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Migration Studies of Chloropropanols from Paperboard Packaging

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Migration Studies of Chloropropanols from Paperboard Packaging MIGRATION STUDIES OF CHLOROPROPANOLS FROM PAPERBOARD PACKAGING IN CONTACT WITH FOODSTUFFS by GREGORY V. PACE A Dissertation submitted to the Graduate School - New Brunswick Rutgers, The State University of New Jersey in partial fulfillment of the requirements for the degree of Doctor of Philosophy Graduate Program in Food Science written under the direction of Professor Thomas G. Hartman and approved by ________________________ ________________________ ________________________ ________________________ New Brunswick, New Jersey January 2011 ABSTRACT OF THE DISSERTATION Migration Studies of Chloropropanols from Paperboard Packaging in Contact with Foodstuffs By GREGORY V. PACE Dissertation Director: Professor Thomas G. Hartman The food processing of acid hydrolyzed vegetable protein (HVP) results in the chlorination of residual lipids to form chloropropanols. 3-chloro-1,2-propanediol (3-monochloropropane-1,2-diol; 3-MCPD), and 1,3-dichloro-2-propanol (1,3-DCP), are the most common chloropropanols found in HVP foods and also soy sauces. The manufacturing process of paperboard food packaging may also produce chloropropanols. 3-MCPD and 1,3-DCP can be found in paperboard when wet-strength resins made with epichlorohydrin are used. 1,3-DCP had been determined to be carcinogenic in rats and mice. 3-MCPD was a suspected carcinogen , and has recently been moving towards classification as a carcinogen. The European (EU) Commission and the US Food and Drug Administration (US FDA) have set maximum levels in food and food paperboard packaging for 3-MCPD ii and 1,3-DCP. In October 2010, 3-MCPD and 1,3-DCP were added to the California Proposition 65 list of compounds known to State to cause cancer. In this investigation, migration studies were conducted to measure 3-MCPD and 1,3-DCP migration into food simulants from the food contact side of polyethylene extrusion-coated paperboard beverage cartons, and also total immersion extractions of both polyethylene extrusion-coated and uncoated paperboard. It is shown that 3-MCPD, found at levels far above the regulatory limits for food packaging, does not migrate at a significant amount through the polyethylene extrusion-coated food contact surface of the paperboard. The aqueous extractions of the entire paperboard and food contact side extractions with aqueous and acidic food simulants were performed using US FDA and EU Commission standard and accelerated migration testing protocols. In these migration studies, an EU standard method for cold water total immersion extractions was compared to migration cell extractions to measure the chloropropanols migration into food simulant solvents from the entire paperboard and the isolated food contact side of polyethylene extrusion-coated paperboard beverage cartons. This research demonstrates that polyethylene food contact coated film can function as a barrier to the migration of 3-MCPD into the food packaged in a polyethylene extrusion-coated paperboard engineered for that purpose. iii ACKNOWLEDGEMENTS and DEDICATION Work included in this dissertation has been previously published by Taylor and Francis, Taylor and Francis Group, in Food Additives and Contaminants. Food Additives and Contaminants, Vol. 27, No. 6, June 2010, 844-891. Migration studies of 3-chloro-1,2-propanediol in polyethylene extrusion-coated paperboard food packaging. Gregory V. Pace and Thomas G. Hartman, © 2010 Taylor & Francis I would like to express my sincere appreciation to Dr. Thomas G. Hartman, who was both my M.S and Ph.D. Advisor, for his encouragement to enter the Food Science graduate program and allowing me to work under his guidance and direction on my graduate research. Dr. Hartman has taught me the highly desirable skills of translating technical knowledge and data into practical significance. I also thank my Ph.D. Committee members; Dr. Kit L. Yam, Dr. Henryk Daun, Dr. Tarik H. Roshdy for their valuable feedback on this research. I am grateful to Sun Chemical Corporation for funding my graduate work. In particular, Dr. Richard Durand and Dr. Richard Joyce for their constant support. I gratefully recognize: Dr. Bin Khoo for his laboratory work and training me on the initial samples, and Mr. Joseph Lech for his advice (Mass Spectrometry Lab, Rutgers University); Dr. Ryszard Sprycha and Mr. Richard Castino for their iv microscopy work, Dr. Saeid Savarmand for his teachings on writing research publications, Mr. Ali Virani for suggesting the use of the Dry-Vap® evaporating system, Dr. Danny Rich for his conversions of the graphics used in the published article, and the rest of my Analytical Characterization Teammates for their understanding and support (Sun Chemical). I thank