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Enhanced graphitic domains of unreduced graphene oxide and the interplay of hydration behaviour and catalytic activity
Affiliation:1. School of Materials Science and Engineering, University of New South Wales, Sydney, NSW 2052, Australia;2. Particles and Catalysis Research Laboratory and School of Chemical Engineering, University of New South Wales, Sydney, NSW 2052, Australia;3. Department of Materials Science and Engineering Research Institute of Advanced Materials (RIAM), Seoul National University, Seoul 08826, South Korea;4. Electron Microscopy Unit, Mark Wainwright Analytical Centre, University of New South Wales, Sydney, NSW 2052, Australia;5. Surface Science Laboratory, Toyota Technological Institute, Nagoya 468-8511, Japan;6. Sydney Water, Parramatta, New South Wales 2125, Australia;7. School of Physics and Astronomy, University of Manchester, Manchester M13 9PL, UK;1. Kurnakov Institute of General and Inorganic Chemistry of Russian Academy of Science, Leninskii Pr. 31, 119991, Moscow, Russian Federation;2. M.V. Lomonosov Moscow State University, Faculty of Physics, Leninskie Gory 1-2, Moscow, 119991, Russian Federation;3. Advanced Imaging Core Facility, Skolkovo Institute of Science and Technology, Moscow, 121205, Russian Federation;4. Laboratory for Advanced Carbon Nanomaterials, Chemical Institute, Kazan Federal University, Kremlyovskaya str. 18, Kazan, 420008, Russian Federation;5. Department of Chemistry, Rice University, 6100, Main St., Houston, TX, 77005, USA;1. Centre for Sustainable Materials Research and Technology, School of Materials Science and Engineering, University of New South Wales, Sydney Australia;2. UNESCO Centre for Membrane Science and Technology, School of Chemical Engineering, University of New South Wales, Sydney Australia;3. Sydney Water, Parramatta, New South Wales 2125, Australia;1. Department of Materials Science and Engineering, The Pennsylvania State University, University Park, PA 16802, USA;2. Department of Engineering Science and Mechanics, Materials Research Institute, The Pennsylvania State University, University Park, PA 16802, USA;3. Institute of Nano Biomedicine and Engineering, Department of Instrument Science & Engineering, School of Electronic Information and Electrical Engineering, Shanghai Jiao Tong University, Dongchuan Road, Shanghai 200240, China;1. Advanced Fuel Fabrication Facility, Bhabha Atomic Research Centre, Tarapur, Maharashtra, 401502, India;2. Radiochemistry Division, Bhabha Atomic Research Centre, Trombay, Mumbai, 400085, India;1. School of Chemistry and Chemical Engineering, School of Material Science and Engineering, Hefei University of Technology, Hefei, Anhui 230009, PR China;2. AnHui Huanrui Heating Manufacturing Co., Ltd., Hefei 231600, PR China;1. Department of Physics & Astronomy, University of Kansas, Lawrence, KS 66045, USA;2. Department of Electrical Engineering & Computer Science, University of Kansas, Lawrence, KS 66045, USA
Abstract:Previous studies indicate that the properties of graphene oxide (GO) can be significantly improved by enhancing its graphitic domain size through thermal diffusion and clustering of functional groups. Remarkably, this transition takes place below the decomposition temperature of the functional groups and thus allows fine tuning of graphitic domains without compromising with the functionality of GO. By studying the transformation of GO under mild thermal treatment, we directly observe this size enhancement of graphitic domains from originally ≤40 nm2 to >200 nm2 through an extensive transmission electron microscopy (TEM) study. Additionally, we confirm the integrity of the functional groups during this process by a comprehensive chemical analysis. A closer look into the process confirms the theoretical predicted relevance for the room temperature stability of GO and the development of the composition of functional groups is explained with reaction pathways from theoretical calculations. We further investigate the influence of enlarged graphitic domains on the hydration behaviour of GO and the catalytic performance of single atom catalysts supported by GO. Additionally, we show that the sheet resistance of GO is reduced by several orders of magnitude during the mild thermal annealing process.
Keywords:Graphene oxide  Graphitic domains  Transmission electron microscopy  Oxygen evolution reaction  Laminar membranes  Mass transport
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