL HOMEOSTASIS

BY

ALLISON L. MCDANIEL

A Dissertation submitted to the Graduate Faculty of

WAKE FOREST UNIVERSITY GRADUATE SCHOOL OF ARTS AND SCIENCES

in Partial Fulfillment of the Requirements

for the Degree of

DOCTOR OF PHILOSOPHY

Molecular and Cellular Pathology

May 2013

Winston-Salem, NC

Approved by:

Ryan E. Temel, Ph.D., Advisor

Richard Weinberg, M.D., Chair

Lawrence L. Rudel, Ph.D.

John S. Parks, Ph.D.

Gregory Shelness, Ph.D.

TABLE OF CONTENTS

LIST OF FIGURES………………………………………………………….…….……iii

LIST OF TABLES…………………………………………………………..…………...v

LIST OF ABBREVIATIONS………………………………………………...... …….…vi

ABSTRACT……………………………………………………………...……….….…viii

CHAPTER

I. INTRODUCTION………………………………………………………..….1

II. PHYTOSTEROL FEEDING CAUSES TOXICITY IN ABCG5/G8

KNOCKOUT MICE…………………………….………………….…..…..22

III. HEPATIC ABCG8 KNOCKDOWN DOES NOT RESULT IN HIGH

LEVELS OF PHYTOSTEROL ACCUMULATION……………….....….56

IV. HEPATIC ABCG8 KNOCKDOWN PREVENTS LXR AGONIST

INDUCED REVERSE TRANSPORT…………...... 103

V. DISCUSSION…………………………………………..……………..…133

CIRRICULUM VITAE………………………………………………..…………..….145

ii

LIST OF FIGURES

CHAPTER I

Figure 1: Structures of cholesterol and two common phytosterols…...... 7

CHAPTER II

S. Figure 1: Bodyweight measurement………………………...... …32

Figure 1: Measurement of body and tissues weights…...... ………33

Figure 2: Assessment of liver pathology……………...... …………35

Figure 3: Tissue sterol concentrations……………...... …………..39

Figure 4: Plasma characterization…………...... ………………….41

Figure 5: Cardiac histology…………………...... ………………….44

CHAPTER III

S. Figure I: Dietary sterol content and composition……………...... ……….…68

Figure 1: ABCG8 and ABCG5 expression……………….…...... …………...70

Figure 2: Biliary cholesterol concentration……………………..………….…74

S. Figure II: Biliary composition………………………….……….………...75

iii

S. Figure III: Body and liver weights of CON and G8HKD mice……….....……….77

Figure 3: Plasma sterol concentrations………………………………...... …….79

S. Figure IV: Plasma sterol distributions……………………...... ……82

Figure 4: Liver sterol concentrations………………………………...... ……….85

Figure 5: Fecal neutral sterol excretion……………………………...... …….89

S. Figure V: Liver sterol concentrations after 12 weeks of G8HKD and high

phytosterol diet feeding………………………………...... …………..92

CHAPTER IV

Figure 1: ABCG8 and ABCG5 expression…………...... ……………….…115

Figure 2: Biliary sterol concentrations…………………………...... …118

Figure 3: Plasma sterol mass and radioactivity……………...... ……….120

Figure 4: Liver sterol mass and radioactivity………………………...... …122

Figure 5: Fecal neutral sterol mass and radioactivity…………...... ………124

iv

LIST OF TABLES

CHAPTER II

Table 1: RT-PCR primers……………………...... …….……….29

S. Table 1: Dietary sterol compositions…………...... ……...……..32

Table 2: Hepatic and splenic expression……...... ……….37

CHAPTER III

S. Table I: Diet ingredients………………………………...... ……..67

v

LIST OF ABBREVIATIONS

ABCA1 – ATP-Binding Cassette Transporter A1

ABCB11 – ATP-Binding Cassette Transporter B11

ABCG1 – ATP-Binding Cassette Transporter G1

ABCG5 – ATP-Binding Cassette Transporter G5

ABCG8 – ATP-Binding Cassette Transporter G8

ACAT2 – Acyl-CoA:Cholesterol O-Acyltransferase 2

BLVRA – Biliverdin Reductase A

CD68 – Cluster of Differentiation 68

CHD – Coronary Heart Disease

CYP7A1 – Cholesterol 7α-hydroxylase

HDL – High Density Lipoprotein

HMGCS – Hydroxy-Methylglutaryl CoA Synthase

HO-1 – Hemeoxygenase 1

IL-6 – Interleukin 6

KO – Knockout

LDL – Low Density Lipoprotein

LXR –

NAFLD – Non Alcoholic Fatty Liver Disease

PLTP – Phospholipid Transfer

RCT – Reverse Cholesterol Transport

RXR – Retinoid X Receptor

vi

SCD1 – Stearoyl-CoA Desaturase-1

SR-BI – Scavenger Receptor Class B Type I

SREBP1C – Sterol Regulatory Element Binding Protein 1C

TICE – Trans Intestinal Cholesterol Excretion

UGT1a – Diphosphoglucuronate Glucuronosyltransferase 1A

WT – Wild Type

vii

ABSTRACT

Allison L. McDaniel, BS, BA

THE ROLE OF ABCG5/G8 IN STEROL HOMEOSTASIS

Dissertation under the direction of

Ryan E. Temel, Ph.D., Assistant Professor of Pathology – Lipid Sciences

ATP-binding cassette transporters G5 and G8 (ABCG5/G8) excrete excess phytosterols and cholesterol from the body, thus playing a crucial role in sterol metabolism and whole body sterol homeostasis. The significance of phytosterol exclusion from the body is still unknown. Furthermore, there is evidence that

ABCG5/G8 plays slightly different roles in sterol metabolism in the liver and small intestine. The goal of these studies is to define the tissue-specific role of

ABCG5/G8 in whole body sterol homeostasis and to determine the significance of phytosterol exclusion from the body.

The first aim was to determine the significance of phytosterol exclusion from the

body. Wild-type and ABCG5/G8 knockout mice were fed a phytosterol-enriched

diet. The high-phytosterol diet was extremely toxic to the ABCG5/G8 knockout

mice but had no adverse effects on wild-type mice. ABCG5/G8 knockout mice died prematurely and developed a phenotype that included high levels of plant

viii sterols in many tissues, liver abnormalities, and severe cardiac lesions. These data show that plant sterols are excluded from the body because they are toxic when present at high levels.

The second aim was to determine whether hepatic ABCG5/G8 function is required for phytosterol exclusion from the plasma and tissues of mice. An anti- sense oligonucleotide (ASO) targeted to ABCG8 was used to knock down

ABCG8 expression in the liver of C57Bl/6 mice. Mice with hepatic ABCG8 knockdown did not accumulate high levels of phytosterols but did appear to have alterated hepatic cholesterol metabolism.

The third aim was to determine whether hepatic ABCG5/G8 function is necessary for LXR agonist mediated increases in cholesterol excretion and macrophage reverse cholesterol transport. An ABCG8 ASO was used to knock down ABCG8 expression in the liver of C57Bl/6 mice and RCT was measured. When mice had decreased hepatic ABCG8 expression, cholesterol excretion and macrophage

RCT were not stimulated with LXR agonist treatment. These data suggest that

ABCG5/G8, a downstream target of LXR, is required for LXR stimulated increases in cholesterol excretion and macrophage RCT.

Together, these studies show that the role of ABCG5/G8 in sterol metabolism and homeostasis is complex and has not been completely discovered.

ix

CHAPTER I

INTRODUCTION

Coronary heart disease (CHD) is the leading cause of death in the United States.

Approximately every 34 seconds, one American will have a coronary event, and

approximately every minute, one American will die of one1. In addition to mortality

and decreased quality of life for those affected, CHD brings a significant public

and private financial burden. For 2009, it was estimated that the total direct and

indirect cost of cardiovascular disease reached $312.6 billion dollars1, making it

the most costly disease in the United States.

One of the most popular drugs used in the treatment of CHD is statins. Statins

lower low density lipoprotein cholesterol (LDL-c) levels by inhibiting endogenous

cholesterol synthesis. It has long been observed that the strongest risk factors

that predict CHD are increased LDL-c and decreased high density lipoprotein

cholesterol (HDL-c) levels2. The widely used LDL-c lowering statins have, indeed,

reduced CHD events and mortality. Despite their successes, they have only

reduced CHD mortality by approximately 30%3, which still leaves a significant

CHD burden.

Since decreased HDL-c levels are also a strong predictor of CHD, much

emphasis has been placed on HDL metabolism research. Developing treatment

1

options that utilize the beneficial properties of HDL could be a powerful tool in battling CHD. Many mechanisms have been proposed to explain how HDL could decrease the formation of atherosclerosis4-6. The most widely accepted

mechanism is HDL driven reverse cholesterol transport (RCT).

RCT plays an important role in maintaining whole body cholesterol homeostasis.

It is undeniable that cholesterol is vital to the maintenance and function of many

biological processes. For example, cholesterol is an important component of

cellular membranes, can act as a signalling molecule, and serves as a precursor

for steroid hormones and bile acids. Too much bodily cholesterol accumulation

can, however, become detrimental. Cholesterol homeostasis is a delicate

balance between dietary cholesterol absorption, endogenous cholesterol

synthesis, cholesterol utilized for biological processes, and cholesterol excretion

from the body. Imbalances in cholesterol homeostasis that result in net

cholesterol accumulation can lead to diseases like atherosclerosis and non-

alcoholic fatty liver disease (NAFLD). For this reason, the body has complex

regulatory systems to help maintain correct sterol balance.

One part of this regulatory system is RCT. RCT is the movement of cholesterol

from peripheral tissues to the liver. In this process, cholesterol is effluxed from

the peripheral tissues onto HDL particles via ATP-binding cassette transporters

A1 (ABCA1) and G1 (ABCG1)7, 8. The HDL particles travel through the plasma compartment to the liver, where they offload the cholesterol by scavenger

2

receptor class B type I (SR-BI) mediated selective cholesterol uptake 9, 10. Once cholesterol reaches the liver it can be incorporated into membranes, converted into bile acids, esterified for storage, or secreted into the bile. The primary way for hepatic cholesterol to exit the body is through direct secretion into bile followed by fecal excretion. Because of its contributing role to cholesterol excretion from the body, RCT undoubtedly plays an important part in maintaining cholesterol homeostasis. Because increasing cholesterol excretion via RCT is an attractive therapeutic target for CHD treatment, it is important to study and understand the RCT pathway.

In order for biliary cholesterol to reach the small intestine for excretion, it must first be secreted into the bile. Two of the critical that regulate this process are ATP-binding cassette transporter G5 (ABCG5) and ATP-binding cassette transporter G8 (ABCG8). Together, ABCG5 and ABCG8 (ABCG5/G8) make up a membrane bound heterodimer that is primarily expressed in the liver and small intestine. Both ABCG5 and ABCG8 must be expressed in order for the

proteins to be trafficked to the cell surface11, 12. Once at the cell surface,

ABCG5/G8 flops sterols from the inner leaflet to the outer leaflet of the canalicular membrane13. The canalicular membrane can then secrete

cholesterol-containing vesicles from the outer leaflet into bile14, 15.

Several mouse studies have demonstrated that altering ABCG5/G8 expression

affects biliary cholesterol levels. Yu L et al.16 first showed that ABCG5/G8

3

knockout (KO) mice had a 90% reduction in biliary cholesterol concentrations

when compared to wild type (WT) mice. Additional studies revealed that

overexpression of ABCG5/G8 caused increases to biliary cholesterol

concentrations17, and that biliary cholesterol concentrations correlate to the

relative amount of ABCG5/G8 expression18. Studies conducted in ABCG5 KO19,

20 and ABCG8 KO21 mice also show significant reductions in biliary cholesterol

concentrations, further confirming that expression of both is required for

biliary cholesterol secretion.

Mouse studies using dietary cholesterol and synthetic compounds to increase

ABCG5/G8 expression have also resulted in biliary cholesterol changes. The

gene cluster for ABCG5 and ABCG8 is a direct target of the oxysterol-activated

nuclear receptors Liver X Receptor (LXR) alpha and LXR beta. When fed a high

cholesterol diet, hepatic and small intestinal ABCG5/G8 mRNA levels were

significantly increased22. Administration of synthetic ligands of LXR and its

heterodimeric partner, retinoid X receptor (RXR), also caused significant

increases in hepatic and small intestinal ABCG5/G8 mRNA levels23.

Furthermore, treatment with an LXR agonist was shown to significantly increase biliary cholesterol concentrations in mice24, and these increases in biliary cholesterol concentrations required the presence of ABCG5/G825. These

comprehensive studies firmly establish the critical function of ABCG5/G8 in biliary cholesterol secretion and, therefore, the important role of ABCG5/G8 in biliary fecal sterol loss and RCT.

4

Since ABCG5/G8 is critical for cholesterol movement from the liver into the bile, it

follows that ABCG5/G8 likely plays a role in hepatic cholesterol homeostasis and

metabolism. This does appear to be the case, as several groups have reported

changes in hepatic cholesterol metabolism when ABCG5/G8 is absent26, 27. For example, on low cholesterol diets ABCG5/G8 KO mice have significant reductions in plasma and hepatic cholesterol concentrations28-30. Despite these

reductions, there are no compensatory increases in cholesterol synthesis genes.

Hepatic mRNA levels of HMG-CoA synthase and reductase are actually reduced

by 50% in ABCG5/G8 KO mice. Drawing conclusions from these studies about

the role of ABCG5/G8 in hepatic cholesterol metabolism is difficult, however,

since ABCG5/G8 deficiency causes significant plant sterol (or phytosterol)

accumulation.

The importance of ABCG5/G8 in preventing phytosterol absorption was actually

discovered prior to its role in biliary cholesterol secretion. In 1974, Bhattacharyya

and Connor described a new lipid storage disease, termed , in two

sisters with plant sterol accumulation in blood and tissues31. Patients with

sitosterolemia accumulate plant sterols in many tissues and often present with

tendinous and cutaneous xanthomas and hypersterolemia32, 33. There are also

indications that plasma plant sterol accumulation has negative effects on platelet

biology34. Subsequent work identified genetic mutations to ABCG5 and ABCG8

as the cause of sitosterolemia35-37.

5

It has long been observed that although a typical diet generally contains similar

amounts of cholesterol and phytosterols, intestinal cholesterol absorption rates

are 40% to 60%, but phytosterols are mostly excluded from the body due to

intestinal absorption rates of less than 5%38, 39. When ABCG5/G8 is disrupted,

however, dietary phytosterols are hyper absorbed by the small intestine. Patients

who lack functional ABCG5/G8 absorb 20-30% of phytosterols from the small

intestinal lumen40, 41. Mouse models with ABCG5 and/or ABCG8 disruption display a phenotype similar to human sitosterolemia patients. There are subtle differences among the mouse models, but all have significant accumulation of plant sterols in plasma and tissues19, 20, 42-45.

The need for discrimination between plant sterols and cholesterol is not fully

understood. The discrimination against phytosterols has a basis in chemical

structure. Phytosterols and cholesterol both have the tetracyclic structure and 3β-

hydroxyl group which are characteristic of sterols. They differ from each other in

the position and number of double bonds and additional alkyl side chains. These

subtle structural differences between phytosterols and cholesterol result in

differential processing by mammalian systems. For example, campesterol, with a

single-carbon side chain at carbon 24, typically has a plasma concentration 500

times less than cholesterol; whereas, the concentration of sitosterol, with a 2-

carbon side chain at carbon 24, is about 20,000 times lower than cholesterol46.

Although they have limited absorption, phytosterols can still participate in a number of biological functions by acting as a cholesterol absorption inhibitor47, 48,

6 an antioxidant49, an anticarcinogen50, and an immune system regulator51. When hyper absorbed, phytosterols can potentially alter many more biological functions.

Figure 1. Structures of cholesterol and two common phytosterols

As previously mentioned, hepatic cholesterol metabolism is altered when phytosterols accumulate in ABCG5/G8 KO mice. It is not completely clear, however, how much of the changes in cholesterol metabolism are due to the mass accumulation of plant sterols versus the lack of ABCG5/G8 function. It is possible that the complete role of ABCG5/G8 in cholesterol metabolism is partly masked by the accumulation of plant sterols. Interestingly, a study was published in 2012 by Su K, et al52 that used ABCG5/G8 KO mice fed phytosterol-free diets in order to prevent phytosterol accumulation in plasma and tissues. When mice were fed a phytosterol-free high fat diet, development of nonalcoholic fatty liver disease was accelerated in the ABCG5/G8 KO mice when compared to WT

7

mice. These results support the idea that ABCG5/G8 plays a role in sterol

metabolism beyond its function in limiting phytosterol absorption.

Additionally, some studies raise the possibility that ABCG5/G8 may play slightly

different roles in the liver and the small intestine where they are primarily

expressed. Under an unusual circumstance, a patient with sitosterolemia

received a liver transplant that resolved the disease53. The transplanted liver

presumably had ABCG5/G8 intact, resulting in a unique human model of small

intestine specific ABCG5/G8 deficiency. Prior to transplant, the patient had a

plasma phytosterol concentration of greater than 500 μmol/L. Post-transplant, plasma phytosterol concentrations dropped to below 60 μmol/L. This study indicates that when small intestinal ABCG5/G8 function was absent, the presence of hepatic ABCG5/G8 was sufficient to limit phytosterol accumulation.

