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Engineered Graphene and Metal-Organic Framework Nanocomposites for Supercapacitor and Sensing Applications

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Engineered Graphene and Metal-Organic Framework Nanocomposites for Supercapacitor and Sensing Applications Engineered Graphene and Metal-Organic Framework Nanocomposites for Supercapacitor and Sensing Applications A thesis submitted in fulfilment of the requirement for the degree of Master of Philosophy Chemical Engineering and Advanced Materials by Truc Van Ngo August 2019 School of Chemical Engineering and Advanced Materials Faculty of Engineering, Computer and Mathematical Sciences The University of Adelaide, South Australia SA 5000, Australia i Dedication To my parents “Hoa Van Ngo” and “Phuong Thi Lai” who are always beside me with their generous loves & To my beloved wife “Trang Hong Pham” and my mother-in-law “Hong Dieu Truong”, who always motive me with their endless support & To my 7-year-daughter “Kim Khanh Pham Ngo, who is smart and cute. i Table of contents Declaration............................................................................................................... iv Abstract..................................................................................................................... v Acknowledgments.................................................................................................... vi List of Tables........................................................................................................... viii List of Figures.......................................................................................................... ix Overview and thesis outline ................................................................................... xiii Publications from this Master of Philosophy project......................................... xvi References................................................................................................................ xviii Chapter 1. Literature review.................................................................................. 1 1.1 Background.......................................................................................................... 2 1.2 Graphene and its derivatives.............................................................................. 4 1.3 Metal-organic framework (MOF) materials....................................................... 24 1.4 Nanocomposites made of graphene derivatives and MOFs and applications. 27 1.5 Research gaps.......................................................................................................32 1.6 Aims and objectives of the thesis and thesis outline......................................... 33 1.7 Significance and novelty..................................................................................... 33 References.................................................................................................................. 35 Chapter 2. Methodology.......................................................................................... 43 2.1 Chemical and raw materials............................................................................... 44 2.2 Material preparation........................................................................................... 44 2.3 Materials characterisations techniques............................................................... 46 Conclusion................................................................................................................. 53 References.................................................................................................................. 54 Chapter 3. Hybridisation of MOFs and graphene: a new strategy for synthesis of highly porous 3D structures for high performing supercapacitors............... 55 3.1 Introduction.......................................................................................................... 58 ii 3.2 Experimental........................................................................................................ 61 3.3 Results and discussions........................................................................................ 65 Conclusion................................................................................................................. 80 References.................................................................................................................. 81 Chapter 4. Synthesis and characterisations of GQDs and HKUST-1@GQDs nanocomposites........................................................................................................ 85 4.1 Introduction.......................................................................................................... 86 4.2 Experimental........................................................................................................ 87 4.3 Results and discussions........................................................................................ 87 Conclusion................................................................................................................. 95 References.................................................................................................................. 96 Chapter 5. Pristine graphene (pG)–MOF nanocomposites for chemical vapour sensors...................................................................................................................... 98 5.1 Introduction......................................................................................................... 99 5.2 Experimental....................................................................................................... 100 5.3 Results and discussions....................................................................................... 101 Conclusion................................................................................................................. 109 References................................................................................................................. 110 Chapter 6. Conclusions and future works............................................................. 111 6.1 Conclusions.......................................................................................................... 111 6.2 Future works........................................................................................................ 113 iii Declaration I certify that this thesis is my work conducted at the Losic Research Group, School of Chemical Engineering and Advanced Materials, Faculty of Engineering, Computer and Mathematical and Sciences (ECMS), The University of Adelaide under the supervision of Professor Dusan Losic and Dr Tran Thanh Tung. The thesis was completed in the allocated period of scholarship program as a full-time international student of the master by research (Master of Philosophy, MPhil). I certify that this work contains no material which has been accepted for the award of any other degree or diploma in my name, in any university or other tertiary institution and, to the best of my knowledge and belief, contains no material previously published or written by another person, except where due reference has been made in the text. In addition, I certify that no part of this work will, in the future, be used in a submission in my name, for any other degree or diploma in any university or other tertiary institution without the prior approval of the University of Adelaide and where applicable, any partner institution responsible for the joint-award of this degree. I acknowledge that copyright of published works contained within this thesis resides with the copyright holder(s) of those works. I also give permission for the digital version of my thesis to be made available on the web, via the University’s digital research repository, the Library Search and also through web search engines, unless permission has been granted by the University to restrict access for a period of time. Name: Truc Van Ngo ID: 1697315 Signature: Date: 12 August 2019 iv Abstract The thesis focuses on the preparation of pristine graphene (pG), graphene oxide (GO) and graphene oxide quantum dots (GOQDs), and their nanocomposites with metal- organic frameworks (MOFs) including Cu-1,3,5 benzenetricarboxylate (BTC) framework (HKUST-1), zeolitic imidazolate framework (ZIF-8), and Zr6O4(OH)4(C8H4O4)6 framework (UiO-66), for supercapacitors and sensors applications. These engineered composite materials will find applications, firstly for supercapacitors; the GO/HKUST-1 composite material was laser-scribed, forming a novel morphology, highly porous and conductive L-rGO-C-MOF structure. As a result, the nano-porous architecture material displays a high capacitance of 390 F/g. Secondly, for sensor application, the pG-MOF nanocomposites show acceptable sensing responses towards different chemical vapours and their discriminations. In short, the thesis is dealing with extensive experiments of synthesis and characterisation of nanocomposite materials based on graphene derivatives and MOFs. The remarkable properties of these materials are expected to place them as promising materials for energy storage and sensing devices. v Acknowledgements The completion of this Master of Philosophy (MPhil)’s thesis would not be possible without the enormous support of my supervisors, colleagues, and my family. I would like to express my immense gratitude to all who were always beside me and contributed to this success of my research journey in different ways. The first and foremost, I would like to express my most profound gratitude to Prof. Dusan Losic, who greatly supervised, instructed and directed me from the beginning of my candidature. Without his support and supervision,
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