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Investigation of Zeolite Systems: Focus on Fenton Chemistry Oxidative Stress from Asbestos Like Minerals and Zeolite-Based Dissolved Oxygen Sensing

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Investigation of Zeolite Systems: Focus on Fenton Chemistry Oxidative Stress from Asbestos Like Minerals and Zeolite-Based Dissolved Oxygen Sensing INVESTIGATION OF ZEOLITE SYSTEMS: FOCUS ON FENTON CHEMISTRY OXIDATIVE STRESS FROM ASBESTOS LIKE MINERALS AND ZEOLITE-BASED DISSOLVED OXYGEN SENSING DISSERTATION Presented in Partial Fulfillment of the Requirements for the Degree Doctor of Philosophy in the Graduate School of The Ohio State University By Toni Ann Ruda ***** The Ohio State University 2007 Dissertation Committee: Approved by Prof. Prabir K. Dutta, Advisor Prof. Susan Olesik _________________________________ Prof. W. James Waldman Advisor Graduate Program in Chemistry Prof. Bernard LaLonde ABSTRACT The research in this dissertation has focused on studying zeolite systems in two areas. The first goal of the research was to examine particle properties leading to hydroxyl radical related toxicity. The second goal was to create an efficient optical oxygen sensor for intracellular monitoring of oxygen. Asbestos is known to cause a variety of respiratory health problems; however, the exact mechanism leading to these problems is unknown. Typically, asbestos participates in Fenton chemistry producing hydroxyl radicals which lead to toxicity in vivo. During these times of oxidative stress in vivo, the intracellular oxygen is under flux. Being able to monitor the intracellular oxygen concentration can provide critical information related to the condition of the cell. Initially, studies were performed focusing on Fenton chemistry and oxidative stress from asbestos like minerals. Researchers are striving to elucidate an exact mechanism of asbestos toxicity because it has led and is still leading to multiple respiratory health problems. The physicochemical characteristics of asbestos contributing to respiratory health problems are not fully defined. The goal of this research was to correlate particle toxicity with physicochemical characteristics to help eventually elucidate the mechanism of asbestos toxicity. After the asbestos is inhaled, the particles interact with lung lining fluid, which contains antioxidants. The antioxidants ii have the ability to reduce ferric iron on the asbestos particles. The particles are then phagocytosed by macrophages, and subsequently an oxidative burst is induced in an effort to remove the inhaled particles. During this oxidative burst, hydrogen peroxide is produced inducing Fenton chemistry with the ferrous iron. Mimicking the oxidative burst process with minerals having properties similar to that of asbestos, but different toxicities, can provide great insight as to the critical physicochemical characteristics related to toxicity. Mordenite, a benign aluminosilicate, and erionite, a highly carcinogenic aluminosilicate, were iron ion-exchanged, exposed to antioxidants, and then exposed to hydrogen peroxide to induce oxidative burst. Monitoring the production of hydroxyl radicals determined if differences between the physicochemical properties of the mineral aluminosilicates resulted in differing Fenton activity. The conclusion of this study was that the coordination of the iron on the mineral surface plays an important role in Fenton activity. During the oxidative burst, a flux of oxygen within the cell occurs. Being able to monitor the hydroxyl radical production, along with the oxygen consumption, would be useful in understanding the full mechanism of what happens during particle inhalation. Furthermore, efficient monitoring of intracellular oxygen concentration is an important area of research that can provide insight as to cellular function and status. This leads into the second and main component of this research, creation of efficient optical oxygen with a novel matrix to prevent probe leaching and provide linear Stern-Volmer plots. The probe utilized is tris(2,2’-bipyridyl) ruthenium(II), and the matrix is siliceous zeolite-Y. The goal of this research was to improve the loading level of a sensor previously iii established in our research group then demonstrate the sensor’s abilities in the following areas: (1) monitoring dissolved oxygen in solution via a glucose oxidase assay as an in situ measurement via emission quenching, (2) monitoring dissolved oxygen in macrophage cells during an oxidative burst via confocal microscopy, and (3) demonstrating the ability to immobilize the ruthenium loaded zeolite on the end of a fiber optic and discussing future optimization to improve the sensing parameters. The synthetic scheme utilized to load the tris(2,2’-bipyridyl) ruthenium(II) inside of the siliceous zeolite-Y supercages was altered by changing the ruthenium precursor and some of the experimental conditions to improve the loading level. The results showed an improved loading level of the ruthenium complex in the zeolite, which did not leach and gave linear Stern-Volmer plots during oxygen quenching experiments. In the realms of intracellular monitoring of