Subsequently, the authors of this study concluded that hepatic ABCG5/G8 function is the primary determinant of steady state plasma phytosterol concentration. Further studies need to be done to confirm this conclusion, and to date no other data from models of tissue-specific ABCG5/G8 deficiency have been published.

In conjunction with its potential tissue specific role in phytosterol metabolism, there is evidence that ABCG5/G8 could also play a tissue specific role in the

RCT pathway. As previously stated, ABCG5/G8 is an LXR target gene and expression is required for LXR agonist mediated increases in biliary cholesterol

8

concentrations54, 55. Recently, it was reported that constitutive LXRα activation in

the small intestine caused increases in RCT in mice56. The same study showed

that hepatic-specific LXR activation did not cause any significant changes to

RCT. In line with these findings, activation of small intestinal LXR with an

intestinal-specific LXR agonist promoted macrophage RCT in mice57. Since this evidence is all indirect, it is important to directly test whether ABCG5/G8 functions in a tissue specific manner to regulate RCT and macrophage specific

RCT.

Based on the gaps in knowledge highlighted by this introduction, experiments

were designed to answer the following experimental questions:

1) What is the significance of phytosterol exclusion from the body?

To determine the significance of phytosterol exclusion from the body, we

fed wild-type and ABCG5/G8 knockout mice a diet enriched with plant

sterols. The high-phytosterol diet was extremely toxic to the ABCG5/G8

knockout mice but had no adverse effects on wild-type mice. ABCG5/G8

knockout mice died prematurely and developed a phenotype that included

high levels of plant sterols in many tissues, liver abnormalities, and severe

cardiac lesions.

9

2) Is hepatic ABCG5/G8 function required to prevent phytosterol

accumulation in plasma and tissues?

In order to determine whether hepatic ABCG5/G8 function is required for

phytosterol exclusion from the body, an anti-sense oligonucleotide (ASO)

targeted to ABCG8 was used to knockdown ABCG8 expression in the liver

of C57Bl/6 mice. Surprisingly, mice with hepatic ABCG8 knockdown did

not accumulate high levels of phytosterols but did appear to have alterated

hepatic cholesterol metabolism.

3) Is hepatic ABCG5/G8 function required for LXR agonist mediated

increases in RCT and/or macrophage RCT?

In order to test whether hepatic ABCG5/G8 function is necessary for LXR

agonist mediated increases in cholesterol excretion and macrophage

reverse cholesterol transport, an anti-sense oligonucleotide (ASO)

targeting ABCG8 was used to knockdown ABCG8 expression in the liver

of C57Bl/6 mice and RCT was measured. Interestingly, when mice had

decreased hepatic ABCG8 expression, cholesterol excretion and

macrophage RCT were not stimulated with LXR agonist treatment. This

data suggest that it is ABCG5/G8, a downstream target of LXR, that is

required for LXR stimulated increases in cholesterol excretion and

macrophage RCT.

10

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21

CHAPTER II

PHYTOSTEROL FEEDING CAUSES TOXICITY IN ABCG5/G8 KNOCKOUT MICE

Allison L McDaniel, Heather M Alger, Janet K Sawyer, Kathryn L Kelley, Nancy D Kock, J Mark Brown, Ryan E Temel, and Lawrence L Rudel

The following chapter was published in American Journal of Pathology. Stylistic variations are due to requirements of the journal.

22

ABSTRACT

Plant sterols, or phytosterols, are very similar in structure to cholesterol and are abundant in typical diets. It is unknown, however, why the body poorly absorbs plant sterols. Mutations in the ABC transporters G5 and G8 are known to cause an accumulation of plant sterols in blood and tissues (sitosterolemia). In order to determine the significance of phytosterol exclusion from the body, we fed wild type and ABCG5/G8 knockout mice a diet enriched with plant sterols. The high phytosterol diet was extremely toxic to the ABCG5/G8 knockout mice but had no adverse effects on wild type mice. ABCG5/G8 knockout mice died prematurely and developed a phenotype that included high levels of plant sterols in many tissues, liver abnormalities, and severe cardiac lesions. This study is the first to report such toxic effects of phytosterol accumulation in ABCG5/G8 knockout mice. We believe this new data supports the conclusion that plant sterols are excluded from the body because they are toxic when present at high levels.

INTRODUCTION

One of the longstanding mysteries of sterol metabolism is the need for discrimination between plant sterols (or phytosterols) and cholesterol. It has long been observed that while a typical diet generally contains similar amounts of cholesterol and phytosterols, intestinal cholesterol absorption rates are 40 to

60% while phytosterols are mostly excluded from the body due to intestinal absorption rates of less than 5% (1;2). The discrimination against phytosterols

23 has a basis in chemical structure. Campesterol, with a single carbon side chain at carbon 24 typically has a plasma concentration 500 times less than cholesterol while the concentration of sitosterol, with a 2 carbon side chain at carbon 24, is about 20,000 times lower than cholesterol (3).

The need for discrimination among sterols is not fully understood. In 1974,

Bhattacharyya and Conner (4) described a new lipid storage disease termed β- sitosterolemia, in two sisters with plant sterol accumulation in blood and tissues.

Subsequently, several other patients with sitosterolemia have been identified (5).

Patients accumulate plant sterols in many tissues and often present with tendinous and cutaneous xanthomas and hypercholesterolemia (5;6). There are also indications that plasma plant sterol accumulation has negative effects on platelet biology (7). Elimination of plant sterols from their diet is an effective treatment for patients (7;8).

Subsequent work has identified genetic mutations to the heterodimeric ABC transporters, ABCG5 and ABCG8, as the cause of sitosterolemia (9-11). Both

ABCG5 and ABCG8 must be expressed for their co-transport from the endoplasmic reticulum (ER) to the cell surface (12;13). Therefore, mutations to either or both of these proteins can result in a loss of functionality. These proteins are mainly expressed in the intestine and liver on the apical surface of enterocytes and hepatocytes (12;14). They apparently function to transport

24 cholesterol and phytosterols into bile in the liver and into the lumen of the small intestine (15), although the full functional significance is yet to be determined.

The identification of ABCG5 and ABCG8 as important players in sterol transport has led to the discovery and creation of several mouse models that lack one or both of the proteins. By genetic manipulations, ABCG5 single knockout, ABCG8 single knockout, and ABCG5/G8 double knockout mice have been created.

Additionally, one mouse model with a spontaneous mutation of ABCG5 has been previously described in the literature. The trac mutant mouse, which develops thrombocytopenia and cardiomyopathy, has a spontaneous point mutation at base 1435 of Abcg5 that results in a premature stop codon (16). The trac mutant mice and the genetically modified knockout mice have subtle differences among the models, but all have the fundamental accumulation of plant sterols in plasma and tissues (15;17-20). This phenotype is similar to that of human patients with sitosterolemia. Clearly, ABCG5 and ABCG8 play an essential role in excluding plant sterols from the body, although the purpose underlying this function is not well understood.

In order to determine the significance of phytosterol exclusion from the body, wild type and ABCG5/G8 knockout (KO) mice were fed a diet high in phytosterols

(0.2% w/w). The high phytosterol diet had no adverse effects on wild type mice, but surprisingly was extremely toxic to ABCG5/G8 KO mice. High levels of tissue plant sterol accumulation cause premature death, highly complex cardiac lesions,

25 liver damage, and hepatosplenomegaly, which have not been previously reported in this model.

METHODS

Animals and diet: ABCG5/G8 KO mice have been described previously (21).

WT and ABCG5/G8 KO mice on a mixed background of 81.5% C57Bl/6, 12.5%

SvJae, 6% 129SvEv were housed in a specific pathogen-free animal facility in plastic cages in a temperature-controlled room (22°C) with a daylight cycle from

6AM to 6PM. The mice were fed ad libitum a standard rodent chow diet

(5P00Prolab; LabDiet) prior to the start of the high-phytosterol diet and had free access to water. At 6-8 weeks of age, female WT and ABCG5/G8 KO mice were fed a low-fat (10% of energy as palm oil enriched fat) synthetic diet containing

0.2% (w/w) phytosterols and 0.001% (w/w) cholesterol (Supplemental Table 1) for 6 weeks. The diet was made at the Wake Forest University Primate Center

Diet Laboratory. Body weights were measured weekly throughout the study. All animal procedures were approved by the institutional animal care and use committee at Wake Forest University Health Sciences.

Measurement of plasma and tissue lipid concentrations: After a 4 h fast, blood was collected from mice that had been fed the synthetic diets for 6 weeks.

Tissues were flushed with saline, removed, weighed and either snap-frozen in liquid nitrogen or fixed in 10% neutral buffered formalin (NBF) for later analyses.

26

To determine total plasma cholesterol and phytosterol concentrations, 25μL of plasma was placed into a glass tube containing 21μg 5α-cholestane and extracted in 2:1 CHCl3:methanol overnight. Erythrocytes were separated from

plasma and rinsed with saline before an overnight extraction in 2:1

CHCl3:methanol. 5α-cholestane was used as an internal standard. For tissue

analysis of cholesterol and phytosterol concentrations, ∼50mg of frozen tissue

was placed into a glass tube containing 135 μg 5α-cholestane. were extracted in 2:1 CHCl3:methanol at room temperature overnight. Total sterol

mass was measured for all samples by gas-liquid chromatography as described

previously (22).

Hematologic measurements: After a four-hour fast, a blood sample was

obtained via submandibular puncture biweekly after high-phytosterol diet feeding

began. Separate tubes were used for blood collection of serum and plasma

samples. Samples were spun to separate erythrocytes. Serum chemistry values

were determined by ANTECH Diagnostics (Lake Success, NY). Hematocrit

values were determined by collection of blood into hematocrit tubes and spun to

pack red cells (VWR International, West Chester, PA).

Real Time Polymerase Chain Reaction (RT-PCR) analysis of gene

expression in livers and spleens: Frozen pieces (~50mg) of liver and spleen

were homogenized into 1ml of Trizol Reagent (Invitrogen) and total RNA was

extracted according to manufacturer’s instructions. Recovery and integrity of

27

RNA was determined and cDNA was made using Omniscript Reverse

Transcriptase (Qiagen) and 1μg of RNA according to manufacturer’s instructions.

Relative was determined in each cDNA sample using forward and reverse primers designed to each gene of interest (Table 1) and SYBR-

Green PCR master mix (Applied Biosciences). Reactions were monitored on an

ABI Prism 7000 Sequence Detection System using the cycling parameters: 50oC-

2min, 95oC-10min, (95oC-15sec, 60oC-1min)-40 cycles, 60oC-1min, 60oC dissociation. Relative expression of each gene was normalized to expression of a housekeeping gene (actin or 18S ribosomal RNA) to control for intra-/inter- sample variation and expressed as arbitrary units (AU).

28

TABLE 1

Gene Primer 1 (5’→3’) Primer 2 (5’→ 3’)

ABCA1 CGTTTCCGGGAAGTGTCCTA GCTAGAGATGACAAGGAGGATGGA

ABCB11 GACATGCTTGCGAGGACCTT AGCGTTGCCGGATGGA

BLVRA CTTGATGGAAGAGTTCGAATTCCT GTGAAGCGAAGAGATCCTTTTAGC

CD68 CCTCCACCCTCGCCTAGTC TTGGGTATAGGATTCGGATTTGA

CYP7A1 AGCAACTAAACAACCTGCCAGTACTA GTCCGGATATTCAAGGATGCA

Cyclophilin TGGAGAGCACCAAGACAGACA TGCCGGAGTCGACAATGAT

HMGCS GCCGTGAACTGGGTCGAA GCATATATAGCAATGTCTCCTGCAA

HO1 CAACAGTGGCAGTGGGAATTTA CCAGGCAAGATTCTCCCTTACC

IL-6 CTGCAAGAGACTTCCATCCAGTT AGGGAAGGCCGTGGTTGT

PLTP TGGGACGGTGTTGCTCAA CCCACGAGATCATCCACAGA

SCD1 CCGGAGACCCCTTAGATCGA TAGCCTGTAAAAGATTTCTGCAAACC

SR-BI TCCCCATGAACTGTTCTGTGAA TGCCCGATGCCCTTGA

SREBP1C GGAGCCATGGATTGCACATT GGCCCGGGAAGTCACTGT

UGT1A CACCACACCTGCGCCC CCAATCACATCCAAGGAGTGGTA

Table 1. RT-PCR primers.

29

Histology: Hearts were preserved in 10% neutral buffered formalin (NBF) for at least 24 hours, processed routinely for histology, cut at 6 microns, and sections were stained with hematoxylin and eosin (H and E), Masson’s trichrome and Von

Kossa. Snap-frozen liver samples were preserved for 48 hours in 10% NBF, followed by cryo-preservation in 20% sucrose, prior to routine histology processing and staining with H and E. Tissues were examined by light microscopy in a blinded fashion by a board certified anatomic veterinary pathologist. To determine Kupffer cell infiltration, cells were counted in a single microscopic field for each liver section. Kupffer cell number was normalized to the total number of hepatocytes in each field. In order to quantitate cardiac fibrosis, trichrome stained sections were used. An outline of the heart chambers was traced and subtracted from the total heart area. Then, areas of fibrosis were traced and normalized to the calculated heart area.

Statistical Analyses and Data Presentation: Data are expressed as the mean

± SEM. Significance of differences was determined for each group of values by

ANOVA (Tukey-Kramer honestly significant difference) or unpaired t-test.

A p value < 0.05 was considered significant. All analyses were performed using

GraphPad Prism 4 software (LaJolla, CA).

30

RESULTS

ABCG5/G8 KO mice failed to gain weight and developed hepatosplenomegaly when fed a high phytosterol diet

When fed a diet rich in plant sterols, wild type mice maintained a normal phenotype, while ABCG5/G8 KO mice showed generally poor health, characterized by weight loss, hunching, lethargy, and decreased life span

(unpublished observations by McDaniel & Alger). Figure 1A shows that wild type mice gained weight over a six week timecourse of the high phytosterol diet feeding, while the ABCG5/G8 KO mice did not gain weight relative to their baseline measurement. This phenotype was not seen in ABCG5/G8 KO mice fed a diet containing an identical amount of cholesterol (see Supplemental Fig 1 &

Supplemental Table 1 at http://ajp.amjpathol.org). This observation suggests that the effects were not caused by a general accumulation of sterols in the body, but rather, were caused specifically by the accumulation of plant sterols.

Further investigation revealed that by 6 weeks, the ABCG5/G8 KO mice fed the high phytosterol diet had a high liver to bodyweight ratio (Fig 1B). Measurement of organ weights showed significantly higher liver mass and spleen mass (Fig

1C) in ABCG5/G8 KO mice compared to wild type mice. This organ enlargement translated into significantly increased percentages of total bodyweight for liver and spleen (Fig 1D). By contrast, there was no change in the mass or percentage of bodyweight of the kidneys or lungs of ABCG5/G8 KO mice (Fig 1C

& 1D).

31

Supplemental Figure 1. Bodyweight measurement. Animals were fed a high cholesterol diet (0.2% w/w) for 6 weeks. WT (n=5), ABCG5/G8 KO (n=8). Bodyweights were measured weekly.

Diet Cholesterol Campesterol Stigmasterol Sitosterol High (mg Phytostero sterol/100g 11 51.8 54.2 91.4 l dried weight) % of diet 5 25 26 44 High (mg Cholester sterol/100g 199.9 5.6 3.7 12.3 ol dried weight) % of diet 90 3 2 6

Supplemental Table 1. Dietary sterol compositions.

32

Figure 1. Measurement of body and tissues weights. Animals were fed a diet rich in plant sterols (0.2%) for 6 weeks. WT (n=5), ABCG5/G8 KO (n=10). (A) weekly bodyweight in grams, (B) terminal liver to bodyweight ratio multiplied by 100, (C) terminal organ mass in grams, and (D) percentage of total bodyweight as individual tissue. * indicates p<0.05 as measured by ANOVA and Tukey- Kramer post-test.

33

In ABCG5/G8 KO mice, plant sterol accumulation caused liver damage

To further characterize the health of the phytosterol-fed ABCG5/G8 KO mice, serum chemistry values were assessed. Serum ALT/SGPT (alanine transaminase/glutamic-pyruvic transaminase) concentrations were found to be elevated in ABCG5/G8 KO mice at all timepoints, in contrast to concentrations in wild type mice that remained in the normal range (Fig 2A). ABCG5/G8 KO mice showed no changes in serum glucose, urea nitrogen (BUN), creatinine, total protein, alkaline phosphatase, calcium, or phosphorus when compared to wild type mice over the 6 week dietary timecourse (data not shown).

Sections of liver from wild type and ABCG5/G8 KO mice stained with H and E were reviewed by an anatomic veterinary pathologist (Fig 2B-E). ABCG5/G8 KO mouse livers (Fig 2D-E) had piecemeal necrosis and hepatocellular degeneration, cellular rounding and detachment (red arrows), and prominent diffuse Kupffer cell hyperplasia (green arrows). Quantification of Kupffer cells in these livers revealed a 2.19 fold increase in the number of Kupffer cells present in ABCG5/G8 KO mouse livers as compared to wild type. This increase in

Kupffer cells was also reflected by a higher ratio of Kupffer cells to hepatocytes

(WT = 0.68, KO = 2.01). Further confirming the histological increase in Kupffer cells, a significant 2.3 fold increase in the hepatic macrophage marker, CD68, was measured by mRNA levels in ABCG5/G8 KO mice (Table 2). Wild type mouse livers (Fig 2B-C) were considered normal.

