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Fabrication of Advanced Electrode Materials for Electrochemical FABRICATION OF ADVANCED ELECTRODE MATERIALS FOR ELECTROCHEMICAL SUPERCAPACITOR APPLICATIONS FABRICATION OF ADVANCED ELECTRODE MATERIALS FOR ELECTROCHEMICAL SUPERCAPACITOR APPLICATIONS By RYAN YUK YEUNG POON, B.ENG A Thesis Submitted to the School of Graduate Studies in Partial Fulfillment of the Requirements for the Degree Doctor of Philosophy McMaster University © Copyright by Ryan Poon, December 2019 Ph.D. Thesis Ryan Yuk Yeung Poon McMaster University Materials Science and Engineering McMaster University DOCTOR OF PHILOSOPHY (2019) Hamilton, Ontario (Materials Science and Engineering) TITLE: Fabrication of Advanced Electrode Materials for Electrochemical Supercapacitor Applications AUTHOR: Ryan Yuk Yeung Poon, B.Eng. (McMaster University, Canada) SUPERVISOR: Dr. Igor Zhitomirsky, Distinguished Engineering Professor, Ph.D., P.Eng. NUMBER OF PAGES: CCXVI, 216 II Ph.D. Thesis Ryan Yuk Yeung Poon McMaster University Materials Science and Engineering Lay Abstract In modern society, the demand for clean and renewable energy have grown drastically and there is a need in development of advanced energy storage devices. Currently, the most common energy storage devices are batteries or conventional capacitors. Batteries can store a large amount of energy, however they are limited by their low power performance. Capacitors can charge and discharge rapidly, but the amount of energy stored is relatively low. Other than batteries and capacitor, electrochemical supercapacitors are emerging energy storage devices that offer the advantages of high power and energy density, fast charge-discharge and long lifetime. The objective of this work was to develop advanced nanocomposite electrode materials for electrochemical supercapacitor applications. New colloidal processing strategies have been developed and advanced dispersants were employed for the fabrication of high performance nanocomposites for electrochemical supercapacitor applications. The results presented in this work showed exceptional performances compared to literature data and paved a new way for further developments. III Ph.D. Thesis Ryan Yuk Yeung Poon McMaster University Materials Science and Engineering Abstract Electrochemical supercapacitors (ESs) are currently under development for electronics and automotive applications due to their hybrid properties inherited from batteries and capacitors. ESs exhibit higher power densities than batteries and energy densities than capacitors, and offer long cyclic life and rapid charge-discharge suitable for many applications. A promising candidate of electrode materials is manganese dioxide (MnO2), which has the advantages of high theoretical capacitance, low cost and environmentally friendly. However, the low electronic and ionic conductivities of MnO2 have limited its performance for practical applications. It has been demonstrated in literature that composite materials, which consist of conductive additives such as multi-walled carbon nanotubes (MWCNTs) and MnO2 can address this problem, however further investigations are required to produce ESs with superior performance for real-world applications. In this dissertation, novel colloidal fabrication techniques have been developed and advanced dispersants were employed to fabricate advanced nanocomposite electrodes. MnO2-MWCNTs composite electrode was fabricated with use of multifunctional dispersant. The multifunctional dispersant cetylpyridinium chloride (CPC) showed good dispersion of MWCNTs and capability of forming complex with the precursor of MnO2, which improved the homogeneity of the composite and generated unique morphology. The MnO2-MWCNTs composite electrode fabricated exhibited remarkable areal capacitance at high active mass loadings. New scalable fabrication technique was developed for MnO2- MWCNTs by using high solubility sodium permanganate (NaMnO4) precursor. The IV Ph.D. Thesis Ryan Yuk Yeung Poon McMaster University Materials Science and Engineering fabricated composite electrode showed superior performance compared to electrodes fabricated by other colloidal techniques at similar mass loading. Liquid-liquid extraction was employed to address the problem of particles agglomeration upon drying. Bio-inspired advanced extractor lauryl gallate (LG) was used for liquid-liquid extraction of particles. LG has organic catechol group allowed for strong adsorption on inorganic particles. Using LG as an advanced extractor has facilitated the transfer of particles from aqueous to organic phase to prevent agglomeration associated with drying procedure and improved mixing with MWCNTs. Advanced dispersants from bile acid salts and charged aromatic dyes families such as sodium taurodeoxychloate (TDS) and tolonium chloride (TL) were used