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Dyuthi T-2428.Pdf DEVELOPMENT OF ELECTROCHEMICAL AND OPTICAL SENSORS FOR SOME FOOD ADDITIVES AND PHARMACEUTICALS Thesis submitted to Cochin University of Science and Technology in partial fulfilment of the requirements for the award of the degree of Doctor of Philosophy in Chemistry by Soumya T. Cyriac Department of Applied Chemistry Cochin University of Science and Technology Kochi – 22 October 2017 Development of Electrochemical and Optical Sensors for some Food Additives and Pharmaceuticals Ph.D. Thesis under the Faculty of Sciences By Soumya T. Cyriac Research Fellow Department of Applied Chemistry Cochin University of Science and Technology Kochi, India 682022 Email: [email protected] Supervising Guide Dr. K. Girish Kumar Professor & Head Department of Applied Chemistry Cochin University of Science and Technology Kochi, India 682022 Email: [email protected] Department of Applied Chemistry Cochin University of Science and Technology Kochi, India 682022 October 2017 DEPARTMENT OF APPLIED CHEMISTRY COCHIN UNIVERSITY OF SCIENCE AND TECHNOLOGY KOCHI - 682022, INDIA Dr. K. Girish Kumar Tel: 0484 - 2575804 Professor & Head E-mail: [email protected] Date: 30 October 2017 Certified that the work entitled “Development of Electrochemical and Optical Sensors for Some Food Additives and Pharmaceuticals”, submitted by Ms. Soumya T. Cyriac, in partial fulfilment of the requirements for the degree of Doctor of Philosophy in Chemistry to Cochin University of Science and Technology, is an authentic and bonafide record of the original research work carried out by her under my supervision at the Department of Applied Chemistry. Further, the results embodied in this thesis, in full or in part, have not been submitted previously for the award of any other degree. All the relevant corrections and modifications suggested by the audience during the pre-synopsis seminar and recommended by the Doctoral committee have been incorporated in the thesis. K. Girish Kumar (Supervising Guide) I hereby declare that the work presented in this thesis entitled “Development of Electrochemical and Optical Sensors for some Food Additives and Pharmaceuticals” is based on the original work carried out by me under the guidance of Dr. K. Girish Kumar, Professor & Head, Department of Applied Chemistry, Cochin University of Science and Technology and has not been included in any other thesis submitted previously for the award of any degree. Kochi-22 Soumya T. Cyriac 30/10/2017 Wxw|vtàxw àÉ `ç ctÜxÇàá‹ Completion of this work was possible with the support extended by several people. I would like to acknowledge and thank each one of them for their help and guidance during this amazing journey. Words are deserting my thoughts to express my thanks and gratitude to Dr. K. Girish Kumar, Professor & Head, Department of Applied Chemistry, Cochin University of Science and Technology, Kochi, who has given me values of sincerity, perseverance, tolerance, patience to life and personality. I am extremely grateful to him for providing resolute guidance and valuable advice which always came with faith and confidence in my abilities during my research programme. I also remain indebted for his fatherly support during the times when I was really down. Without his support, it would have been very difficult to complete this research work successfully. It is my privilege to have Dr. K. Sreekumar, Professor, Department of Applied Chemistry, Cochin University of Science and Technology, Kochi, as my Doctoral Committee Member. I am thankful to him for resolute guidance, constructive counsel, critical appreciation and continuous help during course of this study for which I shall remember him with great respect for all the time to come. I take this opportunity to express my extreme thanks to all faculty members of Department of Applied Chemistry, CUSAT for their inspiration and timely help. I also acknowledge help of various non – teaching staff members who rendered me a lot of support. At this point, special mention must be made about Dr. Anitha I, Principal, Government College, Kongad, Palakkad, for her keen interest in all my matters with extreme gratefulness in my mind. I express my gratefulness to Manager Rev. Fr. Nelson Thaiparambil, Principal Dr. Mathew V and Management of St. Michael’s college, Cherthala for all the supports given to me. I acknowledge my colleagues at St. Michael’s college, Cherthala, Dr. Manoj, Seena miss, Dr. Peral, Liya miss, Libin sir, Dr. Beena and Dr. Saranya for their help and good wishes. Research scholars often talk about loneliness during their course of study but this is something which I never experienced in our lab. Very special thanks to all my lab mates for imparting a lot of help by sharing professional skills and knowledge. During my initial period