34

Figure 2. Assessment of liver pathology. (A), biweekly measures of serum ALT (SGPT) expressed as U/dL showed significant increases in the phytosterol fed ABCG5/G8 KO mice. (B-E) Photomicrographs of liver from wild type mice (B, C) and ABCG5/G8 KO mice (D, E). Liver from the wild type mice was considered within normal limits. That from the ABCG5/G8 KO mice shows piecemeal hepatocellular necrosis with cellular rounding and detachment (red & yellow arrows), nuclear pyknosis, hepatocellular swelling, and Kupffer cell hyperplasia (green arrows). H and E 100X. *indicates p<0.05 as measured by ANOVA and Tukey-Kramer post-test.

35

In order to examine the effects of phytosterol accumulation on hepatic lipid and bile acid metabolism, a variety of genes were selected and mRNA levels were measured by RT-PCR. As previously reported by Yu et al (21), ABCG5/G8 KO mice had a significant decrease in hepatic hydroxymethylglutaryl CoA synthase

(HMGCS) mRNA when compared to wild type mice. Other significant changes to hepatic mRNA levels included an increase in stearoyl-CoA desaturase-1 (SCD1) and a decrease in ATP-binding cassette transporter B11 (ABCB11). Expression levels of scavenger receptor class B member I (SR-BI), ATP-binding cassette transporter A1 (ABCA1), phospholipid transfer protein (PLTP), sterol regulatory element binding protein 1C (SREBP1C), and cholesterol 7α-hydroxylase

(CYP7A1) were not significantly different between wild type and ABCG5/G8 KO mice. Preliminary data was obtained suggesting that in these mice, phytosterols are not converted into C21 bile acids as had been suggested to occur in rats

(23)(Alger and Bjorkhem, unpublished results). More work, however, needs to be done to determine the specific roles phytosterols may play in hepatic lipid and bile acid metabolism.

36

Hepatic Gene Expression

WT ABCG5/G8 KO p Bilirubin Metabolism BLVRA 12.38 ± 0.94 10.86 ± 1.84 0.5656 HO-1 7.73 ± 0.79 24.93 ± 4.06 * 0.0061 UGT1a 38.29 ± 4.14 18.34 ± 2.77 * 0.0069

Inflammatory Markers CD68 12.7 ± 2.68 29.8 ± 3.29 * 0.007 IL-6 3.1 ± 0.65 3.4 ± 0.66 0.7672

Lipid Metabolism HMGCS 27.90 ± 2.68 14.62 ± 2.82 * 0.0145 SR-BI 8.8 ± 1.86 9.2 ± 1.45 0.8670 ABCA1 4.3 ± 0.40 5.3 ± 0.76 0.2924 SCD1 145.5 ± 18.53 305.5 ± 45.01 * 0.0167 PLTP 1.36 ± 0.31 1.18 ± 0.11 0.6046 SREBP1C 2.3 ± 0.27 3.1 ± 0.32 0.1271

Bile Acid Metabolism CYP7A1 22.9 ± 8.61 18.1 ± 2.66 0.6104 ABCB11 9.3 ± 0.97 4.4 ± 0.34 * 0.0029

Splenic Gene Expression

WT ABCG5/G8 KO p

BLVRA 10.61 (0.62) 13.86 (0.97) * 0.0369 HO-1 26.31 (1.66) 31.19 (6.83) 0.5059 HMGCS 8.53 (0.97) 8.25 (0.86) 0.6891

Table 2. Hepatic and splenic gene expression. mRNA was extracted from terminal tissues. Gene expression was normalized to Cyclophilin or 18s ribosomal RNA and expressed as average units (AU) ± SEM. * indicates p<0.05 as measured by unpaired t-test.

37

ABCG5/G8 KO mice accumulated plant sterols in a variety of tissues

Because ABCG5/G8 KO mice accumulate plant sterols in liver and plasma on a chow based diet with only natural phytosterol levels (15), we measured the total sterol concentrations across several tissues. Liver, heart, spleen, kidney, lung, and adrenal tissues from ABCG5/G8 KO mice all have greatly increased levels of phytosterols, relative to wild type mice, but minimal changes in the amount of total sterol present - with the exception of adrenal tissue (Fig 3A & B). As a result, phytosterols account for a large percentage of the total sterol amounts in the tissues of ABCG5/G8 KO mice. In fact, tissue total sterol composition reached as high as 77% phytosterol in the liver (Fig 3C). Other plant sterol- containing tissues had a range of total sterol composition from 41-72% phytosterol (Fig 3C). As previously reported in chow-fed ABCG5/G8 KO mice

(19), plant sterols did not accumulate in the brain to the same extent as other tissues (Fig 3A & C).

38

Figure 3. Tissue sterol concentrations. Sterols from terminal tissues were extracted and analyzed by GC. Plant sterol values are shown in white and cholesterol values are shown in black. (A) Plant sterol mass expressed as μg/mg of tissue wet weight. (B) Cholesterol mass expressed as μg/mg of tissue wet weight. (C) Tissue plant sterol and cholesterol values expressed as percentages of the total sterol concentration.

39

Total plasma sterol concentration was over 2-fold higher in ABCG5/G8 KO mice compared to wild type mice (Fig 4A). This increase was due to a plasma phytosterol concentration of 250mg/dL (Fig 4A), which resulted in almost 75% of total plasma sterol to be plant sterol in ABCG5/G8 KO mice (Fig 4B). As previously reported in chow fed ABCG5/G8 KO mice, plasma cholesterol concentrations decreased in the phytosterol-fed ABCG5/G8 KO mice as compared to wild type mice ((15), Fig 4A).

Hematocrit and erythrocyte sterol composition were also measured since macrothrombocytopenia has been observed in both human patients with sitosterolemia and in ABCG5/G8 KO mice (7;20). After receiving the phytosterol- enriched diet for only 2 weeks, ABCG5/G8 KO mice had lower hematocrit, compared to wild type mice (Fig 4C) that persisted at weeks 4 and 6.

Additionally, the erythrocyte sterol composition of ABCG5/G8 KO mice, which began at 38% phytosterol at baseline, increased to almost 60% phytosterol over the 6 week dietary timecourse (Fig 4D).

40

Figure 4. Plasma characterization. Terminal plasma samples were collected for analysis. (A) Sterols were extracted and expressed as mg/dL of plasma. Plant sterol values are shown in white and cholesterol values are shown in black. (B) Plasma plant sterol and cholesterol values expressed as percentages of the total sterol concentration. (C) Biweekly hematocrit measurements are expressed as % of blood that is erythrocytes. (D) Biweekly erythrocyte plant sterol content is shown as a percentage of the total sterol concentration. * indicates p<0.05 as measured by ANOVA and Tukey-Kramer post-test.

41

Erythrocyte clearance gene expression was elevated in ABCG5/G8 KO mice

The liver and spleen both play an important role in erythrocyte removal from the plasma. Since the liver and spleen were significantly enlarged and the erythrocytes of ABCG5/G8 KO mice contained a large amount of plant sterol that could affect their function, RT- PCR was used to measure the expression of several hepatic and splenic genes involved in erythrocyte clearance. These genes were selected based on previous studies by Meurs et al (24) describing the erythrocyte clearance pathway and the genes involved in the controlled breakdown of erythrocyte bilirubin. These genes included BLVRA (biliverdin reductase A), HO-1 (hemeoxygenase 1), UGT1A (diphosphoglucuronate glucuronosyltransferase 1A), and HMGCS (HMG-CoA synthase). Relative hepatic and splenic gene expression was normalized to cyclophilin and compared between wild type and ABCG5/G8 KO mice on the high phytosterol diet. Consistent with the findings of hepatosplenomegaly and reduced hematocrit, expression of hepatic HO-1, UGT1-a, and HMGCS along with splenic

BLVRA were significantly altered in mice lacking ABCG5/G8 (Table 2).

ABCG5/G8 KO mice develop complex cardiac lesions

During necropsy, an unusual cardiac phenotype was detected in the ABCG5/G8

KO mice. Approximately half of the phytosterol-fed ABCG5/G8 KO mice had irregularly shaped and sized areas of pallor in the left ventricle (Fig 5A). In order

42 to characterize these cardiac lesions, hearts fixed in neutral buffered formalin were sectioned and stained with H and E, Von Kossa, and Masson’s trichrome. H and E staining confirmed that the wild type hearts did not have lesions (Fig 5B).

H and E stained hearts from ABCG5/G8 KO mice, however, had extensive myocardiocyte loss with replacement by fibrosis and calcification (Fig 5B). Von

Kossa and Masson’s trichrome stains confirmed the presence of calcium and collagen in these cardiac lesions (Fig 5B). Morphometric quantification of the fibrosis revealed a >20 fold increase in the amount of myocardial fibrosis detected in ABCG5/G8 KO mice compared to wild type mice. When cross sectional fibrosis was measured, approximately 20% of the area was fibrotic in

ABCG5/G8 KO mouse heart, but less than 1% of the area was fibrotic in wild type mouse heart.

43

Figure 5. Cardiac histology. (A) Gross images of hearts from wild type (top) and ABCG5/G8 KO mice (bottom – labeled G5G8 in the figure). The ABCG5/G8 KO mice had areas of pallor on the left ventricular free wall (red arrows). Lesions were absent in the wild type hearts. (B) Photomicrographs of wild type and ABCG5/G8 KO mouse hearts. Wild type hearts were considered within normal limits. Hearts from ABCG5/G8 KO mice had extensive left ventricular myocardial loss (H and E) with replacement by fibrous connective tissue (Masson’s trichrome) and extensive mineralization (Von Kossa). Lesions were absent in the wild type mice. 4X and 40X magnification is indicated.

44

DISCUSSION

This study shows for the first time specific toxicities that occur when phytosterols accumulate at high levels in the body. ABCG5/G8 KO mice, which hyperabsorb plant sterols, fail to gain weight, become lethargic and hunched, and die prematurely when fed a high phytosterol diet. This phenotype is specific to plant sterol accumulation, as we did not see signs of poor health in ABCG5/G8 KO mice fed a high (0.2% w/w) cholesterol diet. Toxic side effects have not been reported in other studies where ABCG5/G8 double knockout mice were fed chow based diets containing relatively lower levels of phytosterols (15;19).

In agreement with other studies (15;19), campesterol and sitosterol were the main plant sterol species that accumulated in ABCG5/G8 KO mice fed the plant sterol rich diet. Plant sterols accumulated to very high levels in the tissues of phytosterol-fed ABCG5/G8 KO mice. Phytosterols constituted 77% of all hepatic sterols in our mice and ranged from 41-72% of sterols in spleen, heart, kidney, lung, and adrenal glands. These values are much higher than reported values in

ABCG5/G8 knockout mice fed a chow diet (15). On a chow diet, plasma phytosterol concentrations in ABCG5/G8 KO mice averaged 30-50mg/dL (15;19).

On the high phytosterol diet we used, however, plasma phytosterol levels reached 5 times that amount.

The extreme levels of phytosterol accumulation caused damage in several tissues. ABCG5/G8 KO mice had hepatosplenomegaly and liver damage. Most

45 strikingly, ABCG5/G8 KO mice developed extensive myocardial calcification and fibrosis with loss of myocardiocytes. Contrastingly, cardiomyopathy with multifocal myocardial fibrosis was reported in the trac mutant mouse, but cardiac lesions were not described (16).

The trac mutant mice have a naturally occurring spontaneous mutation only in

ABCG5 that causes them to accumulate plant sterols. Interestingly, this particular mutation seems to be associated with a less severe phenotype than seen here in phytosterol-fed ABCG5/G8 KO mice. The trac mutant mice, however, were not fed the high phytosterol diet. Trac mutant mice become hunched and have a shortened life span of 4-6 months on a regular chow diet (16). In comparison,

ABCG5/G8 KO mice died as early as 3 months of age when fed the high phytosterol diet (5 weeks of diet feeding). Other gross indicators of poor health found in our ABCG5/G8 KO mice, like lethargy and failure to gain weight, were not reported in trac mutant mice.

The differences between these mouse models could be attributed to the amount of phytosterols that accumulate in the body. Trac mutant mice have plasma phytosterol concentrations of approximately 130mg/dL, which fall in between chow-fed ABCG5/G8 knockout mice (30-50mg/dL) and phytosterol-fed

ABCG5/G8 KO mice (>250mg/dL). This would support the idea that the level of toxicity of phytosterols depends on the total amount of accumulation in the body.

46

Studies in both humans and mouse models have revealed macrothrombocytopenia as a marker of sitosterolemia (7;20). The plasma phenotype of ABCG5/G8 KO mice fed a high phytosterol diet was consistent with those findings. Erythrocyte phytosterol content increased by 20% and significant decreases in hematocrit were seen as early as 2 weeks of phytosterol-enriched diet feeding. Hepatic HO-1, UGT-1A, HMGCS, and splenic BLVRA expression levels were significantly altered in ABCG5/G8 KO mice. These data indicate that the erythrocyte clearance pathway is upregulated, which could be an attempt to clear altered red blood cells.

Other studies have not reported large accumulations of phytosterols in the brain of ABCG5/G8 knockout mice (19). Alternatively, P.J. Jansen et al. measured a small but significant amount of phytosterols, 600-1000 ng/mg dry weight, in the brain of chow fed ABCG5 or ABCG8 knockout mice (25). In our study, we also found small but significant amounts of plant sterols that averaged 230 ng/mg in the brain of ABCG5/G8 KO mice fed a high phytosterol diet. These levels of phytosterols in the brain were miniscule (<2%) compared to the amounts that accumulated in other tissues.

The findings of this study are useful in relation to dietary phytosterol supplementation, which is currently used to reduce the risk of coronary heart disease (CHD) (26;27). Plant sterols are thought to reduce plasma cholesterol concentrations by inhibiting cholesterol absorption (28;29). Most individuals are

47 able to exclude plant sterols from the body via ABCG5/G8, and the FDA allows phytosterol-enriched foods to be classified as “generally recognized as safe.” In several species of animals, presumably with ABCG5/G8 intact, that have been administered high doses of plant sterols, there have been no reports of toxicity

(2). Some debate still exists, however, about the safety of dietary phytosterol supplementation, specifically concerning their potential cytotoxic effects on endothelial cells in arteries.

Our study shows that an extremely high concentration of phytosterols in plasma and tissues is widespread and toxic. This phenotype seems to depend specifically on the amount of phytosterols that accrue. The presence of intact

ABCG5/G8 in an individual appears to offer full protection against dietary phytosterol accumulation, and there is no indication that long term exposure could cause levels of phytosterols to build up to toxic levels. Consequently, dietary supplementation with phytosterols appears safe for the general population.

Our findings also lend novel insight into the body’s need for discrimination between plant sterols and cholesterol. We have shown for the first time that high levels of tissue plant sterol accumulation cause premature death, extensive cardiac lesions, liver damage, and hepatosplenomegaly. These toxicities appear related to accumulation of high levels of unesterified phytosterols that cannot be efficiently metabolized into bile acids nor esterified for storage in lipid droplets.

48

Accumulation as the free sterol probably results in accumulation in membranes with subsequent disruption of membrane integrity. In conclusion, our data show that ABCG5/G8’s role in phytosterol exclusion from the body is one of protection from the toxic effects of plant sterols.

49

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55

CHAPTER III

HEPATIC ABCG8 KNOCKDOWN DOES NOT RESULT IN HIGH LEVELS OF PHYTOSTEROL ACCUMULATION

Allison L. McDaniel, Lawrence L Rudel, J. Mark Brown, Ryan E. Temel

56

ABSTRACT

ABCG5/G8 limits sterol accumulation in the body by transporting cholesterol and phytosterols into bile in the liver and into the lumen of the small intestine. Under an unusual circumstance, a patient with β–sitosterolemia received a liver transplant that resolved the disease. This study indicates that when small intestinal ABCG5/G8 function remains absent, the presence of hepatic

ABCG5/G8 is sufficient to limit phytosterol accumulation. The authors of this study concluded that hepatic ABCG5/G8 function is the primary determinant of steady state plasma phytosterol concentration. To date no other data from models of tissue-specific ABCG5/G8 deficiency have been published to confirm this finding. In order to determine whether hepatic ABCG5/G8 function is required for phytosterol exclusion from the body, an anti-sense oligonucleotide (ASO) targeted to ABCG8 was used to knockdown ABCG8 expression in the liver of

C57Bl/6 mice. Surprisingly, mice with hepatic ABCG8 knockdown did not accumulate high levels of phytosterols but did appear to have alterated hepatic cholesterol metabolism.

INTRODUCTION

Sitosterolemia is a lipid storage disease in which genetic mutations to adenosine triphosphate-binding cassette transporter G5 or G8 (ABCG5/G8) cause significant plant sterol (or phytosterol) accumulation in the blood and tissues of patients. Since the discovery of sitosterolemia, many studies have examined the

57 role of ABCG5/G8 in sterol metabolism. Genetic mouse models of whole body

ABCG5/G8 deficiency have phenotypes similar to human patients with sitosterolemia, including reduced levels of biliary sterols and marked accumulation of plant sterols in their blood and tissues1, 2. These findings reveal

that the apparent physiological role of ABCG5/G8 is to limit sterol accumulation in the body by transporting cholesterol and phytosterols into bile in the liver and into the lumen of the small intestine.

