Adsorptive Surface Modification of Cellulose Nanocrystals to Stabilize Nutraceuticals Loaded Lipid Carriers for Food Application
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The University of Maine DigitalCommons@UMaine Electronic Theses and Dissertations Fogler Library Fall 12-18-2020 Adsorptive Surface Modification of Cellulose Nanocrystals to Stabilize Nutraceuticals Loaded Lipid Carriers for Food Application Avinash S. Patel University of Maine, [email protected] Follow this and additional works at: https://digitalcommons.library.umaine.edu/etd Part of the Food Chemistry Commons, Food Processing Commons, Other Food Science Commons, and the Other Nutrition Commons Recommended Citation Patel, Avinash S., "Adsorptive Surface Modification of Cellulose Nanocrystals to Stabilize Nutraceuticals Loaded Lipid Carriers for Food Application" (2020). Electronic Theses and Dissertations. 3303. https://digitalcommons.library.umaine.edu/etd/3303 This Open-Access Thesis is brought to you for free and open access by DigitalCommons@UMaine. It has been accepted for inclusion in Electronic Theses and Dissertations by an authorized administrator of DigitalCommons@UMaine. For more information, please contact [email protected]. ADSORPTIVE SURFACE MODIFICATION OF CELLULOSE NANOCRYSTALS TO STABILIZE NUTRACEUTICALS LOADED LIPID CARRIERS FOR FOOD APPLICATION By Avinash Singh Patel M.S. Banaras Hindu University, India, 2014 B.S. Mahatma Gandhi Kashi Vidyapith, India, 2012 A DISSERTATION Submitted in Partial Fulfillment of the Requirements for the Degree of Doctor of Philosophy (in Food and Nutrition Sciences) The Graduate School The University of Maine December 2020 Advisory Committee: Mary E. Camire, Professor of Food Science & Human Nutrition, Co-Advisor Robert C. Causey, Professor of Animal and Veterinary Sciences, Co-Advisor Carl P. Tripp, Professor of Chemistry Mehdi Tajvidi, Associate Professor of Renewable Nanomaterials Denise I. Skonberg, Professor of Food Science and Human Nutrition © 2020 Avinash Singh Patel All Rights Reserved ii ADSORPTIVE SURFACE MODIFICATION OF CELLULOSE NANOCRYSTALS TO STABILIZE NUTRACEUTICALS LOADED LIPID CARRIERS FOR FOOD APPLICATION By Avinash Singh Patel Dissertation Co-Advisors: Dr. Mary Ellen Camire and Dr. Robert Causey An Abstract of the Dissertation Presented in Partial Fulfillment of the Requirements for the Degree of Doctor Philosophy (in Food and Nutrition Sciences) December 2020 Lipid carriers such as emulsions and liposomes have been widely studied as carriers for different nutraceuticals. However, lipid carriers' physicochemical instability results in the leakage of loaded nutraceuticals and the low solubility into the digestion medium, thus reducing the bioaccessibility. Cellulose nanocrystals (CNC) are nano-sized cellulose derivatives obtained after hydrolysis of cellulosic matrices that possess potential applications in functional foods and nutraceuticals. However, hydrophilicity, anionic surface potential, and poor re-dispersibility limit CNC’s applications. The primary objectives of this research were 1) to modify CNC via adsorbing polyethylene glycol (PEG) to stabilize liposomes and to study its physiochemical stability at different in vitro gastrointestinal tract (GIT) conditions, pH levels (1-11), temperatures (4-100 ºC) and illumination periods (4-72 hours); 2) to modify CNC via adsorbing lauric acid to stabilize O/W emulsion and to study its physicochemical stability at different pH (1-11), dilution factors (1-10 times), storage period (up to 30 days) and GIT conditions. Phycobiliprotein and beta-carotene were chosen as model nutraceuticals. iii In study 1, particle size and microscopic analysis revealed a better physical/kinetic stability for the liposomes stabilized with PEG-adsorbed CNC than the liposomes stabilized with unmodified CNC, resulting in significantly (p≤0.05) smaller average particle size during the initial and mouth phases of the in vitro GIT study, nonetheless a significant (p≤0.05) increase in the particle size from ~300 nm to ~5500 nm at gastric phase due to lower pH. Moreover, stabilized liposomes retained the attributes of phycobiliprotein against pH, illumination, and a temperature of 60 ̊C. In study 2, lauric acid-adsorbed CNC affirmed the kinetic/physical stability of emulsions throughout the GIT phases. Results exhibited a maximum of 65% beta-carotene bioaccessibility for the emulsion stabilized with modified CNC, and 71% for the emulsion stabilized with unmodified CNC. Moreover, a higher amount of lipid oxidation was recorded for the emulsion with stabilized modified CNC than the emulsion stabilized with gum Arabic. Although modified CNC retains the kinetic/physical stability of lipid carriers; however, it increases lipid carriers' chemical instability and decreases the loaded nutraceuticals' bioaccessibility. A strategic