dissolved oxygen as well as fiber optic sensing, parameters have been established demonstrating the working ability of the ruthenium loaded zeolite providing a basis for future optimization. iv I would like to dedicate this work to the three most important people in my life… My parents, Michael and Tanya Ruda… for always providing support, encouragement, and unconditional love. My soulmate, Brendan Eberenz… for believing in my ability and loving me completely. v ACKNOWLEDGMENTS I would like to thank Dr. Prabir K. Dutta, my advisor, for all of his support throughout my studies. Dr. Dutta is a true inspiration, always ready to bring ideas to the table, ask challenging questions, and provide support for his students. His blunt honesty, although sometimes difficult to take, has made me stronger. I especially appreciate that he is an excellent listener, whether I am talking about my ideas related to research, lack of ideas related to research, or ideas related to ways that I believe would make the lab run more efficiently. Thanks for all your guidance Dr. Dutta. My collaborator, Dr. James Waldman, also deserves a gigantic thanks. His help was integral to several parts of my research. Dr. Waldman’s biological knowledge amazes me. I appreciate that he answered my most basic biological questions without making me feel completely ignorant. Also, a huge help in the biological realm were Amber Nagy, a graduate student under Dr. Waldman, and Elizabeth Wheeler, who ran the confocal fluorescence microscope. I truly appreciate the time and assistance everyone provided. Thank you for all the biological knowledge. Team Dutta has played an important role in my research progress, and also in my daily life. I would like to thank current team members: Dr. Supriya Sabbani; Dr. Rajesh Cheruvallil for trying to bestow his infinite wisdom on me, even when he has to repeat vi something multiple times; Bill Schumacher for his support at IGERT functions; Brian Peebles for always telling me jokes even though he often has to explain them to me and also for being a good listener; Haoyu Zhang for his extreme kindness and helpfulness both in and out of the lab; Dedun Adeyemo for taking over my job (good luck) and providing me an outlet for wedding dress conversation; Kevin Cassidy for updating me on the crazy news happenings in the world; Julia Rabe for offering support while I was writing. I would also like to thank Team Dutta members who left within the past year or so: Dr. Yanghee Kim for sharing her huge amount of wisdom with me, as well as enjoying conversation about important topics such as fashion and what stores are having the best sales; John Spirig for interesting jokes and news stories, always taking care to be tasteful when I’m around. Finally, I would like to thank past Team Dutta members that I have had the pleasure of working with: Dr. Ramasamy Ramamoorthy; Dr. Marla DeLucia; Dr. Joe Trimboli; Dr. John Doolittle; Dr. Bob Kristovich; Dr. Nick Szabo; Dr. Jiun-Chan Yang; Dr. Kefa Onchoke; and Dr. Hyunjung Lee; as well as all the Team Dutta members that came before me (especially those that left behind well written notebooks). Thank you Team Dutta. My final thanks go to my mom, dad, and soon-to-be husband. I will do my best to put into words how much my parents and Brendan mean to me, although it will never match the intensity of the feelings in my heart. Mom and dad, you have truly played a profound role in my life; encouraging me to enroll in graduate school and providing the support I needed to finish graduate school. Dad, thank you for constantly emphasizing how important an education is by reminding vii me how little shopping I would be able to do without a good job. That has definitely been a motivating factor for me to get out of school and have more time to go shopping! Mom, you have supported me on a daily basis through phone conversations, helping me to rationalize how to balance this time in my life so that I get my work done efficiently but don’t miss out on the fun life has to offer. I appreciate you always reminding me that my hard work will pay off in the future, and that just having my degree will open more doors than I can imagine. Knowing that you both are ALWAYS on my side, supporting me, and having the willingness to do absolutely anything for me is amazing. You both provided an infinite amount of love and encouragement, especially when I was stressed and feeling down. I can’t thank you both enough for all you have done for me. The love and support you both provided to me was so necessary while in graduate school and while I was trying to complete this work. I am so incredibly lucky to truly have the best parents ever. I love you so much, and thank you for everything. Brendan, my soulmate and soon-to-be husband, thank you for dealing with me during the times of extreme stress and crankiness I’ve had while finishing my research. At times when I wouldn’t even want to deal with myself you still embrace me with encouragement and love. You have been incredible at picking up so much of the slack I left while working on my dissertation, both in taking care of the house chores and the wedding plans.
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