The effects of phytosterol accumulation in models of ABCG5/G8 deficiency are substantial. Several groups have reported changes in hepatic cholesterol metabolism when phytosterols are increased1, 3, 4. For example, on low

cholesterol diets ABCG5/G8 KO mice have significant reductions in plasma and

hepatic cholesterol concentrations1, 4, 5. Despite these reductions, there are no

compensatory increases in the expression genes involved in cholesterol

synthesis. Hepatic mRNA levels of HMG-CoA synthase and reductase are

actually reduced by 50% in ABCG5/G8 KO mice. The consequences of

accumulation become dire when the phytosterol concentrations reach very high

levels. We recently reported that feeding ABCG5/G8 KO mice a diet enriched in

phytosterols (0.2% w/w) was extremely toxic5. The high plant sterol diet caused

dramatic increases to plasma and tissue phytosterol concentrations in

ABCG5/G8 KO mice, resulting in premature death, liver abnormalities, and

severe cardiac lesions.

58

From these studies of ABCG5/G8 KO mice, it is not completely clear how much of the changes in sterol metabolism are due to the mass accumulation of plant sterols versus the lack of ABCG5/G8 function. It is possible that the complete role of ABCG5/G8 in sterol metabolism is partly masked by the accumulation of plant sterols. Interestingly, a study was published in 2012 by Su K, et al6 that

used ABCG5/G8 KO mice fed phytosterol-free diets in order to prevent

phytosterol accumulation in plasma and tissues. When mice were fed a

phytosterol-free high fat diet, development of nonalcoholic fatty liver disease was

accelerated in the ABCG5/G8 KO mice when compared to WT mice. These

results support the idea that ABCG5/G8 plays a role in sterol metabolism beyond

its function in limiting phytosterol absorption.

Additionally, some studies raise the possibility that ABCG5/G8 may play slightly

different roles in the liver and the small intestine where they are primarily

expressed. Under an unusual circumstance, a patient with sitosterolemia

received a liver transplant that resolved the disease7. The transplanted liver

presumably had ABCG5/G8 intact, resulting in a unique human model of small

intestine specific ABCG5/G8 deficiency. Prior to transplant, the patient had a

plasma phytosterol concentration of greater than 500 μmol/L. Post-transplant, plasma phytosterol concentrations dropped to below 60 μmol/L. This study indicates that when small intestinal ABCG5/G8 function remained absent, the presence of hepatic ABCG5/G8 was sufficient to limit phytosterol accumulation.

Subsequently, the authors of this study concluded that hepatic ABCG5/G8

59 function is the primary determinant of steady state plasma phytosterol concentration. Further studies need to be done to confirm this conclusion, and to date no other data from models of tissue-specific ABCG5/G8 deficiency have been published.

The goal of this study was to address the relative contribution of hepatic

ABCG5/G8 function to whole body sterol metabolism. In order to do this, an anti- sense oligonucleotide (ASO) targeted to ABCG8 was used to knockdown ABCG8 expression in the liver of C57Bl/6 mice. Based on the results from the human liver transplant patient, we hypothesized that phytosterols would accumulate in the plasma and tissues of mice with hepatic ABCG8 knockdown. Surprisingly, mice with hepatic ABCG8 knockdown did not accumulate high levels of phytosterols but did significantly alterat hepatic cholesterol metabolism.

METHODS

Animals and diet: Female C57Bl/6 mice 6-8 weeks of age were ordered from

Harlan Laboratories (Indianapolis, IN). At 7-9 weeks of age, mice were fed a low- fat (10% of energy as palm oil enriched fat) synthetic diet containing either 0.01%

(w/w) phytosterols and 0.003% (w/w) cholesterol (Low Sterol Diet); 0.01% (w/w) phytosterols and 0.2% (w/w) cholesterol (High Cholesterol Diet); or 0.2% (w/w) phytosterols and 0.003% (w/w) cholesterol (High Phytosterol Diet) (Supplemental

Table I, Supplemental Figure I) for 6 or 12 weeks. The diets were made at the

Wake Forest University Primate Center Diet Laboratory. In conjunction with diet

60 feeding, mice received bi-weekly intraperitoneal injections of a nontargeting control ASO or ABCG8 ASO (50mg/kg/week). The 20-mer phosphorothioate

ASOs were designed to contain 2'-0-methoxyethyl groups at positions 1 to 5 and

15 to 20, and were synthesized, screened, and purified as described previously8 by ISIS Pharmaceuticals (Carlsbad, CA).

ABCG5/G8 KO mice have been described previously1. At 6-8 weeks of age, female WT and ABCG5/G8 KO mice (81.5% C57Bl/6, 12.5% SvJae, 6%

129SvEv) were fed a low-fat (10% of energy as palm oil enriched fat) synthetic diet containing either 0.01% (w/w) phytosterols and 0.003% (w/w) cholesterol

(Low Sterol Diet); 0.01% (w/w) phytosterols and 0.2% (w/w) cholesterol (High

Cholesterol Diet); or 0.2% (w/w) phytosterols and 0.003% (w/w) cholesterol (High

Phytosterol Diet) (Supplemental Table I, Supplemental Figure I) for 6 weeks. The diets were made at the Wake Forest University Primate Center Diet Laboratory.

All mice were fed ad libitum a standard rodent chow diet (5P00Prolab; LabDiet) prior to the start of the high-phytosterol diet and had free access to water. Mice were housed in a specific pathogen-free animal facility in plastic cages in a temperature-controlled room (22°C) with a daylight cycle from 6AM to 6PM.

Bodyweights were measured weekly throughout all studies. Experimental animals were euthanized following a 4 h fast during the light cycle. All experimental protocols were approved by the Institutional Animal Care and Use

Committee at the Wake Forest University School of Medicine.

61

Real Time Polymerase Chain Reaction (RT-PCR) analysis of gene expression in liver and duodenum: Total mRNA was extracted from ∼100 mg of liver and small intestinal segment 2 with Trizol (Invitrogen Life Technologies) using the protocol provided by the manufacturer. The mRNA was resuspended in diethyl pyrocarbonate water, and 1 μg of mRNA was reverse transcribed to cDNA using qScript cDNA SuperMix (Quanta Biosciences) under the following conditions: 25°C for 5 min, 42°C for 30 min, and 85°C for 5 min. The cDNA was diluted 1:10 using diethyl pyrocarbonate water, and real-time PCR was done in triplicate with 5 μl of cDNA, 10 μl of SYBR GREEN PCR master mix (Applied

Biosystems), 3 μl of diethyl pyrocarbonate water, and 1 μl of forward and reverse primer (20 pmol) for a final reaction volume of 20 μl. The primer sequences are are as follows: ABCG8 (F: 5’-AAC CCT GCG GAC TTC TAC G; R: 5’-CTG CAA

GAG ACT GTG CCT TCT); ABCG5 (F: 5’-TCC TGC ATG TGT CCT ACA GC; R:

5’-ATT TGC CTG TCC CAC TTC TG); β-actin (F: 5’-GCT CTG GCT CCT AGC

ACC AT; R: 5’-GCC ACC GAT CCA CAC AGA GT). PCR was then run on the

Sequence Detection System 7500 (Applied Biosystems) using the following conditions: 50°C for 2 min, 95°C for 10 min, and 40 cycles of 95°C for 10 s and

60°C for 30 s. The fluorescence measurement used to calculate threshold cycle

(Ct) was made at the 60°C point. A dissociation curve was run at the end of the reaction to ensure a single amplification product. All Ct values were normalized to β-actin mRNA concentration of the sample to take total mRNA concentration into account. The average of Ct values from the CON LS mice were set to 1 and

62 all other groups were expressed as the fold change compared to the CON LS group.

Immunoblotting: Tissue homogenates were made from liver and duodenum in a membrane buffer (0.25M sucrose, 2mM MgCl2, 20mM Tris, pH 7.5).

Homogenates were spun for 10 minutes at 2000 x g, 4°C. Supernatants were

collected and spun for 45 minutes at 100,000rpm, 4°C. The pellet was

resuspended in a membrane solubilization buffer (1% Triton X-100, 4mM CaCl2,

80mM NaCl, 50mM Tris, pH 8.0) using a 1cc 28G1/2 U-100 insulin syringe to completely resuspend the pellet. The membrane proteins (15μg/lane) were separated by 4–12% SDS-PAGE, transferred to polyvinylidene difluoride membranes, and incubated with an anti-ABCG8 antibody. The ABCG8 antibody was kindly provided by Greg Graf, University of Kentucky.

Measurement of Biliary, Plasma, and Hepatic lipid concentrations: At necropsy, blood was collected by heart puncture and was placed into a tube containing protease inhibitor cocktail (Sigma) dissolved in 5% EDTA, 5% NaN3.

Gallbladder bile was collected, and then the liver was removed, weighed, and snap-frozen in liquid N2. The small intestine from the pyloric valve to the cecum

was removed, cleaned of fat and luminal contents while on ice, and cut into either

three sections of equal length. The intestinal sections were snap-frozen in liquid

N2 and stored along with the liver and bile samples at −80°C. The blood was

centrifuged at 12,000 g for 10 min at 4°C, and plasma lipids were extracted with

63

2:1 CHCl3/methanol in the presence of 21 μg 5α-cholestane at room temperature overnight. The lipid extract was dried down under N2 and saponified by adding

1mL ethanol and 100μL 50% KOH and heating at 60°C for 1 hour. Neutral lipids

were extracted by adding hexane and deionized water, vortexing, and

centrifuging at 2,000 g for 10 min. The hexane phase was then analyzed by gas- liquid chromatography9 for total sterol content. To determine plasma lipoprotein

sterol distribution, lipoprotein classes were separated by gel filtration

chromatography as described previously10.

For analysis of the liver lipid composition, ∼100 mg of liver was thawed, minced,

and weighed in a glass tube. Lipids were extracted with 2:1 CHCl3/methanol in

the presence of 135 μg 5α-cholestane at room temperature overnight. The lipid

extract was dried down under N2 and redissolved in a measured volume of 2:1

CHCl3/methanol. Dilute H2SO4 was added to the sample, which was then

vortexed and centrifuged to split the phases. An aliquot of the organic phase was

dried down under N2, dissolved in hexane, and analyzed for free sterol content by gas-liquid chromatography9. The remaining organic phase was saponified by

adding 2mL ethanol and 200μL 50% KOH and heating at 60°C for 2 hours.

Neutral lipids were extracted by adding hexane and deionized water, vortexing,

and centrifuging at 2,000 g for 10 min. The hexane phase was then analyzed by

gas-liquid chromatography9 for total sterol content.

64

For analysis of biliary lipid concentrations, a measured volume (3–10 μl) of bile was extracted with 2:1 CHCl3/MeOH in the presence of 10 μg 5α-cholestane. The organic phase was analyzed for sterol content by gas-liquid chromatography9 and for PL content using Phospholipids B (Wako) enzymatic assay kit11, 12. The

aqueous phase was analyzed for BA content by an enzymatic assay using

hydroxysteroid dehydrogenase13, 14.

Fecal Neutral Sterol excretion: After being fed the synthetic diets for 5 weeks,

mice were singly housed on wire bottom cages. After 3 days, the feces were

collected, dried in a 70°C vacuum oven, weighed, and crushed into a fine powder. A measured mass (50–100 mg) of feces was placed into a glass tube containing 135 μg of 5α-cholestane as an internal standard. The feces were saponified and the neutral lipids were extracted into hexane as described above.

Mass analysis of the extracted neutral sterols was conducted by gas-liquid

chromatography as described previously9. Fecal neutral cholesterol mass

represents the sum of cholesterol, coprostanol, and coprostanone in each

sample.

Statistical Analyses and Data Presentation: Data are expressed as the mean

± SEM. Significance of differences was determined for each group of values by

ANOVA (Tukey-Kramer honestly significant difference) or unpaired t-test.

A p value < 0.05 was considered significant. All analyses were performed using

JMP version 5.0.12 software (SAS Institute, Inc., Cary, NC).

65

RESULTS

In order to test whether hepatic knockdown of ABCG5/G8 function would result in phytosterol accumulation, an ABCG8 ASO was used to decrease hepatic ABCG8 mRNA levels in C57Bl/6 mice. Mice treated with a non-targeting control ASO

(CON) and the ABCG8 hepatic knockdown (G8HKD) mice were challenged with

diets containing different amounts of sterols (Supplemental Figure I). The low

sterol (LS) diet contained 0.003% cholesterol and 0.01% phytosterol. The high

cholesterol (HC) diet contained 0.2% cholesterol and 0.01% phytosterol. The

high phytosterol (HP) diet contained 0.003% cholesterol and 0.2% phytosterol.

All three diets were identical otherwise (Supplemental Table I). The predominant

phytosterol species in all diets was sitosterol (%), followed by campesterol (%)

and stigmasterol (%) (Supplemental Figure I).

66

Low Sterol High Cholesterol High Phytosterol

g of ingredient/100g of diet

Fish Oil (Omega Protein) 0.2000 0.2000 0.2000

Palm Oil 4.0000 4.0000 4.0000

Casein, USP 8.0000 8.0000 8.0000

Lactalbumin 4.0000 4.0000 4.0000

Dextrin 17.0000 17.0000 17.0000

Sucrose 17.0000 17.0000 17.0000

Wheat Flour, self-rising 35.0000 35.0000 35.0000

Alphacel 7.2687 7.0688 7.0687

Crystalline Cholesterol 0.0000 0.2000 0.0000

Vitamin Mixture, Teklad 2.5000 2.5000 2.5000

Hegsted Salt Mixture 5.0000 5.0000 5.0000

B-sitosterol (ICN) 0.0103 0.0103 0.2103

Tenox 20A 0.0018 0.0018 0.0018

MTS-50 0.0191 0.0191 0.0191

Supplemental Table I: Diet Ingredients. All diets are comprised of 12% of energy as lipid, 71% of energy as carbohydrate, and 18% of energy as protein.

67

Supplemental Figure I: Dietary Sterol Content and Composition. Sterols were extracted from diet samples and analyzed by gas-liquid chromatography. IA) Dietary sterol content expressed as mg of sterol/100g dry weight. IB) Dietary sterol composition expressed as the percentage of individual sterol species to total sterols.

68

We chose to feed the HP diet in order to examine whether a large amount of dietary phytosterol would be required to detect phytosterol accumulation in G8HKD

mice. Additionally, we fed the HC diet in order to determine whether phenotypic

effects seen in G8HKD mice were specific to the type of dietary sterol that was fed.

Since it has been well established that whole body ABCG5/G8 knockout (KO)

mice accumulate significant amounts of plasma and tissue plant sterols, we fed

ABCG5/G8 KO mice and their wild type (WT) littermates all three diets to

compare to the CON and G8HKD mice.

ABCG8 ASO treatment decreases hepatic RNA and protein levels

In order to determine the effectiveness of our ABCG8 ASO, we measured

hepatic RNA and protein levels of ABCG8. In all groups treated with the ABCG8

ASO, hepatic ABCG8 RNA levels were decreased (Figure 1A). Compared to

CON mice, hepatic ABCG8 RNA was decreased by 83% in the G8HKD mice on

the LS diet, 82% on the HC diet, and 69% on the HP diet. These decreases in

hepatic RNA translated to decreases in hepatic ABCG8 protein expression as

well (Figure 1C). Hepatic ABCG8 protein expression was decreased in the G8HKD mice on all diets when compared to CON mice. As expected, administration of the ABCG8 ASO had no effect on the hepatic mRNA levels of ABCG5 (Figure

1B).

69

Figure 1. ABCG8 and ABCG5 expression. Liver and duodenum were collected from CON and G8HKD mice at necropsy. RNA and membrane proteins were isolated as described in the methods section. Gene expression for individual

70 samples was measured by rt-PCR. Average units were calculated and normalized to β-actin. A) Hepatic ABCG8 RNA expression. B) Hepatic ABCG5 RNA expression. C) Duodenal ABCG8 RNA expression. D) Duodenal ABCG5 RNA expression. Data are expressed as mean±SEM (n=4-5 per diet group). Data analyzed by 2-way ANOVA followed by Student t tests for post hoc analysis. Bars that do not share a common letter are significantly different (p<0.05). Membrane proteins from liver and duodenum (15μg) were fractionated by 4-12% polyacrylamide gel in the presence of SDS and immunoblotted with an anti- ABCG8 antibody. E) Gel shows hepatic ABCG8. F) Gel shows duodenal ABCG8.

71

ASOs preferentially target gene expression in the liver. High doses and long term treatment can, however, cause RNA knockdown in other tissues. Since

ABCG5/G8 is also expressed in the small intestine, we measured small intestinal

RNA and protein levels. ABCG8 ASO treatment did decrease small intestinal

RNA levels by 45% on the LS diet, 26% on the HC diet, and 43% on the HP diet when compared to CON ASO treatment (Figure 1D). These decreases in mRNA levels translated only to minimal decreases in small intestinal ABCG8 protein expression (Figure 1F). Administration of the ABCG8 ASO had no effect on duodenal mRNA levels of ABCG5 (Figure 1E).