modification of CNC is needed to ensure the stability of lipid carriers and increased nutraceuticals bioaccessibility. iv DEDICATION I dedicate this dissertation to my beloved mother, who taught me to believe in myself, my father, who taught me to believe in hard work and dedication, and my teachers and friends for providing me knowledge, devotion, and encouragement. iii ACKNOWLEDGMENTS Fervently and modestly, I extol the genuine cooperation, inspiration and affection offered to me by the Co-Chairman of the advisory committee, Dr. Mary Ellen Camire, Professor of Food Science & Human Nutrition, in completing the research work in time, successfully. The present work bears the impression of her concrete suggestions, guidance, and meticulous attention to detail. I humbly place on record my respect and gratitude to Dr. Balunkeswar Nayak (former advisor), previously Associate Professor, School of Food and Agriculture, for his valuable guidance and cooperation towards completing my research and study. I am grateful to members of my advisory committee, Dr. Robert Causey, Dr. Carl P. Tripp, Dr. Mehdi Tajvidi, and Dr. Denise Skonberg, for constant motivation, rendered at all stages of this endeavor and my study period. I record my profound thanks to the India Council of Agricultural Research (ICAR), New Delhi, India, for awarding me with a prestigious Netaji Subhas International Fellow award (award number: 18(02)/2016-EQR/Edn.) and financial support to perform my doctoral degree at the University of Maine. I want to thank the USDA National Institute of Food and Agriculture Hatch project ME-021914, for financial support of my research work through the Maine Agricultural and Forest Experiment Station (MAFES). I owe a deep debt of thankfulness and heartfelt regards to Dr. Abhijit Kar, ICAR- IARI, New Delhi for his endless inspirational help and Mr. Kuldeep Katiyar, Nicholas Shoes, Pvt. Ltd., Greater Noida, India for his generous financial supports providing a iv security bond of $10,000 FD (fix deposit) in favor of the ICAR, India until successful completion of the degree program. My sincere thanks to the Intensive English Institute and Office of International Programme for their kind support in my first year of classes and creating an overwhelming and friendly environment around the campus making this place feel like home. I also record my sincere thanks to Dr. L. Brian Perkins, Katherine Davis-Dentici, David Labrecque, and Kelly Edwards for their guidance and assistance on instrumentation and analysis. I would like to thank SuriyaPrakash Lakshmibalasubrmaniam and my other past and current labmates and friends (Praveen Sappati, Richa Arya, Adoum Fadaya Arabi, Samuel Akomea Frempong, Zach Dijkhoff, Holly Leung, Rosanna Woodruff, Islam Hafez and all my SFA family members, UMaine, for helping me in one or the other manner during my research work. Mere words of acknowledgment will never express my deepest sense of gratitude and indebtedness to my father Shri. Umashankar Patel, my brothers (Anurag and Ashwani) and sisters (Mrs. Shalendri Patel and Mrs. Arati Patel), my family members, whose much-cherished love, inspiration ever encouraging moral support; selfless sacrifices enabled me to pursue my studies with unfailing zeal and devotion. To them, I owe more than I say. The words are not eloquent enough to express my special feeling for my mother Smt. Basmati Devi, whose moral support, deep affection, encouragement, ever willing help and understanding always envisioned me throughout this research work. Last but not least, none is forgotten, but all of them may not be mentioned. v TABLE OF CONTENTS DEDICATION ...............................................................................................................v ACKNOWLEDGMENTS ........................................................................................... vi CHAPTERS 1. INTRODUCTION .................................................................................................1 1.1. Background ...................................................................................................1 1.2. Objectives .....................................................................................................5 2. LITERATURE REVIEW ......................................................................................7 2.1. Nutraceuticals .................................................................................................8 2.1.1. Phycobiliproteins (PBP) ....................................................................10 2.1.2. Characteristics of PBP .......................................................................11 2.1.3. Stability of PBP .................................................................................12 2.1.4. Carotenoids .......................................................................................14