of research, my seniors Dr. Rema, Dr. Sindhu, Dr. Renjini, Dr. Leena, Dr. Laina, Dr. Sobhana, Dr. Theresa, Dr. Divya and Dr. Anuja had given me valuable tips that made my research to go unhindered. My dear lab mates, Jesny chechi, Dr. Jintha, Dr. Monica, Zafna, Unni, Ammu, Ambily, Sheela Miss, Shalini, Sanu and Manna have all extended their support in a very special way, and I gained a lot from them, through their personal and scholarly interactions. I am greatly indebted to Unni and Ammu for their untiring assistance during preparation of thesis. No appropriate word could be traced in the lexicon of heart for affection, moral support and constant inspiration bestowed upon me by my friends Sreejith, Ajith, Sruthy, Meera, Shanty and Gopika. I would like to extend my gratefulness to all my friends in polymer, biochemistry, physical, organic and inorganic labs. A special thanks to Dr. Rakesh and Dr. Rethikala, my M.Sc. classmates, for their help, support and well wishes. I owe a lot to my parents, who encouraged and helped me at every stage of my personal and academic life and longed to see this achievement come true. I deeply miss my father, who is not with me to share this joy. Words cannot express how much I am grateful to my mother, sisters and in-laws for all the sacrifices that you’ve made on my behalf. I am also grateful to my uncles, aunties and cousins who have supported me all way along. I am very much indebted to my in-laws who supported me in every possible way to see completion of this work. Your prayer has been the force which sustained me this far. I fondly recall with love, emotional support and consistent encouragement exhibited by my husband and son. For the financial services rendered, I thank Council of Scientific and Industrial Research (CSIR), India for fellowship, Directorate of Extramural Research and Property Rights, DRDO, New Delhi and Kerala State Council for Science, Technology and Environment, Kerala for the funding assistance in the form of projects. I am happily acknowledging help extended by scientists at STIC, CUSAT, Department of Photonics, CUSAT and Amrita Center for Nanosciences, Amrita University, Kochi for analyzing various samples. Above all, I bow myself in front of the almighty for all blessings showered upon me throughout my life. Soumya T. Cyriac Sensors have found extensive applications in diverse fields such as medicine, agriculture, industry, defence and transport. They offer attractive means to solve concerns related to everyday life of man. Sensors and sensing devices are increasingly captivating the attention of scientists across globe. Chemical sensors are miniaturised devices that can deliver information in presence of specific compounds or ions, even in complex biological samples. Chemical sensing consists of two major steps: recognition and transduction. Based on their signal transduction methods, chemical sensors can be categorized into electrochemical sensors, optical sensors, mass sensitive sensors and heat sensitive sensors. Electrochemical and optical sensors are developed for the determination of food additives and pharmaceuticals during the course of present study. Based on excellent electrochemical properties of glassy carbon electrodes (GCE), chemically modified with polymers and gold nanoparticles, four voltammetric sensors were developed for food additives, propyl gallate, tert-butylhydroquinone, ponceau 4R and acid green 50. Nanostructured gold nanoparticles were used for colorimetric determination of tetracycline, a pharmaceutical and ethylenediamine passivated carbon dots were used as fluorescent probes for food colorant, sunset yellow. Thesis entitled “Development of electrochemical and optical sensors for some food additives and pharmaceuticals” is divided into nine chapters. A brief outline of chapters is given below. Chapter 1 outlines a brief introduction to different types of chemical sensors and discusses in detail about voltammetric, colorimetric and fluorescent sensors. Detailed reviews on research work in the field of above sensors are also incorporated in this chapter. Chapter 2 gives a brief description of materials and methods used for fabrication of various sensors. Instruments used for different studies are also mentioned. Preparations of different kinds of buffer solutions and description of reference methods for validating applicability of developed sensors are also included in this chapter. Chapter 3 reports development of gold nanoparticle/poly(p-aminobenzenesulphonic acid) composite modified glassy carbon electrode (AuNP/poly(p-ABSA)/GCE) for electrochemical determination of propyl gallate (PG). Experimental parameters such as effect of pH, number of cycles of electrodeposition, number of cycles of electropolymerization and scan rate were
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