G8HKD mice have decreased biliary cholesterol concentrations

To further test the effectiveness of our ABCG8 ASO, we measured biliary lipids in

G8HKD mice and compared them to ABCG5/G8 KO mice. Since ABCG5/G8 function is critical for biliary cholesterol secretion, knocking down hepatic ABCG8 should decrease biliary cholesterol concentrations. Similar to previous reports,

ABCG5/G8 KO mice have almost no biliary cholesterol (Figure 2A). This observation in ABCG5/G8 KO mice is independent of the amount of dietary sterol fed. Biliary cholesterol concentrations in G8HKD mice were also significantly

decreased in all dietary groups (Figure 2B). When compared to CON mice, biliary

cholesterol concentrations were decreased in the G8HKD mice by 80% on the LS

diet, 72% on the HC diet, and 65% on the HP diet. The amount of dietary

cholesterol decreased the effectiveness of the ABCG8 ASO, which translated to

72 a less impressive decrease in biliary cholesterol concentration in G8HKD mice on the HC diet. Biliary phospholipid and biliary bile acid concentrations are largely unaffected in both ABCG5/G8 KO and G8HKD mice (Supplemental Figure II).

73

Figure 2. Biliary cholesterol concentration. Sterols were extracted from the gall bladder bile of WT, ABCG5/G8 KO, CON, and G8HKD mice and measured by gas-liquid chromatography. Biliary cholesterol concentration is expressed as μmol/mL of bile. Data are expressed as mean±SEM (n=3-8 per group). Data analyzed by 2-way ANOVA followed by Student’s t test for post hoc analysis. Bars that do not share a common letter are significantly different (p<0.05).

74

Supplemental Figure II: Biliary Lipid Composition. Lipids were extracted from the gall bladder bile of WT, ABCG5/G8 KO, CON, and G8HKD mice and analyzed by enzymatic assays for phospholipid and bile acid content. Biliary lipid concentration is expressed as μmol of lipid/mL of bile. Data are expressed as mean±SEM (n=3-8 per group). Data analyzed by 2-way ANOVA followed by Student t tests for post hoc analysis. Bars that do not share a common letter are significantly different (p<0.05).

75

G8HKD mice have a normal outward appearance when fed HP diet

As we have previously shown, feeding a HP diet to ABCG5/G8 KO mice is

extremely toxic. These mice failed to gain weight, died prematurely, and

accumulated very high levels of plant sterols in many tissues which seemed to

cause liver abnormalities and severe cardiac lesions. When compared to the

ABCG5/G8 KO mice fed the HP diet, ABCG5/G8 KO mice fed the LS or HC diet

accumulated less phytosterol in liver and plasma (Figure 3B and Figure 4A) and

appeared phenotypically normal. G8HKD mice fed LS, HC, or HP diets also

appeared phenotypically normal. The mice gained weight normally

(Supplemental Figure III) and did not die prematurely (unpublished observation,

ALM). Liver to bodyweight ratios were not different from CON mice in the G8HKD

mice fed LS or HP diets (Supplemental Figure III). There was, however, a

significant increase in the liver size of G8HKD mice fed the HC diet. Livers of these

mice appeared large and pale at the time of necropsy (unpublished observation,

ALM).

76

Supplemental Figure III: Body and liver weights of CON and G8HKD mice. IIA) Percent change in body weight from baseline after six weeks of diet and ASO treatment. IIB) Liver weight as a percentage of body weight after six weeks of diet and ASO treatment. Data are expressed as mean±SEM (n=4-5 per group). Data analyzed by 2-way ANOVA followed by Student t tests for post hoc analysis. Bars that do not share a common letter are significantly different (p<0.05).

77

G8HKD mice do not accumulate high levels of plasma phytosterols

As others have reported, ABCG5/G8 KO mice accumulate high levels of phytosterol in plasma. Plasma phytosterol concentrations in ABCG5/G8 KO mice ranged from 60-257mg/dL depending on the diet fed (Figure 3B). ABCG5/G8 KO

mice fed the HP diet have the highest concentration of plasma phytosterol

(257mg/dL), followed by ABCG5/G8 KO mice fed the LS diet (131mg/dL) and the

HC diet (60mg/dL). These values were significantly higher than all WT groups

who had plasma phytosterol concentrations of less than 5mg/dL. When

expressed as a percentage, whole body ABCG5/G8 deficiency results in a high

percentage of total plasma sterols as plant (24-74%) (Figure 3D). ABCG5/G8 KO

mice fed the HP diet have the highest percentage of plasma phytosterol (74%),

followed by ABCG5/G8 KO mice fed the LS diet (52%) and the HC diet (24%).

The predominant phytosterol species that accumulated in ABCG5/G8 KO mice

was sitosterol, which was also the main phytosterol species in our diets.

78

79

Figure 3. Plasma sterol concentrations. Sterols were extracted from the plasma of WT, ABCG5/G8 KO, CON, and G8HKD mice and measured by gas- liquid chromatography. 2A & 2E) Plasma total sterol concentrations. 2B & 2F) Plasma phytosterol concentrations. 2C & 2G) Plasma cholesterol concentrations. 2D & 2H) Individual sterol species as a percentage of total plasma sterol concentration. Data are expressed as mean±SEM (n=4-10 per group). Data analyzed by 2-way ANOVA followed by Student’s t test for post hoc analysis. Bars that do not share a common letter are significantly different (p<0.05).

80

Hepatic specific knockdown of ABCG5/G8 function did result in a statistically significant increase in plasma phytosterol levels in G8HKD mice compared to CON

mice on the LS and HP diets, but not the HC diet (Figure 3F). The increases

were, however, minimal with plasma phytosterol concentrations reaching a

maximum of 15mg/dL in the G8HKD mice fed HP diet. G8HKD mice fed the HP diet

have the highest concentration of plasma phytosterol (15mg/dL), followed by

G8HKD mice fed the LS diet (5mg/dL) and the HC diet (0.4mg/dL). When

expressed as a percentage, G8HKD mice accumulate only a small percentage of

total plasma sterols as plant (0.2-13%) (Figure 3H). G8HKD mice fed the HP diet have the highest percentage of plasma phytosterol (13%), followed by G8HKD

mice fed the LS diet (4%) and the HC diet (0.2%). The predominant phytosterol

species that accumulated in G8HKD mice was campesterol, which differed from

the ABCG5/G8 KO mice that predominantly accumulated sitosterol.

Plasma cholesterol levels are significantly reduced in ABCG5/G8 KO mice compared to WT mice on the LS and HP diets, and not changed on the HC diet

(Figure 3C). Further confirming that G8HKD mice are protected from the

ABCG5/G8 KO phenotype, there were no significant reductions in any G8HKD

plasma cholesterol levels compared to CON mice (Figure 3G). In fact, plasma

cholesterol was doubled in G8HKD mice compared to CON mice fed the HC diet.

This significant increase in plasma cholesterol concentration was primarily in

VLDL and HDL fractions (Supplemental Figure IV).

81

Supplemental Figure IV: Plasma Lipoprotein Sterol Distribution. Plasma lipoprotein sterol distributions were determined by online gel-filtration HPLC using Infinity Cholesterol reagent. TL indicates Transition Lipoprotein. IIIA-IIIC) 10μL of plasma from 5 WT mice per diet group (solid line) or 5 ABCG5/G8 KO mice per diet group (dashed line) mice was pooled for analysis. Tracings

82 represent the values for pooled samples. IIID-IIIF) Plasma sterol from CON (n=4- 5 per diet group; solid line) and G8HKD (n=5 per diet group; dashed line) mice was analyzed. Tracings represent the average of values for individual mice.

83

G8HKD mice do not accumulate large amounts of hepatic phytosterol

As expected, ABCG5/G8 KO mice accumulate significant amounts of phytosterol

in liver (Figure 4A). The amount of hepatic phytosterol detected (1.8-6.2μg/mg

wet weight) depended on the amount of dietary sterol mice are fed. ABCG5/G8

KO mice fed the HC diet accumulated the most hepatic phytosterol (6.2ug/mg

wet weight), followed by ABCG5/G8 KO mice fed the HP diet (3.0μg/mg wet

weight) and the LS diet (1.8μg/mg wet weight). These values were significantly higher than all WT groups who had hepatic phytosterol concentrations of less

than 0.3μg/mg wet weight. It is surprising that ABCG5/G8 KO mice fed the HC

diet accumulated three times more hepatic phytosterol than the ABCG5/G8 KO

mice fed HP diet, since the HC diet contained much less phytosterol than the HP

diet. When expressed as a percentage of total hepatic sterol, however,

ABCG5/G8 KO mice fed the HP diet have the highest percentage of hepatic

phytosterol (77%), followed by ABCG5/G8 KO mice fed the LS diet (55%) and

the HC diet (13%) (Figure 4B). The predominant phytosterol species that

accumulated in ABCG5/G8 KO mice was sitosterol, which was also the main

phytosterol species in our diets. All ABCG5/G8 KO mice accumulated a

significant amount of phytosterol in the unesterified form (Figure 4C). Only

ABCG5/G8 KO mice fed the HC diet were able to accumulate a significant

amount of esterified phytosterol (Figure 4D).

84

85

Figure 4. Liver sterol concentrations. Sterols were extracted from the livers of WT, ABCG5/G8 KO, CON, and G8HKD mice and measured by gas-liquid chromatography. All hepatic lipid values were normalized to the wet weight of the extracted piece of liver. 2A & 2E) Total hepatic sterol concentrations of cholesterol and phytosterols. 2B & 2F) Individual sterol species as a percentage of total hepatic sterol. 2C & 2G) Hepatic free sterol concentrations of cholesterol and phytosterols. 2D & 2H) Hepatic esterified sterol concentrations of cholesterol and phytosterols. Hepatic esterified sterol was calculated by multiplying the mass difference between total sterol and free sterol by 1.67. Data are expressed as mean±SEM (n=4-9 per group). Data analyzed by 2-way ANOVA followed by Student’s t test for post hoc analysis. Bars that do not share a common letter within the sterol statistics row are significantly different (p<0.05).

86

When fed the same diets, G8HKD mice do have a significant increase in hepatic

phytosterol concentrations compared to CON mice on the HC and HP diets, but

not the LS diet (Figure 4E). The increases were, however, minimal with hepatic

phytosterol concentrations reaching a maximum of 0.55μg/mg wet weight in the

G8HKD mice fed HP diet. G8HKD mice fed the HP diet have the highest

concentration of hepatic phytosterol (0.55μg/mg wet weight), followed by G8HKD mice fed the HC diet (0.51μg/mg wet weight) and the LS diet (0.19μg/mg wet weight). When expressed as a percentage of total hepatic sterols, G8HKD accumulate 0.7-11% of sterol as phytosterol in the liver. G8HKD fed the HP diet

have the highest percentage of hepatic phytosterol (11%), followed by G8HKD

mice fed the LS diet (4%) and the HC diet (0.7%) (Figure 4F). The predominant

phytosterol species that accumulated in the G8HKD mice was campesterol, which differed from the ABCG5/G8 KO mice that predominantly accumulated sitosterol.

The minor amount of hepatic phytosterol found in G8HKD mice was mostly stored

in esterified form (Figure 4G and H).

There was no significant difference in the amount of hepatic cholesterol

measured between WT and ABCG5/G8 KO mice on any diet (Figure 4A). There

was also no significant difference in the amount of hepatic cholesterol measured

between WT and G8HKD mice on the LS or HP diet (Figure 4E). Interestingly,

there was a significant 5.7 fold increase in hepatic cholesterol concentration in

G8HKD mice compared to CON mice when fed the HC diet.

87

ABCG5/G8 KO and G8HKD mice have reduced FNS excretion when fed HC

diet

In order to get a more complete picture of sterol balance in our mouse models, we measured FNS excretion. ABCG5/G8 KO mice had no significant differences in fecal neutral phytosterol excretion when compared to WT mice on any of the diets (Figure 5A). We did see a large increase in fecal neutral phytosterol excretion in both WT and ABCG5/G8 KO mice fed the HP diet. There were no differences in fecal neutral cholesterol excretion in ABCG5/G8 KO mice compared to WT mice on the LS and HP diets. We did, however, measure a significant reduction in fecal neutral cholesterol excretion in ABCG5/G8 KO mice on the HC diet when compared to WT.

88

Figure 5. Fecal neutral sterol excretion. Neutral sterols were extracted from the feces of WT, ABCG5/G8 KO, CON, and G8HKD mice and measured by gas- liquid chromatography. Fecal neutral sterol excretion of cholesterol and phytosterols was normalized to the number of days feces were collected and mouse body weights. Data are expressed as mean±SEM (n=4-9 per group). Data analyzed by 2-way ANOVA followed by Student’s t test for post hoc analysis. Bars that do not share a common letter within the sterol statistics row are significantly different (p<0.05).

89

Similarly, G8HKD mice had no significant differences in fecal neutral phytosterol

excretion when compared to CON mice on any of the diets (Figure 5B). Both

CON and G8HKD mice that were fed the HP diet had large increases in fecal

neutral phytosterol excretion. There were no differences in fecal neutral

cholesterol excretion in G8HKD mice compared to CON mice on the LS and HP

diets. Interestingly, we also measured a highly significant reduction in fecal

neutral cholesterol excretion in G8HKD mice compared to CON mice on the HC

diet.

G8HKD mice are protected from further phytosterol accumulation after 12

weeks of treatment

In order to determine whether the amount of phytosterol accumulation in G8HKD

mice would increase over time, we treated C57Bl/6 mice with control ASO or

ABCG8 ASO and fed the HP diet for 12 weeks. On the HP diet, the G8HKD mice treated for 6 weeks accumulated a small amount of hepatic phytosterol

(0.55μg/mg wet weight) (Figure 4E). When diet and ASO treatment were increased to 12 weeks, the G8HKD mice only increased hepatic phytosterol

accumulation slightly (0.68μg/mg wet weight) (Supplemental Figure VA).

Additionally, the percentage of total hepatic sterols as plant increased from 13%

after 6 weeks to 16% after 12 weeks of treatment (Supplemental Figure VB).

Hepatic free phytosterols in G8HKD mice increased to 0.35μg/mg wet weight and

90 hepatic esterified phytosterols decreased to 0.55μg/mg wet weight after 12 weeks of treatment (Supplemental Figure VC and D).

91

Supplemental Figure V: Liver sterol concentrations after 12 weeks of G8HKD and high phytosterol diet feeding. C57Bl/6 mice were fed the high phytosterol diet and treated with CON or ABCG8 ASO for 12 weeks. Sterols were extracted from liver and measured by gas-liquid chromatography. All hepatic lipid values were normalized to the wet weight of the extracted piece of liver. VA) Total hepatic sterol concentrations. VB) Individual sterol species as a percentage of total hepatic sterol. VC) Hepatic free sterol concentrations of cholesterol and total phytosterols. VD) Hepatic esterified sterol concentrations of cholesterol and total phytosterols. Hepatic esterified sterol was calculated by multiplying the mass difference between total sterol and free sterol by 1.67. Data are expressed as mean±SEM (n=4 per group). Data analyzed by 2-way ANOVA followed by Student t tests for post hoc analysis. Bars that do not share a common letter within the sterol statistics row are significantly different (p<0.05).

92

DISCUSSION

The major finding of this study is that liver-specific impairment of ABCG5/G8 function does not result in high levels of phytosterol accumulation. Compared to their WT counterparts, mice with whole body ABCG5/G8 deficiency had very high plasma and hepatic phytosterol concentrations in a dietary sterol dependent manner. The G8HKD mice did not achieve these high levels of plasma and hepatic

phytosterol. Therefore, intestinal ABCG5/G8 function is sufficient to prevent high

levels of plant sterol accumulation in mice. This supports the idea that small

intestinal ABCG5/G8 is part of the body’s first line of defense in preventing

dietary plant sterol buildup. When small intestinal ABCG5/G8 is functional, it

appears that hepatic ABCG5/G8 serves as a backup to secrete into bile any plant

sterols that do get absorbed.

Although the G8HKD mice did not accumulate as much plasma and liver plant

sterols as the ABCG5/G8 KO mice on the same diets, G8HKD plasma and liver

plant sterol concentrations were still significantly elevated when compared to

their CON counterparts. The small amount of phytosterol present in G8HKD mice was primarily campesterol. ABCG5/G8 whole body knockout mice also accumulated significant amounts of campesterol, but the primary phytosterol species in their liver and plasma was sitosterol. The same finding was reported in

ABCG5/G8 KO mice by Yu, L et al2. These observations could mean that campesterol is the first phytosterol species to accumulate under conditions of dietary challenge or alterations of hepatic ABCG5/G8 function. Since

93 campesterol is more efficiently absorbed than sitosterol1, 15, it follows that

campesterol would be the first plant sterol species to accumulate.

The majority of hepatic phytosterols in the ABCG5/G8 KO mice on the LS and

HP diets were free sterol. One explanation for this could be related to the

availability of sterols for incorporation into plasma membranes. Since a large

percentage of the total hepatic sterols in our ABCG5/G8 KO mice on the LS and

HP diets were phytosterols (55-75%), the phytosterols were likely used in their

free form to help maintain cellular membrane structures. This idea could be supported by our data from the ABCG5/G8 KO mice fed the HC diet. Those mice had a much higher concentration of hepatic cholesterol, likely resulting in less membrane incorporation and more esterification and storage of phytosterols.

Alternatively, it is known that the sterol esterifying ACAT2 (acyl-

CoA:cholesterol O-acyltransferase 2) preferentially selects cholesterol over phytosterols for esterification9. This could also explain why the majority of hepatic

phytosterols were in the free form in ABCG5/G8 KO mice fed LS and HP diets.