Dr. Juanita Parris (Sun Chemical) and Dr. Tarik H. Roshdy (Hoffman La-Roche) for their official review of the article published in Food Additives and Contaminants, June 2010. I extend sincere gratitude to Dr. Kit Yam and his Graduate students – the “Y-Team”; Mr. Xi Chen, Mr. Vara Prodduck, Ms. Luni Shen (Rutgers University Food Science), for their professional-like assistance in converting the graphics, format, and flow of this Dissertation into a high quality publication. I thank the Department Of Food Science Faculty, Staff, and fellow Graduate Students whom I have had the pleasure and honor to work with, learn from, and collaborate with, during my Graduate studies at Rutgers University. To all my family, cousins and friends, in particular; Lori, Susan, Pat, Mike and Li, Chuck, Bernard, George, Bill, and Charmaine, who encouraged and challenged me, keeping me grounded and focused on this goal, regardless of the trials and tribulations swirling around me. v This Research and work for the Doctorate of Philosophy is Dedicated to: My Mom Terry, you are my Hero. Though you did not graduate high school, you emphasized the importance of a quality education. You sacrificed to ensure you provided me with that education, while demonstrating perseverance, unconditional love, passion for life, and the drive to overcome all obstacles. These became my model, teaching me the life-lessons that earn you an equal share in this Doctorate of Philosophy. My Sons, Lucien and Christian, Both of you are my Inspirations. Since you both were born, and through all our experiences, you taught me the importance of playing and having fun, happily living life, showing love, and dedication to purpose. vi TABLE OF CONTENTS ABSTRACT OF THE DISSERTATION...................................................................................ii ACKNOWLEDGEMENTS and DEDICATION ........................................................................iv TABLE OF CONTENTS .................................................................................................... vii LISTS OF TABLES ...........................................................................................................ix LIST OF ILLUSTRATIONS................................................................................................xi 1. INTRODUCTION ...................................................................................................... 1 2. LITERATURE REVIEW .............................................................................................. 9 2.1. Chloropropanols in Foods............................................................................. 9 2.2. Paper Chemicals in the Manufacturing of Paper and Paperboard.....................11 2.2.1. Paper and Paperboard Chemicals .....................................................11 2.2.2. Wet-Strength Paper Chemicals .........................................................13 2.2.3. Epichlorohydrin Containing Wet-strength Resins ................................15 2.3. Health Concerns of Chloropropanols ............................................................20 2.4. US FDA and EU Commission Regulatory Compliance of Chloropropanols in Foods and Food Packaging................................................................................................22 2.5. USA State of California Regulatory Listing of Chloropropanols ........................24 2.6. Methods for Determination of Chloropropanols .............................................25 2.7. Chloropropanols in Paperboard Packaging ....................................................32 2.8. 3-MCPD Migration through Polyethylene Extrusion-Coated Food Contact film into Foods .................................................................................................................36 3. OBJECTIVES...........................................................................................................38 3.1. Hypothesis.................................................................................................38 3.2. Research Objectives ...................................................................................38 3.3. Research Tasks...........................................................................................39 4. EXPERIMENTAL DESIGN..........................................................................................41 4.1. Reagents, Reference Standards, and Materials..............................................41 4.2. Sample Descriptions Used in this Research ...................................................46 4.3. Total Immersion Aqueous Extractions of the Entire Paperboard Cartons..........52 4.4. Experimental Design variables for Total Immersion Testing of Paperboard Cartons .................................................................................................................55
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