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THE FATE and SPECIATION of ARSENIC in SOILS and POULTRY PRODUCTION SYSTEMS by Jennifer M. Seiter a Dissertation Submitted To

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THE FATE and SPECIATION of ARSENIC in SOILS and POULTRY PRODUCTION SYSTEMS by Jennifer M. Seiter a Dissertation Submitted To THE FATE AND SPECIATION OF ARSENIC IN SOILS AND POULTRY PRODUCTION SYSTEMS by Jennifer M. Seiter A dissertation submitted to the Faculty of the University of Delaware in partial fulfillment of the requirements for the degree of Doctor of Philosophy in Plant and Soil Sciences Spring 2009 Copyright 2009 Jennifer Seiter All Rights Reserved UMI Number: 3360255 INFORMATION TO USERS The quality of this reproduction is dependent upon the quality of the copy submitted. Broken or indistinct print, colored or poor quality illustrations and photographs, print bleed-through, substandard margins, and improper alignment can adversely affect reproduction. In the unlikely event that the author did not send a complete manuscript and there are missing pages, these will be noted. Also, if unauthorized copyright material had to be removed, a note will indicate the deletion. ______________________________________________________________ UMI Microform 3360255 Copyright 2009 by ProQuest LLC All rights reserved. This microform edition is protected against unauthorized copying under Title 17, United States Code. _______________________________________________________________ ProQuest LLC 789 East Eisenhower Parkway P.O. Box 1346 Ann Arbor, MI 48106-1346 THE FATE AND SPECIATION OF ARSENIC IN SOILS AND POULTRY PRODUCTION SYSTEMS by Jennifer M. Seiter Approved: ___________________________________________________________ Blake C. Meyers, Ph.D. Chairperson of the Department of Plant and Soil Sciences Approved: ___________________________________________________________ Robin W. Morgan, Ph.D. Dean of the College of Agriculture and Natural Resources Approved: ___________________________________________________________ Debra H. Norris, M.S. Vice Provost for Graduate and Professional Education ii I certify that I have read this dissertation and that in my opinion it meets the academic and professional standard required by the University as a dissertation for the degree of Doctor of Philosophy. Signed: _______________________________________________________ Donald L. Sparks, Ph.D. Professor in charge of dissertation I certify that I have read this dissertation and that in my opinion it meets the academic and professional standard required by the University as a dissertation for the degree of Doctor of Philosophy. Signed: _______________________________________________________ William W. Saylor, Ph.D. Member of dissertation committee I certify that I have read this dissertation and that in my opinion it meets the academic and professional standard required by the University as a dissertation for the degree of Doctor of Philosophy. Signed: _______________________________________________________ J. Thomas Sims, Ph.D. Member of dissertation committee I certify that I have read this dissertation and that in my opinion it meets the academic and professional standard required by the University as a dissertation for the degree of Doctor of Philosophy. Signed: _______________________________________________________ Antonio Lanzirotti, Ph.D. Member of dissertation committee iii ACKNOWLEDGEMENTS The path that brought me to the University of Delaware was relatively straight forward. While I was an undergraduate at the State University of New York at Brockport, I discovered a love for soil science. A resource soil scientist from the USDA in New York State inspired me to pursue an advanced degree in soil science, particularly soil chemistry. I was astounded and amazed at how complex it was, and I had to know more. It turns out that my advisor at SUNY Brockport, Dr. Mark Noll, graduated from the University of Delaware. It wasn’t until after I applied to the Plant and Soil Sciences Department that I realized he had actually graduated from Dr. Sparks’ group. This is truly a small world. I want to sincerely thank Dr. Sparks for providing me with a number of wonderful opportunities to learn and grow as a research scientist. Dr. Sparks has proved to be a superb advisor on many levels. I know I would not have made it through this process without his guidance. I have valued his scientific expertise during the course of this Ph.D. degree, and his integrity and generosity did not go unnoticed. If I discover a new mineral or element, I promise to name is Sparksite or Sparksium. I figure it is the least that I could do. I would also like to thank the present and past members of the Environmental Soil Chemistry program for their camaraderie and friendship over the past five and half years. iv I sincerely wish them the best on their future endeavors. I especially want to thank Ryan Tappero (I am his “second wife” after all), Brandon