Since ABCG5/G8 is required for biliary sterol secretion1, 16, its crucial role in

biliary RCT is firmly established. RCT is traditionally defined as the transport of excess peripheral cholesterol to the liver via HDL where it is then secreted into

bile and excreted in the feces 17. Until recently, biliary secretion was the

universally accepted pathway by which peripheral cholesterol was excreted from

the body in the feces. If biliary cholesterol excretion was the only contributor to

94 fecal sterol loss, one would expect dramatically decreased fecal sterol output to accompany decreases in biliary cholesterol levels. This is not the case, however, in several mouse models that exhibit little to no biliary cholesterol secretion 18-20.

Along with several studies conducted in rats, dogs, and humans 18, 21-23, these

observations have led our group and others to the discovery of a novel pathway

for non-biliary cholesterol excretion which is called transintestinal cholesterol

excretion (TICE).

The hallmark features of models that primarily use the TICE pathway to excrete

cholesterol are severly diminished biliary cholesterol secretion, with no

accumulation of hepatic cholesterol due to normal levels of fecal neutral sterol

excretion. Since our G8HKD mice had dramatically decreased levels of biliary

cholesterol, we predicted that the TICE pathway would compensate for the loss

of biliary sterol secretion, resulting in normal FNS excretion and no accumulation

of hepatic cholesterol in the G8HKD mice. This appears to be the case when comparing G8HKD mice on the LS and HP diets to the CON mice. Despite the more than 80% reduction in biliary cholesterol levels, G8HKD mice had levels of

FNS excretion and hepatic cholesterol similar to CON mice on the LS and HP

diets.

Surprisingly, we found an opposite result in G8HKD mice fed the HC diet. G8HKD

mice on the HC diet had more than a 70% reduction in biliary cholesterol

concentration. The high level of dietary cholesterol fed to these mice unmasked a

95 significant reduction in fecal neutral sterol excretion and a dramatic increase in hepatic cholesterol accumulation when compared to CON mice. These data suggest that the G8HKD mice have a disfunction in the TICE pathway and

subsequently cannot compensate for the reduction in biliary sterol secretion with

the dietary cholesterol challenge.

In 2003, Yu, L et al24 reported that ABCG5/G8 is required for LXR agonist

induced increases in fecal neutral sterol excretion. Presumably, since biliary

cholesterol secretion could not be increased with an LXR agonist due to

ABCG5/G8 deficiency, fecal neutral sterol excretion also could not be increased.

Several years later, multiple studies showed the existence of the TICE pathway

and that it could compensate for loss of biliary sterol secretion18-23. In 2009, van

der Veen et al25 showed that the TICE pathway could be strongly stimulated by

LXR activation. Since fecal neutral sterol excretion could not be stimulated in

ABCG5/G8 KO mice treated with an LXR agonist, these historic studies support

the idea that ABCG5/G8 may play an important role in the TICE pathway. More

specifically, our data from the G8HKD mice suggest that it is hepatic ABCG5/G8

function that may be required for the TICE pathway to operate. Alternatively, it is

possible that the decreased biliary cholesterol secretion is causing the increased

heptic cholesterol levels in G8HKD mice fed a high cholesterol diet, not a disfunctional TICE pathway. Further studies need to be done to confirm what our data suggest.

96

The findings from this study show that hepatic ABCG5/G8 function is not necessary to prevent bodily phytosterol accumulation and support a novel tissue specific role for hepatic ABCG5/G8 in cholesterol metabolism. These initial results generated using ASO technology highlight the importance of developing a genetic mouse model of complete tissue-specific ABCG5/G8 deficiency in which to perform additional studies. These future studies have the potential to unveil the complete role of ABCG5/G8 in hepatic sterol metabolism.

97

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102

CHAPTER IV

HEPATIC ABCG8 KNOCKDOWN PREVENTS LXR AGONIST INDUCED REVERSE CHOLESTEROL TRANSPORT

Allison L. McDaniel, Lawrence L Rudel, J. Mark Brown, Ryan E. Temel

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ABSTRACT

Key regulators of ABCG5/G8 expression are the nuclear receptors liver x receptor (LXR) α and LXRβ. LXR activation using synthetic agonists leads to increased fecal neutral sterol loss in mice, presumably because ABCG5/G8 mediates an increase in biliary cholesterol concentration. There is evidence that

ABCG5/G8’s role in RCT may be tissue-specific. In liver-specific LXRα knockout mice, cholesterol excretion and macrophage RCT were not stimulated upon LXR agonist treatment. Because ABCG5/G8 is transcriptionally regulated by LXR, hepatic ABCG5/G8 mRNA was not induced with LXR agonist treatment in those mice. Taken together, these studies suggest that hepatic ABCG5/G8, a downstream target of LXR, may be required for LXR mediated increases in RCT.

In order to test whether hepatic ABCG5/G8 function is necessary for LXR agonist mediated increases in cholesterol excretion and macrophage reverse cholesterol transport, an anti-sense oligonucleotide (ASO) targeting ABCG8 was used to knockdown ABCG8 expression in the liver of C57Bl/6 mice and RCT was measured. Interestingly, when mice had decreased hepatic ABCG8 expression, cholesterol excretion and macrophage RCT were not stimulated with LXR agonist treatment. This data suggest that it is ABCG5/G8, a downstream target of

LXR, that is required for LXR stimulated increases in cholesterol excretion and macrophage RCT.

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INTRODUCTION

Reverse cholesterol transport (RCT) is an important pathway that helps prevent

excess accumulation of cholesterol in peripheral tissues. RCT is defined as the

movement of cholesterol from peripheral tissues to the liver via HDL or when

cholesteryl ester transfer protein is present, LDL1. Once cholesterol reaches the

liver it can be secreted into the bile by the ATP-binding cassette transporters G5

and G8 (ABCG5/G8)2. Biliary cholesterol that reaches the lumen of the small intestine can then be reabsorbed or excreted in the feces. Because of its critical role in biliary cholesterol secretion, ABCG5/G8 can significantly affect the amount of biliary cholesterol available for excretion into the feces.

Key regulators of ABCG5/G8 expression are the nuclear receptors liver x receptor (LXR) α and LXRβ. LXR activation using synthetic agonists leads to increased fecal neutral sterol loss in mice3. Presumably this increase is caused

by an ABCG5/G8 mediated increase in biliary cholesterol concentration since

ABCG5/G8 KO mice did not have increased fecal neutral sterol excretion when

treated with an LXR agonist4. It has also been shown that LXR agonist stimulated

macrophage RCT is impaired in ABCG5/G8 KO mice5. From these global

knockout studies, it is clear that ABCG5/G8 plays an important role in LXR

stimulated cholesterol excretion and macrophage RCT.

Interestingly, there is evidence that the role of ABCG5/G8 in RCT may be tissue-

specific. In liver-specific LXRα knockout mice, cholesterol excretion and

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macrophage RCT were not stimulated upon LXR agonist treament6. Because

ABCG5/G8 is transcriptionally regulated by LXR, hepatic ABCG5/G8 mRNA was

not induced with LXR agonist treatment in those mice. Taken together, these

studies suggest that hepatic ABCG5/G8, a downstream target of LXR, may be

required for LXR mediated increases in RCT.

We hypothesized that knocking down hepatic ABCG5/G8 function would

decrease LXR stimulated cholesterol excretion and macrophage RCT. In order to

test this hypothesis, an anti-sense oligonucleotide (ASO) targeting ABCG8 was

used to knockdown ABCG8 expression in the liver of C57Bl/6 mice and

macrophage RCT was measured. Indeed, when mice had decreased hepatic

ABCG8 expression, cholesterol excretion and macrophage RCT were not

stimulated with LXR agonist treatment.

METHODS

Animals and diet: Female C57Bl/6 mice 6-8 weeks of age were ordered from

Harlan Laboratories (Indianapolis, IN). At 7-9 weeks of age, mice were fed a low- fat (10% of energy as palm oil enriched fat), low sterol (0.01% (w/w) phytosterols,

0.003% (w/w) cholesterol) synthetic diet for 6 weeks. The diets were made at the

Wake Forest University Primate Center Diet Laboratory. In conjunction with diet

feeding, mice received bi-weekly intraperitoneal injections of a nontargeting

control ASO or ABCG8 ASO (50mg/kg/week). The 20-mer phosphorothioate

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ASOs were designed to contain 2'-0-methoxyethyl groups at positions 1 to 5 and

15 to 20, and were synthesized, screened, and purified as described previously7 by ISIS Pharmaceuticals (Carlsbad, CA).

All mice were fed ad libitum a standard rodent chow diet (5P00Prolab; LabDiet) prior to the start of the synthetic diet and had free access to water. Mice were housed in a specific pathogen-free animal facility in plastic cages in a temperature-controlled room (22°C) with a daylight cycle from 6AM to 6PM.

Experimental animals were euthanized following a 4 h fast during the light cycle.

All experimental protocols were approved by the Institutional Animal Care and

Use Committee at the Wake Forest University School of Medicine.

J774 Cell Culture and [3H]-Cholesterol Loading: J774 mouse macrophages were a generous gift from Dr. George Rothblat (The Children’s Hospital of

Philadelphia). Cells were grown in RPMI-1640 medium supplemented with 10% fetal bovine serum (FBS), 100 U/ml penicillin, and 100 μg/ml streptomycin. [3H]-

Cholesterol loading was initiated by incubating cells for 48 hours with 5 μCi/ml

[3H]-cholesterol and 100 μg/ml acetylated LDL in 10% FBS containing RPMI-

1640. The resulting foam cells were washed twice with phosphate buffered saline and equilibrated for an additional 12-hour period in serum free RPMI-1640 supplemented with 0.2%bovine serum albumin (BSA). Cells were then harvested and resuspended in serum-freeRPMI-1640 immediately before injection. On average, the cell suspension contained ~10x106 cells/ml at ~3x106 dpm/ml. All

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cell suspensions were analyzed microscopically in order to count and to ensure

viability before injection, and all mice were injected within 5 minutes of

resuspension of freshly isolated foam cells.

In Vivo Macrophage RCT: In vivo measurement of macrophage RCT was

conducted essentially as described by Rader and colleagues (Zhang et al., 2003;

Naik et al. 2006), with minor modifications. Briefly, mice were gavaged with either

vehicle or 25 mg/kg T0901317 daily for seven consecutive days. On the 5th day

of treatment, mice were injected intraperitoneally with ~500 μl [3H]-cholesterol labeled foam cell suspension containing ~10x106 cells/ml at ~3x106 dpm/ml. To allow quantitative fecal collection, mice were housed individually on wire bottom cages for 48 hours with ad libitum access to food and water. At 6, 24, and 48 hours post injection, blood was collected via the submandibular vein, and 20 μl of isolated plasma was used to determine [3H]-cholesterol recovery.

Measurement of Biliary, Plasma, and Hepatic lipid concentrations and [3H]-

cholesterol recovery: At necropsy, blood was collected by heart puncture and

was placed into a tube containing protease inhibitor cocktail (Sigma) dissolved in

5% EDTA, 5% NaN3. Gallbladder bile was collected, and then the liver was

removed, weighed, and snap-frozen in liquid N2. The small intestine from the

pyloric valve to the cecum was removed, cleaned of fat and luminal contents

while on ice, and cut into either three sections of equal length. The intestinal

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sections were snap-frozen in liquid N2 and stored along with the liver and bile samples at −80°C.

Blood was centrifuged at 12,000 g for 10 min at 4°C, and plasma lipids were extracted with 2:1 CHCl3/methanol in the presence of 21 μg 5α-cholestane at

room temperature overnight. The lipid extract was dried down under N2 and

saponified by adding 1mL ethanol and 100μL 50% KOH and heating at 60°C for

1 hour. Neutral lipids were extracted by adding hexane and deionized water, vortexing, and centrifuging at 2,000 g for 10 min. The hexane phase was then analyzed by gas-liquid chromatography8 for total sterol content. To determine

plasma lipoprotein sterol distribution, lipoprotein classes were separated by gel

filtration chromatography as described previously9.

For analysis of the liver lipid composition, ∼100 mg of liver was thawed, minced, and weighed in a glass tube. Lipids were extracted with 2:1 CHCl3/methanol in

the presence of 135 μg 5α-cholestane at room temperature overnight. Following

extraction, a measured volume of solvent was dried down under N2 and

resuspended in scintillation cocktail for count recovery determination. Total tissue

recovery is calculated per total organ weight. The remaining lipid extract was

dried down under N2 and redissolved in a measured volume of 2:1

CHCl3/methanol. Dilute H2SO4 was added to the sample, which was then

vortexed and centrifuged to split the phases. An aliquot of the organic phase was

dried down under N2, dissolved in hexane, and analyzed for free sterol content

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by gas-liquid chromatography8. The remaining organic phase was saponified by

adding 2mL ethanol and 200μL 50% KOH and heating at 60°C for 2 hours.

Neutral lipids were extracted by adding hexane and deionized water, vortexing, and centrifuging at 2,000 g for 10 min. The hexane phase was then analyzed by gas-liquid chromatography8 for total sterol content.

For analysis of biliary lipid concentrations, a measured volume (3–10 μl) of bile was extracted with 2:1 CHCl3/MeOH in the presence of 10 μg 5α-cholestane. The organic phase was analyzed for sterol content by gas-liquid chromatography8 and for PL content using Phospholipids B (Wako) enzymatic assay kit10, 11. The

aqueous phase was analyzed for BA content by an enzymatic assay using

hydroxysteroid dehydrogenase12, 13.

Fecal Neutral Sterol excretion and [3H]-cholesterol recovery: After 3 day

fecal collection, the feces were dried in a 70°C vacuum oven, weighed, and

crushed into a fine powder. A measured mass (50–100 mg) of feces was placed

into a glass tube containing 135 μg of 5α-cholestane as an internal standard. The feces were saponified and the neutral lipids were extracted into hexane as described above. Following extraction, a measured volume of solvent was dried

3 down under N2 and resuspended in scintillation cocktail for [ H] recovery determination. Mass analysis of the extracted neutral sterols was conducted by gas-liquid chromatography as described previously8. Fecal neutral cholesterol

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mass represents the sum of cholesterol, coprostanol, and coprostanone in each

sample.

The [3H] bile acid-containing aqueous phase was acidified by adding 200μL HCl.

The acidified aqueous phase (pH <1) was then extracted 6 times with 2 ml

hexane to quantitatively recover [3H]-bile acids. All [3H]-bile acid hexane phases

were pooled, dried under N2, and resuspended in scintillation cocktail for [3H] recovery determination.

Real Time Polymerase Chain Reaction (RT-PCR) analysis of gene expression in liver and duodenum: Total mRNA was extracted from ∼100 mg of liver and small intestinal segment 2 with Trizol (Invitrogen Life Technologies) using the protocol provided by the manufacturer. The mRNA was resuspended in diethyl pyrocarbonate water, and 1 μg of mRNA was reverse transcribed to cDNA using qScript cDNA SuperMix (Quanta Biosciences) under the following conditions: 25°C for 5 min, 42°C for 30 min, and 85°C for 5 min. The cDNA was diluted 1:10 using diethyl pyrocarbonate water, and real-time PCR was done in triplicate with 5 μl of cDNA, 10 μl of SYBR GREEN PCR master mix (Applied

Biosystems), 3 μl of diethyl pyrocarbonate water, and 1 μl of forward and reverse primer (20 pmol) for a final reaction volume of 20 μl. The primer sequences are as follows: ABCG8 (F: 5’-AAC CCT GCG GAC TTC TAC G; R: 5’-CTG CAA

GAG ACT GTG CCT TCT); ABCG5 (F: 5’-TCC TGC ATG TGT CCT ACA GC; R:

5’-ATT TGC CTG TCC CAC TTC TG); Cyclophilin (F: 5’-GCG GCA GGT CCA

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TCT ACG; R: 5’-TCC ATC CAG CCA TTC AGT C). PCR was then run on the

Sequence Detection System 7500 (Applied Biosystems) using the following

conditions: 50°C for 2 min, 95°C for 10 min, and 40 cycles of 95°C for 10 s and

60°C for 30 s. The fluorescence measurement used to calculate threshold cycle

(Ct) was made at the 60°C point. A dissociation curve was run at the end of the

reaction to ensure a single amplification product. All Ct values were normalized

to the cyclophilin mRNA concentration of the sample to take total mRNA

concentration into account. The averages of Ct values from the vehicle treated

CON mice were set to 1 and all other groups were expressed as the fold change

compared to the vehicle treated CON group.

Statistical Analyses and Data Presentation: Data are expressed as the mean

± SEM. Significance of differences was determined for each group of values by

ANOVA (Tukey-Kramer honestly significant difference) or unpaired t-test.

A p value < 0.05 was considered significant. All analyses were performed using

JMP version 5.0.12 software (SAS Institute, Inc., Cary, NC).

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RESULTS

In order to test whether hepatic ABCG5/G8 function would be necessary for LXR

agonist mediated increases in fecal neutral sterol excretion, C57Bl/6 were

injected with an ABCG8 ASO to decrease hepatic ABCG8 mRNA levels (G8HKD).

Additionally, a control group of mice (CON) were injected with a non-targeting

ASO. Mice were concomitantly treated with ASOs and fed a low cholesterol

(0.01% w/w), low fat (10% of energy as palm oil) synthetic diet for 6 weeks. For

the last 7 days of treatment, mice were gavaged daily with either vehicle or an

LXR agonist (T0901317, 25mg/kg/day). To measure macrophage RCT, mice

were injected with [3H]-cholesterol labeled J-774 macrophages 2 days prior to

necropsy.