as MWCNTs dispersants, to fabricate composite electrode with alternative metal oxides such as Mn3O4 and V2O3. Furthermore, 3,4-dihydroxybenzaldhyde (DHB) was investigated as a dispersing agent for Mn3O4 and used to fabricate Mn3O4-MWCNTs composite electrode with TL by Schiff base formation. Mn3O4 offers the advantages of small particle size compared to MnO2, and can be converted to MnO2 by electrochemical cycling to enhance capacitive performance. V2O3 was considered as an alternative to MnO2 due to its metallic conductivity at room temperature. An activation procedure has been developed, which promoted the formation of capacitive V2O5 surface layer on conductive V2O3 to increase capacitance. The advanced dispersants have shown excellent dispersion of MWCNTs in aqueous solutions at low concentrations and facilitated the formation of homogeneous composite with Mn3O4 and V2O3. Activation procedures were developed for the Mn3O4 and V2O3 composite electrodes, and the electrodes with high active mass loadings showed exceptional performance after activation. V Ph.D. Thesis Ryan Yuk Yeung Poon McMaster University Materials Science and Engineering Acknowledgement First and foremost, I would like to thank my supervisor Dr. Igor Zhitomirsky for his guidance and constant support throughout my Ph.D. study. You have always been a kind, patience, euthanasic and hardworking supervisor, and have inspired me to carry out high quality research to complete my Ph.D. and this dissertation. You are someone that I look up to, and I feel extremely lucky to be one of your students. I would also like to thank my committee members Dr. Kish and Dr. Kitai, for their valuable inputs and suggestions, and made me realize it is important to know my own weaknesses in research and life. There are also many technicians and staff who helped me in the past few years as well, and I would like to thank Dr. Britten, Victoria Jarvis, Chris Butcher, Danielle Covelli, Doug Culley, Xiaogang Li, Ed McCaffery and Mary-Anne Bechamp for their assistance and support. It was my pleasure to be part of the Zhitomirsky group, and I have enjoyed the time we spent together and the discussions we had about our research and daily life. I would like to thank Jordan Milne, Amanda Clifford, Ri Chen, Aseeb Syed, Cameron Wallar, Mustafa Ata, Haoyu Fan, Pamela Liang, Mohamed Nawwar, Heyfer Zhao and Jessica Liu for their help with research, coursework and daily life. I am incredibly grateful for the endless love and support from my family. Thank you, mom and dad, for your continuous support of my decision, and for sharing your experience in life with me. To my sister and brother, Stephanie and Andrew, thank you for always being there for me and help me through my problems. VI Ph.D. Thesis Ryan Yuk Yeung Poon McMaster University Materials Science and Engineering Last but not least, I would like to thank my love Michele Tsang. I could not have achieved my goals without your encouragement, and I am glad to have you by my side all these years. Thank you for your unconditional love and support in both my academic and personal life. VII Ph.D. Thesis Ryan Yuk Yeung Poon McMaster University Materials Science and Engineering Declaration of Academic Achievements This dissertation was used to fulfill the requirements of the degree Doctor of Philosophy. The major research project was conducted from September 2016 to August 2019. The results of this dissertation were published in 6 papers in peer-reviewed journals, which were listed below: 1. R. Poon and I. Zhitomirsky, “Supercapacitor electrode with high active mass loading”, MRS Communications, vol.8, no. 3, pp. 1135-1138,2018. 2. R. Poon, X. Zhao, M.S. Ata, A. Clifford and I. Zhitomirsky, “Phase transfer of oxide particles for application in thin films and supercapacitors”, Ceramics International, vol. 43, no.11, pp. 8314-8320, 2017. 3. R. Poon and I. Zhitomirsky, “High areal capacitance of Mn3O4-carbon nanotube electrodes”, Materials Letters, vol. 215, pp.4-7, 2018. = = 4. C.J. Wallar , R. Poon and I. Zhitomirsky, “High areal capacitance of V2O3–carbon nanotube electrodes”, Journal of the Electrochemical Society, vol. 164, no. 14, pp. A3620-A3627, 2017. (=: Authors contribute equally to this publication) 5. W. Liang=, R. Poon= and I. Zhitomirsky, “Zn-doped FeOOH-polypyrrole electrodes for supercapacitors”, Materials Letters, vol. 1, no. 1, pp. 124-133, 2019. (=: Authors contribute equally to this publication) = = 6. R. Poon , W. Liang and I. Zhitomirsky, “Mn3O4 and (ZnFe)OOH composites for supercapacitors with high active mass”, Metallurgical and Materials Transaction A, Accepted. (=: Authors contribute equally to this publication) In addition to the work presented above, I have also contributed to 9 papers that are published and submitted in peer-reviewed journals
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