Lafferty (whose willingness to help is immeasurable), and Matt Ginder-Vogel (who helped guide me through the land of XAS). Jerry Hendricks also needs to be recognized has he is an integral part of this group. The soil chemistry group would not be where it is today without his help. I would also like to thank the secretarial staff of Townsend Hall, especially Amy Broadhurst and Kathy Fleischut. They run a well oiled machine. Many sincere thanks go to the rest of my committee members. Each of you have provided insight into my research and have taught me to think outside of my realm of soil science. Working with Dr. Saylor and his group have definitely broadened my horizons. I can honestly say that I didn’t think I would be chasing chickens in a large poultry house or examining poultry livers when I first embarked on this journey. Tony Lanzirotti from the NSLS has been an enormous help. I could not have gotten through all of this work without his guidance. I would like to thank Dr. Sims for his input and support, particularly on the soils portion of this research. It has been a real pleasure to have each of you serve on my committee. Last but not least, I would like to dedicate this work to both my New York and Delaware families. My parents have always been a source of amazing support throughout this journey. I could not have made it this far without them. I have thoroughly enjoyed my life in Delaware, due to the great experience of working here at the University of Delaware and to wonderful people that I have met while living here. ~ Jennifer Seiter v TABLE OF CONTENTS LIST OF TABLES x LIST OF FIGURES xiii ABSTRACT xx Chapter 1: Literature Review: Arsenic and Its Role in the Environment 1.0. Research Rationale and Objectives……………...………………………… 22 1.0.0. Rationale and Focus…………………….…..……………………….. 22 1.0.1. Objectives………………………………..…………………………... 23 1.1. Arsenic and Its Origin……………………….…………….………………. 24 1.1.0. What is Arsenic? …………………………………….…………….. 24 1.1.1. Where Does As Come from? ………………………………………. 25 1.2. Arsenic Speciation in Natural Environments……………………………... 26 1.3. Arsenic in Agriculture…………………………………………………….. 29 1.3.0. General Agricultural Uses of Arsenic in Agriculture……………….. 29 1.3.1. The Use of As in Poultry Industry………………………………….. 31 1.3.2. Government Regulation on Arsenic in Poultry Feeds……………… 33 1.3.3. Poultry Industry on the Delmarva Peninsula……………………….. 35 1.4. Poultry Digestion and Internal Environment……………………………… 36 1.4.0. Avian Digestive and Excretory Systems…………………………… 36 1.4.1. Chemical Environment of the Digestive Tract……………………… 38 1.4.2. Microbial Communities and Their Functions in the Digestive System. 40 1.5 Bioaccumulation of Arsenic………………………………………………. 42 1.5.0Arsenic Accumulation in Plants and Animals………………………... 42 1.5.1 Arsenic Toxicity……………………………………………………… 45 1.5.2. Arsenic and Amino Acid Binding Processes………………………... 46 1.5.3. Arsenic Accumulation in Poultry Tissues…………………………… 52 1.6. Poultry Litter Management Practices…………………………………….. 53 1.7. Arsenic Speciation of Poultry Litter……………………………………… 56 1.7.0. Arsenic Speciation…………………………………………………. 56 1.7.1. Roxarsone Degradation…………………………………………….. 58 1.7.2. Arsenstruvite………………………………………………………. 59 vi 1.8. Arsenic Sorption onto Soils………………………………………………. 60 1.8.0. Arsenic Characterization in Soils…………………………………. 60 1.8.1. Fate and Transport of Arsenic in Poultry Litter Amended Soils…..... 63 1.8.2. Quantifying Retention and Speciation of Arsenic in Soils………….. 65 1.8.3. Quantifying Desorption of Arsenic in Soils……………………….. 70 1.9. The use of Synchrotron Spectroscopy in As Speciation………………….. 73 1.9.0. X-ray Absorption Spectroscopy Described……………………….. 73 1.9.1. Advantages of Using a Synchrotron Microprobe…………………. 77 1.9.2. Using X-ray Absorption Spectroscopy with Redox Sensitive 78 Elements……………………………………………………………………….. 1.9.3. Synchrotron Light Sources…………………………………………. 79 1.10. Introduction to Subsequent Chapters……………………………………. 80 1.11. References………………………………………………………………. 81 Chapter 2: Arsenic Status in Delaware Soils 2.0. Abstract……………………………………………………………………. 99 2.1. Introduction………………………………………………………………... 100 2.1.0. Background Information…………………………………………….. 100 2.1.1. Objectives and Focus……………………………………………….. 105 2.2. Methods and Materials…………………………………………………….. 106 2.2.0. Soil Sample Collection…………………………………………….... 106 2.2.1. Soil Characterization and Analysis………………………………….. 106 2.2.2. Arsenic Sorption by Selected Soil Horizons……………………….... 107 2.2.3. Arsenate Competitive Studies……………………………………….. 109 2.2.4. Arsenic Desorption from Soil Horizons……………………………. 110 2.3. Results and Discussion……………………………………………………. 110 2.3.0. Soil Classification………………………………………………….... 110 2.3.1. Physiochemical Characteristics of Delaware Agricultural and 111 Forested Soils…………………………………………………………………... 2.3.2. Arsenic Status of Agricultural and Forested Soils…………………... 114 2.3.3. Arsenic Sorption by Soil Horizons…………………………….…….
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