LXR agonist treatment attenuates ASO knockdown of hepatic ABCG8

It is known that ABCG8 is transcriptionally upregulated by LXR activation14. Since

ASOs also target mRNA, it was unclear whether ASO knockdown of ABCG8 would be overcome by LXR stimulation. Hepatic levels of ABCG8 and ABCG5 were measured by RT-PCR. All mice treated with ABCG8 ASO had reduced

ABCG8 mRNA levels, but LXR agonist treatment limited the effectiveness of the

ABCG8 ASO (Figure 1). Vehicle treated G8HKD mice had a 64% reduction in

hepatic ABCG8 mRNA when compared to CON mice (Figure 1A). As expected,

LXR agonist treatment of CON mice caused a significant increase in hepatic

ABCG8 mRNA levels (+317%). When administered to G8HKD mice, the LXR

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agonist caused hepatic ABCG8 mRNA to be increased by 160% compared to

vehicle treated G8HKD mice. Hepatic ABCG8 mRNA, however, was still 223%

less in G8HKD mice treated with LXR agonist than the CON mice treated with LXR agonist. As a control, hepatic ABCG5 mRNA expression was also measured.

There was no reduction in hepatic ABCG5 mRNA in the G8HKD mice, and LXR

agonist treatment increased hepatic ABCG5 mRNA to similar levels in both CON

and G8HKD mice (Figure 1B).

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Figure 1. ABCG8 and ABCG5 mRNA expression. Liver and duodenum were collected from CON and G8HKD mice at necropsy and RNA was isolated as described in the methods section. Gene expression for individual samples was measured by RT-PCR. Average units were calculated and normalized to β-actin. A) Hepatic ABCG8 RNA expression. B) Hepatic ABCG5 RNA expression. C) Duodenal ABCG8 RNA expression. D) Duodenal ABCG5 RNA expression. Data are expressed as mean±SEM (n=5-10 per group). Data analyzed by 2-way ANOVA followed by Student t tests for post hoc analysis. Bars that do not share a common letter are significantly different (p<0.05).

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ASOs preferentially target gene expression in the liver. High doses and long term

treatment can, however, cause mRNA knockdown in other tissues. Since

ABCG5/G8 is also expressed in the small intestine, small intestinal mRNA

expression of ABCG8 and ABCG5 was measured. Similar to our previous report

(Chapter III, Fig 1C), intestinal ABCG8 mRNA was decreased by 39% in G8HKD mice compared to CON mice (Figure 1C). LXR agonist treatment increased duodenal ABCG8 expression significantly in CON mice (+152%) and to a lesser extent in G8HKD mice (+136%) when compared to respective vehicle treatment

groups. Similar to hepatic ABCG5, There was no reduction in duodenal ABCG5 mRNA in the G8HKD mice, and LXR agonist treatment increased duodenal

ABCG5 mRNA to similar levels in both CON and G8HKD mice (Figure 1D).

Biliary cholesterol concentration is not reduced in LXR agonist treated

G8HKD mice

To further confirm the effectiveness of the ABCG8 ASO, hepatic biliary lipid

concentrations were measured (Figure 2). Since ABCG5/G8 function correlates

with biliary cholesterol concentrations15, biliary cholesterol concentrations was

predicted to be decreased in G8HKD mice treated with both vehicle and LXR

agonist. With vehicle treatment, G8HKD mice had a 57% reduction in biliary

cholesterol concentration when compared to CON mice (Figure 2A). Compared

to vehicle treatment, CON mice had a 56% increase in biliary cholesterol

concentration after LXR agonist administration. G8HKD mice treated with LXR

116 agonist also had increased biliary cholesterol concentrations (+78%) when compared to vehicle treatment of G8HKD mice. Unfortunately, this LXR agonist induced increase to biliary cholesterol concentration in G8HKD mice reached a level similar to LXR agonist treated CON mice. Biliary phospholipid and biliary bile acid concentrations were not changed between any of the groups (Figure 2B

& 2C).

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Figure 2. Biliary sterol concentrations. Sterols were extracted from the gall bladder bile of CON and G8HKD mice and measured for cholesterol by gas- liquid chromatography and for phospholipids and bile acids by enzymatic assays. Molar ratios of each lipid were calculated by dividing the concentration of each lipid by the total biliary lipid concentration. Data are expressed as mean±SEM (n=6-9 per group). Data analyzed by 2-way ANOVA followed by Student’s t test for post hoc analysis. Bars that do not share a common letter are significantly different (p<0.05).

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LXR agonist treatment increases plasma sterol mass and radioactivity in

CON and G8HKD mice

Plasma total sterol was not changed in G8HKD mice when compared to CON mice

on the low cholesterol diet (Figure 3A). LXR agonist treatment significantly

increased plasma total sterol in both CON and G8HKD mice compared to vehicle treatment. Not surprisingly, there were no significant differences in plasma levels between any of the groups (Figure 3B). After injection with [3H]- cholesterol labeled macrophages, plasma levels of [3H]-cholesterol were

increased in both CON and G8HKD mice treated with the LXR agonist (Figure 3C).

The plasma [3H]-cholesterol levels at necropsy (48h post macrophage injection)

closely mirrored the plasma total sterol mass.

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Figure 3. Plasma sterol mass and radioactivity. Sterols were extracted from the plasma of CON and G8HKD mice and measured by gas-liquid chromatography or counted for [3H]- cholesterol. 2A) Plasma total sterol concentrations. 2B) Plasma triglyceride concentrations. 2C) Time course of plasma [3H]- cholesterol recovery. Data are expressed as mean±SEM (n=4-5 per group). Data analyzed by 2-way ANOVA followed by Student’s t test for post hoc analysis. Bars that do not share a common letter are significantly different (p<0.05).

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LXR agonist treatment increases hepatic triglyceride in CON and G8HKD mice

As expected for low dietary cholesterol feeding, total hepatic sterol concentrations remained very low in all groups (<4μg/mg wet weight) (Figure

4A). In agreement with previous reports, hepatic sterol concentrations were slightly but significantly decreased with LXR agonist treatment in CON mice. LXR agonist treatment did not significantly alter hepatic sterol concentrations in G8HKD mice. It is well established that treatment with the LXR agonist T0901317 causes hepatic hypertriglyceridemia16. CON and G8HKD mice had significant hepatic

triglyceride accumulation with T0901317 treatment (Figure 4B). There were no

significant differences in hepatic [3H]-cholesterol recovery between any of the

groups (Figure 4C).

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Figure 4. Liver sterol mass and radioactivity. Sterols were extracted from the livers of CON and G8HKD mice and measured by gas-liquid chromatography or counted for [3H]-cholesterol. All hepatic lipid values were normalized to the wet weight of the extracted piece of liver. 2A) Total hepatic sterol concentrations. 2B) Hepatic triglyceride concentrations. 2C) Hepatic [3H]- cholesterol recovery. Data are expressed as mean±SEM (n=4-5 per group). Data analyzed by 2-way ANOVA followed by Student’s t test for post hoc analysis. Bars that do not share a common letter are significantly different (p<0.05).

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LXR agonist treatment does not increase fecal neutral sterol excretion in

G8HKD mice

Finally, fecal neutral sterol excretion was not significantly different between

vehicle treated CON and G8HKD mice (Figure 5A). LXR agonist treatment greatly increased fecal neutral sterol excretion in CON mice, but not G8HKD mice. This surprising result was replicated in fecal neutral [3H]sterol recovery (Figure 5B).

There was no significant difference in fecal neutral [3H]sterol count between

vehicle treated CON and G8HKD mice. LXR agonist treatment greatly increased fecal neutral [3H]sterol count in CON mice, but not G8HKD mice. This effect of

LXR agonist treatment seems to be specific to neutral sterol excretion, since

levels of acidic [3H]sterol excretion were increased to a similar extent in both LXR agonist treated CON and G8HKD mice (Figure 5C).

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Figure 5. Fecal neutral sterol mass and radioactivity. Neutral sterols were extracted from the feces of CON and G8HKD mice and measured by gas-liquid chromatography or counted for [3H]-sterol content. 5A) Fecal neutral sterol excretion normalized to the number of days feces were collected and mouse body weights. 5B) [3H]-cholesterol recovery in the feces. 5C) [3H]-bile acid recovery in the feces. Data are expressed as mean±SEM (n=10 per group). Data analyzed by 2-way ANOVA followed by Student’s t test for post hoc analysis. Bars that do not share a common letter are significantly different (p<0.05).

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RESULTS

The major finding of this study is that cholesterol excretion and macrophage RCT

are not stimulated by LXR agonist treatment when hepatic ABCG8 expression is blunted. Hepatic ABCG8 mRNA levels were less than half in LXR stimulated

G8HKD mice than in LXR stimulated CON mice. This attenuation of hepatic

ABCG8 mRNA levels, led to differences in fecal neutral sterol loss and

macrophage RCT when comparing LXR stimulated CON and G8HKD mice.

Similar to previous reports3, LXR agonist treatment greatly increased fecal

neutral sterol excretion in CON mice. In G8HKD mice, however, LXR agonist

treatment failed to significantly increase fecal neutral sterol excretion.

Macrophage RCT, as measured by fecal [3H]cholesterol recovery, closely

mirrored mass fecal neutral sterol excretion. Macrophage RCT was greatly

enhanced in LXR stimulated CON mice but not in LXR stimulated G8HKD mice.

These results suggest that full upregulation of hepatic ABCG8 mRNA is required

for LXR agonist mediated increases in cholesterol excretion and macrophage

RCT.

Since it has been well established that biliary cholesterol concentrations correlate

with ABCG5/G8 expression15, it is surprising that biliary cholesterol

concentrations were similar in LXR stimulated CON and G8HKD mice, despite the differences in hepatic ABCG8 mRNA levels. Biliary cholesterol concentrations were highly variable in the LXR agonist treated CON mice, which could help to explain why there was no apparent difference between the LXR agonist treated

125

groups. Additionally, this possible disconnect between hepatic ABCG8 mRNA

levels and biliary cholesterol concentrations could support the idea that

ABCG5/G8 has another function besides biliary cholesterol secretion that is

crucial to the RCT pathway.

In fact, LXR agonist treatment can still cause fecal neutral sterol excretion to be

increased in several mouse models where biliary contributions to fecal sterol loss

are absent17, 18. These mouse models, however, do not manipulate biliary

cholesterol by altering ABCG5/G8 expression. Calpe-Berdiel L, et al19 reported

that ABCG5/G8 KO mice have impaired LXR agonist stimulated macrophage

RCT. The discrepancy between ABCG5/G8 KO mice and the other models that

also have impaired biliary cholesterol concentrations, suggest that there is a

function of ABCG5/G8 other than biliary cholesterol secretion that is required for

LXR agonist mediated increases to RCT.

Our results agree with the findings by Zhang, Y et al6 that hepatic LXRα expression is required for RCT in mice. Since ABCG5/G8 is transcriptionally regulated by LXR, hepatic ABCG5/G8 mRNA was not increased with LXR agonist treatment in hepatic LXRα KO mice. Similarly, hepatic ABCG8 expression was blunted in LXR agonist treated G8HKD mice that did not have

increased RCT. Our data suggest that it is ABCG5/G8, a downstream target of

LXR, that is required for LXR stimulated increases in cholesterol excretion and

macrophage RCT.

126

Recent studies indicate, however, that the small intestine plays a significant role

in LXR agonist driven cholesterol excretion. For example, macrophage RCT was

stimulated in mice receiving an intestine-specific LXR agonist compound20. In these mice, intestinal but not hepatic ABCG5/G8 (and other target genes) was upregulated. Constitutive activation of small intestinal LXRα has also been shown to increase RCT21. These contradictive findings are puzzling and highlight

the need for more studies to examine the tissue specific role of ABCG5/G8 in

RCT.

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CHAPTER V

DISCUSSION

It has been well established that ABCG5/G8 is a critical regulator of sterol

homeostasis because of its ability to secrete/excrete phytosterols and cholesterol

from the body. The studies presented in this dissertation, however, show that the

role of ABCG5/G8 in sterol metabolism and homeostasis is more complex and

has not been completely discovered.

In regards to phytosterol metabolism, ABCG5/G8 functions to restrict plant sterol

absorption. It appears that ABCG5/G8 excludes plant sterols from the body

because they are toxic when present at high levels. In Chapter II, WT and

ABCG5/G8 KO mice were fed a diet enriched with plant sterols. The high-

phytosterol diet was extremely toxic to the ABCG5/G8 KO mice but had no adverse effects on WT mice. ABCG5/G8 KO mice died prematurely and developed a phenotype that included high levels of plant sterols in many tissues,

liver abnormalities, and severe cardiac lesions.

The findings of this study are useful in relation to dietary phytosterol

supplementation, which is currently used to reduce the risk of coronary heart

disease (CHD)1, 2. Plant sterols are thought to reduce plasma cholesterol concentrations by inhibiting cholesterol absorption3, 4. Most individuals are able to

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exclude plant sterols from the body via ABCG5/G8, and the FDA allows

phytosterol-enriched foods to be classified as “generally recognized as safe.” In

several species of animals, presumably with ABCG5/G8 intact, that have been

administered high doses of plant sterols, there have been no reports of toxicity5.

Some debate still exists, however, about the safety of dietary phytosterol supplementation, specifically concerning their potential cytotoxic effects on endothelial cells in arteries.

Our study shows that an extremely high concentration of phytosterols in plasma and tissues is toxic. This phenotype seems to depend specifically on the amount of phytosterols that accrue. The presence of intact ABCG5/G8 in an individual appears to offer full protection against dietary phytosterol accumulation, and there is no indication that long term exposure could cause levels of phytosterols to build up to toxic levels. Consequently, dietary supplementation with phytosterols appears safe for the general population.

Our findings also lend novel insight into the body’s need for discrimination between plant sterols and cholesterol. We have shown for the first time that high levels of tissue plant sterol accumulation cause premature death, extensive cardiac lesions, liver damage, and hepatosplenomegaly. These toxicities appear related to accumulation of high levels of unesterified phytosterols that cannot be efficiently metabolized into bile acids nor esterified for storage in lipid droplets.

Accumulation as the free sterol probably results in accumulation in membranes

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with subsequent disruption of membrane integrity. Further studies need to be

done, however, in order to determine the molecular mechanisms that underlie phytosterol toxicity. Our data show that ABCG5/G8’s role in phytosterol exclusion

from the body is one of protection from the toxic effects of plant sterols.

A previous study from Miettinen, TA et al6 showed that hepatic ABCG5/G8

function was sufficient to limit phytosterol accumulation, suggesting that hepatic

ABCG5/G8 is the primary determinant of steady state plasma phytosterol

concentration. In Chapter III, we report that hepatic ABCG5/G8 function is not

required to prevent phytosterol accumulation in mice. CON, G8HKD, WT, and

ABCG5/G8 KO mice were fed varying amounts of dietary sterol, and plasma and

tissue sterol concentrations were compared between the groups. Compared to

their WT counterparts, mice with whole body ABCG5/G8 deficiency accumulated

very high plasma and hepatic phytosterol concentrations in a dietary sterol

dependent manner. The G8HKD mice did not achieve these high levels of plasma and hepatic phytosterol. These results show that small intestinal ABCG5/G8

function is sufficient to prevent high levels of plant sterol accumulation in mice.

This would support the idea that small intestinal ABCG5/G8 is part of the body’s

first line of defense in preventing dietary plant sterol absorption and

accumulation. When small intestinal ABCG5/G8 is functional, it appears that

hepatic ABCG5/G8 serves as a backup to secrete into bile any dietary plant

sterols that do get absorbed.

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The G8HKD mouse model also provided an opportunity to study the role of hepatic

ABCG5/G8 function in cholesterol metabolism in a system without dramatic

phytosterol accumulation. This is important because the effects of phytosterol accumulation in models of ABCG5/G8 deficiency are substantial. ABCG5/G8 KO mice on low cholesterol diets have significant reductions in plasma and hepatic cholesterol concentrations 7-9. Despite these reductions, there are no

compensatory increases in cholesterol synthesis genes. It is unclear how much

of the changes in sterol metabolism were due to the mass accumulation of plant sterols versus the lack of ABCG5/G8 function.

Based on data in Chapter III, it appears that hepatic ABCG5/G8 plays an important role in cholesterol metabolism, independent of its ability to transport

phytosterols. G8HKD mice had significant reductions in biliary cholesterol

concentrations irregardless of the amount of dietary sterol fed. Despite the reduction in biliary cholesterol, G8HKD mice were able to maintain levels of

hepatic cholesterol and fecal neutral sterol excretion similar to those of CON

mice on the low sterol and high phytosterol diets. On the high cholesterol diet,

however, G8HKD mice could not maintain appropriate cholesterol homeostasis.

The G8HKD mice accumulated very high levels of hepatic cholesterol and had a

significant decrease in fecal neutral sterol excretion when compared to CON mice. These data suggest that G8HKD mice have a disfunction in the TICE

pathway and subsequently cannot compensate for the reduction in biliary

cholesterol secretion in the face of a dietary cholesterol challenge.

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Since ABCG5/G8 is required for biliary sterol secretion7, 10, its crucial role in

biliary RCT is firmly established. Until recently, biliary secretion was the

universally accepted pathway by which peripheral cholesterol was excreted from

the body in the feces. If biliary cholesterol excretion was the only contributor to

fecal sterol loss, one would expect dramatically decreased fecal sterol output to

accompany decreases in biliary cholesterol levels. This is not the case, however,

in several mouse models that exhibit little to no biliary cholesterol secretion 11-13.

Along with several studies conducted in rats, dogs, and humans 11, 14-16, these

observations have led our group and others to the discovery of a novel pathway

for non-biliary cholesterol excretion which is called transintestinal cholesterol

excretion (TICE).

The hallmark features of models that primarily use the TICE pathway to excrete

cholesterol are severly diminished biliary cholesterol secretion, with no

accumulation of hepatic cholesterol due to normal levels of fecal neutral sterol

excretion. Since our G8HKD mice had dramatically decreased levels of biliary

cholesterol, we predicted that the TICE pathway would compensate for the loss

of biliary sterol secretion, resulting in normal FNS excretion and no accumulation

of hepatic cholesterol in the G8HKD mice. This appears to be the case when comparing G8HKD mice on the LS and HP diets to the CON mice. Despite the more than 80% reduction in biliary cholesterol levels, G8HKD mice had levels of

FNS excretion and hepatic cholesterol similar to CON mice on the LS and HP

diets.

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Surprisingly, we found an opposite result in G8HKD mice fed the HC diet. G8HKD

mice on the HC diet had more than a 70% reduction in biliary cholesterol

concentration. The high level of dietary cholesterol fed to these mice unmasked a significant reduction in fecal neutral sterol excretion and a dramatic increase in hepatic cholesterol accumulation when compared to CON mice. These data suggest that the G8HKD mice have a disfunction in the TICE pathway and

subsequently cannot compensate for the reduction in biliary sterol secretion with

the dietary cholesterol challenge.

Chapter IV focused on the role of hepatic ABCG5/G8 in LXR agonist stimulated

cholesterol excretion and macrophage RCT. Key regulators of ABCG5/G8

expression are the nuclear receptors liver x receptor (LXR) α and LXRβ. LXR

activation using synthetic agonists leads to increased fecal neutral sterol loss in

mice17. Presumably this increase is caused by an ABCG5/G8 mediated increase in biliary cholesterol concentration since ABCG5/G8 KO mice did not have increased fecal neutral sterol excretion when treated with an LXR agonist18. It has also been shown that LXR agonist stimulated macrophage RCT is impaired in ABCG5/G8 KO mice19.

Furthermore, there is evidence that ABCG5/G8’s role in RCT may be tissue- specific. In liver-specific LXRα knockout mice, cholesterol excretion and macrophage RCT were not stimulated upon LXR agonist treament20. Because

ABCG5/G8 is transcriptionally regulated by LXR, hepatic ABCG5/G8 mRNA was

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not induced with LXR agonist treatment in those mice. These studies suggest

that LXR stimulated cholesterol and macrophage RCT may be mediated by

hepatic ABCG5/G8, downstream targets of LXR activation.

In Chapter IV, it was reported that cholesterol excretion and macrophage RCT

were not stimulated by LXR agonist treatment when hepatic ABCG8 expression

was blunted. These results agree with the findings by Zhang, Y et al20 that

hepatic LXRα expression is required for RCT in mice. Since ABCG5/G8 is transcriptionally regulated by LXR, hepatic ABCG5/G8 mRNA was not increased with LXR agonist treatment in hepatic LXRα KO mice. Similarly, hepatic ABCG8 expression was blunted in LXR agonist treated G8HKD mice, and they did not

have increased RCT. Our data suggest that it is ABCG5/G8, a downstream

target of LXR, that is required for LXR stimulated increases in cholesterol

excretion and macrophage RCT.

It has been reported that the LXR agonist T0901317 can strongly stimulate the

TICE pathway21. Initially shown in Chapter III, it appears that G8HKD mice have a

disfunction in the TICE pathway. In support of this observation, LXR agonist

treatment could not stimulate cholesterol excretion or macrophage RCT in G8HKD mice. In corroboration with our findings in Chapter III, these results suggest that hepatic ABCG5/G8 expression is required for TICE.

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While the data is promising, it is important to emphasize the preliminary nature of

these results that were generated using an ASO to knockdown hepatic ABCG8

mRNA. Due to the nature of ASO technology, hepatic ABCG8 knockdown was

incomplete. Additionally, there were some small effects of the ABCG8 ASO on

small intestinal ABCG8 mRNA levels. It would be best to conduct a similar set of

experiments in tissue-specific ABCG5/G8 KO mice.

The most exciting discovery from this body of work is the evidence that a novel role for ABCG5/G8 in cholesterol metabolism and homeostasis exists. At first

glance, it seems that the biology of ABCG5 and ABCG8 is fully understood – once sterols enter a hepatocyte or enterocyte, ABCG5/G8 can secrete them out into bile or the lumen of the small intestine. These studies show, however, that

the role of ABCG5/G8 in maintaining sterol balance is much more complex.

Important questions that remain are: how does sterol reach ABCG5/G8 for

secretion? And what, if any, additional function could ABCG5/G8 have other than

biliary sterol secretion? It is essential to answer these questions to more fully

understand cholesterol metabolism in the liver and small intestine.

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Allison L. McDaniel, BS, BA

Curriculum Vitae

Wake Forest University School of Medicine

NAME: Allison Leigh McDaniel, BS, BA

POSITION TITLE: Doctoral Candidate Department of Pathology Section on Lipid Sciences Wake Forest University School of Medicine GPA: 3.55

ADDRESS: Medical Center Boulevard Winston-Salem, NC 27157 Phone: (423)754-6822 Email: [email protected] [email protected]

EDUCATION: Bachelor of Science, Biology Bachelor of Art, Political Science Cum Laude Emory & Henry College, Emory, VA May 2006 GPA: 3.34

CAREER DEVELOPMENT

In Progress Doctor of Philosophy, Molecular Pathology Wake Forest University School of Medicine

EMPLOYMENT

2007 – Present Graduate Student Research Fellow Department of Pathology, Section on Lipid Sciences, Wake Forest University School of Medicine, Graduate School of Arts and Sciences, Winston-Salem, NC Advisor: Ryan Temel, PhD Co-Advisors: Larry Rudel, PhD & J Mark Brown, PhD

2006 – 2007 Quality Assurance Laboratory Chemist GlaxoSmithKline Pharmaceuticals, Bristol, TN

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HONORS

2011 Early Career Investigator Travel Award Kern Lipid Conference, Vail, CO

2008 – 2011 Graduate Fellow, T32 Integrative Lipid Sciences, Inflammation, and Chronic Diseases Training Program, Wake Forest University School of Medicine, Winston-Salem, NC

2005, 2002 Dean’s List Emory & Henry College, Emory, VA

2004 – 2006 Member, Beta Beta Beta National Biology Honor Society Emory & Henry College, Emory, VA

2003 – 2006 Member, Pi Sigma Alpha National Political Science Honor Society Emory & Henry College, Emory, VA

2003 – 2006 Member, Pi Gamma Mu National Humanities Honor Society Emory & Henry College, Emory, VA

BIBLIOGRAPHY

Published manuscripts:

1. McDaniel AL, Alger HM, Sawyer JK, Kelley KL, Kock ND, Brown JM, Temel RE, and Rudel LL. Phytosterol feeding causes toxicity in ABCG5/G8 knockout mice. [Paper accepted by American Journal of Pathology]

2. Beason DP, Hsu JE, Marshall SM, McDaniel AL, Temel RE, Abboud JA, Soslowsky LJ. Hypercholesterolemia increases supraspinatus tendon stiffness and elastic modulus across multiple species. J Shoulder Elbow Surg. 2012 Sep 13. [Epub ahead of print] PMID: 22981355

3. Owens AP 3rd, Passam FH, Antoniak S, Marshall SM, McDaniel AL, Rudel L, Williams JC, Hubbard BK, Dutton JA, Wang J, Tobias PS, Curtiss LK, Daugherty A, Kirchhofer D, Luyendyk JP, Moriarty PM, Nagarajan S, Furie BC, Furie B, Johns DG, Temel RE, Mackman N. Monocyte tissue factor-dependent activation of coagulation in hypercholesterolemic mice and monkeys is inhibited by simvastatin. J Clin Invest. 2012 Feb 1;122(2):558-68. Epub 2012 Jan 3. PMID: 22214850

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4. Rayner KJ, Esau CC, Hussain FN, McDaniel AL, Marshall SM, van Gils JM, Ray TD, Sheedy FJ, Goedeke L, Liu X, Khatsenko OG, Kaimal V, Lees CJ, Fernandez-Hernando C, Fisher EA, Temel RE, Moore KJ. Inhibition of miR-33a/b in non-human primates raises plasma HDL and lowers VLDL . Nature, 2011 Oct 19;478(7369):404-7. PMID: 22012398

5. Medina MW, Gao F, Naidoo D, Rudel LL, Temel RE, McDaniel AL, Marshall SM, Krauss RM. Coordinately regulated alternative splicing of genes involved in cholesterol biosynthesis and uptake. PLoS One, 2011 Apr 29;6(4):e19420. PMID: 21559365

6. Temel RE, Sawyer JK, Yu L, Lord C, Degirolamo C, McDaniel A, Marshall S, Wang N, Shah R, Rudel LL, Brown JM. Biliary sterol secretion is not required for macrophage reverse cholesterol transport. Cell Metabolism, 2010 Jul 4;12(1):96-102. PMID: 20620999

Manuscripts in preparation:

1. McDaniel AL, Brown JM, Temel RE. Hepatic ABCG8 knockdown does not cause phytosterol accumulation in mice. Planned submission to Arteriosclerosis, Thrombosis and Vascular Biology.

2. McDaniel AL, Brown JM, Temel RE. Transintestinal cholesterol excretion and macrophage reverse cholesterol transport are not stimulated in hepatic ABCG8 knockdown mice treated with an LXR agonist. Journal TBA.

Abstracts/Presentations at National Meetings:

1. McDaniel AL, Brown JM, Temel RE. Transintestinal cholesterol excretion and macrophage reverse cholesterol transport are not stimulated in hepatic ABCG8 knockdown mice treated with an LXR agonist. Gordon Research Conference, Lipid and Lipoprotein Metabolism in Health and Disease, June 2012 [poster presentation].

2. Owens AP, Passam FH, Antoniak S, Marshall SM, McDaniel AL, Rudel L, Williams JC, Hubbard BK, Dutton JA, Wang J, Tobias PS, Curtiss LK, Daugherty A, Kirchhofer D, Luyendyk JP, Moriarty PM, Nagarajan S, Furie BC, Furie B, Johns DG, Temel RE, Mackman N. Monocyte Tissue Factor- Dependent Activation of Coagulation in Hypercholesterolemic Mice and Monkeys Is Inhibited by Simvastatin. Abstract # 42: Arteriosclerosis, Thrombosis, and Vascular Biology Scientific Sessions, 2012.

3. McDaniel AL, Sawyer JK, Lee RG, Graham MJ, Crooke RM, Rudel LL, Brown JM, Temel RE. Liver specific knockdown of ABCG8 causes

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dysfunction of trans intestinal cholesterol efflux. Kern Lipid Conference, 2011[poster presentation].

4. McDaniel AL, Marshall SM, Kelley KL, Lee RG, Graham MJ, Crooke RM, Rudel LL, Temel, RE. Effects of hepatic NPC1L1 suppression on cholesterol metabolism in vervet monkeys. Abstract # P198: Arteriosclerosis, Thrombosis, and Vascular Biology Scientific Sessions, 2011.

5. Cuffe HA, Chung S, Marshall SM, McDaniel AL, Temel RE, Parks JS. Dietary cholesterol is associated with increased adipocyte size and cholesterol content in visceral, but not subcutaneous, fat in African green monkeys. Abstract # P327: Arteriosclerosis, Thrombosis, and Vascular Biology Scientific Sessions, 2011.

6. Owens AP, Marshall SM, McDaniel AL, Williams JC, Johns DG, Temel RE, Mackmam N. Simvastatin intervention attenuates dyslipidemic increases in microparticle tissue factor, inflammation, and the activation of coagulation in nonhuman primates without affecting LDL-C. Abstract # 28: Arteriosclerosis, Thrombosis, and Vascular Biology Scientific Sessions, 2011.

7. McDaniel AL, Marshall S, Kelley KL, Sawyer JK, Kavanagh K, Sprecher DL, Rudel LL, Olsen EJ, Temel RE. PPARδ agonist GW501516 raises plasma HDL-cholesterol and LCAT activity in African green monkeys. Gordon Research Conference, Lipid and Lipoprotein Metabolism in Health and Disease, June 2010 [poster presentation]. 8. McDaniel AL, Marshall SM , Kelley KL, Lee RG, Graham MJ, Crooke RM, Yu L, Rudel LL, Temel RE. Effects of NPC1L1 ASO on cholesterol metabolism in vervet monkeys. Gordon Research Conference, Lipid and Lipoprotein Metabolism in Health and Disease, June 2010.

9. Owens AP, Temel RE, Barcel DA, Marshall SM, McDaniel AL, Mackmam N. Hyperlipidemia Increases Microparticle Tissue Factor and the Activation of Coagulation: A Tale of Mice and Monkeys. Abstract # 20151: Scientific Sessions of the American Heart Association, 2010.

10. McDaniel AL, Lan T, Marshall SM, Boyd CA, Kelley KL, Wilson MD, Sawyer JK, Rudel LL, Temel RE. Dietary n-3 fatty acids have minimal effects on intestinal Niemann-Pick C1 like 1 expression and cholesterol absorption [abstract]. Arterioscler Thromb Vasc Biol. 2009; 29(7):e30 [poster presentation].

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PRESENTATIONS

2012 The tissue specific role of ABCG5/G8 in sterol transport. Lipid Sciences Program Project Group Meeting, Wake Forest School of Medicine, Winston- Salem, NC.

2012 Tissue specific contributions of ABCG5/G8 to sterol transport. 2nd Annual Mini-Symposium on Integrative Lipid Sciences, Inflammation, and Chronic Diseases, Wake Forest School of Medicine, Winston-Salem, NC.

2011 Liver specific knockdown of ABCG8 causes dysfunction of trans intestinal cholesterol efflux [abstract]. Poster presentation, Kern Lipid Conference.02-2009 The Role of Liver Derived Apo-B Containing Lipoproteins in a Non-Biliary Model of Cholesterol Excretion. Wake Forest School of Medicine, Winston- Salem, NC.

2011 The role of hepatic ABCG5/G8 and NPC1L1 in the Trans-Intestinal Cholesterol Efflux pathway. Mini-Symposium on Integrative Lipid Sciences, Inflammation, and Chronic Diseases, Wake Forest School of Medicine, Winston- Salem, NC.

2011 Hepatic ABCG8: A key player in the TICE pathway? Lipid Sciences Program Project Group Meeting, Wake Forest School of Medicine, Winston- Salem, NC.

2010 The Role of Hepatic ABCG5/G8 in Whole Body Sterol Homeostasis. Molecular Pathology Graduate Program Seminar, Wake Forest School of Medicine, Winston-Salem, NC

2010 PPARδ agonist GW501516 raises plasma HDL-cholesterol and LCAT activity in African green monkeys [abstract]. Poster Presentation, Gordon Research Conference, Lipid and Lipoprotein Metabolism in Health and Disease.

TEACHING EXPERIENCE

Lectures:

2012 Anatomy & Physiology, Doctorate of Physical Therapy Course, Winston Salem State University, Winston-Salem, NC

2012 Anatomy & Physiology, Undergraduate Course, Winston-Salem State University, Winston-Salem, NC

Other:

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2008 Assistant Instructor, CampMed for Middle School Students, Department of Biology, State University of New York – Jefferson Community College

2005 – 2006 Supplemental Instructor, Undergraduate General Biology, Emory & Henry College, Emory, VA

PROFESSIONAL MEMBERSHIPS

2008 – Present Member, American Heart Association 2008 – Present Member, Council on Atherosclerosis, Thrombosis and Vascular Biology

COMMUNITY ACTIVITIES

2012 – Present U.S. Army Family Readiness Group (FRG) Leader, Alpha Troop, 1-17 CAV, 82nd CAB, Fort Bragg, NC

Role: Supervises the committees, groups and functions for a FRG consisting of Soldiers, civilians and volunteers assigned to the unit and their families (immediate and extended) for morale, cohesion, communication, unit cooperation and the well being of company personnel and their families. Duties: Supports the commander’s family readiness goals; provides overall leadership of the FRG; schedules, plans, and conducts company Family Readiness Group meetings; delegates FRG responsibilities to select volunteers in order to promote participation in FRG activities and accomplishment of FRG objectives; acts as a liaison between battalion and company level FRGs; identifies needs or unique problems of unit families; tracks FRG appropriated fund budget; serves as a member of the battalion-level steering committee.

2012 – Present Chairperson, Young Alumni Council, Emory & Henry College, Emory, VA

Role: Supervises members of the Young Alumni Council in their efforts to help recent graduates transition into proactive members of the alumni network, encourage young alumni involvement and annual giving, give a voice to young alumni concerns and ideas, plan and promote social, community and networking events designed for young alumni Duties: Provides overall leadership of the Young Alumni Council; schedules, plans, and conducts Young Alumni Council meetings and alumni events; acts as a liason between alumni and Emory & Henry College.

2011 – Present Member, Young Alumni Council, Emory & Henry College, Emory, VA

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