Enhanced graphitic domains of unreduced graphene oxide and the interplay of hydration behaviour and catalytic activity

Tobias Foller; Rahman Daiyan; Xiaoheng Jin; Joshua Leverett; Hangyel Kim; Richard Webster; Jeaniffer E. Yap; Xinyue Wen; Aditya Rawal; K. Kanishka H. De Silva; Masamichi Yoshimura; Heriberto Bustamante; Shery L.Y. Chang; Priyank Kumar; Yi You; Gwan Hyoung Lee; Rose Amal; Rakesh Joshi

doi:10.1016/j.mattod.2021.08.003

Enhanced graphitic domains of unreduced graphene oxide and the interplay of hydration behaviour and catalytic activity

Tobias Foller, Rahman Daiyan, Xiaoheng Jin, Joshua Leverett, Hangyel Kim, Richard Webster, Jeaniffer E. Yap, Xinyue Wen, Aditya Rawal, K. Kanishka H. De Silva, Masamichi Yoshimura, Heriberto Bustamante, Shery L.Y. Chang, Priyank Kumar, Yi You, Gwan Hyoung Lee, Rose Amal, Rakesh Joshi

Department of Materials Science and Engineering

Research output: Contribution to journal › Article › peer-review

18 Citations (Scopus)

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.

Original language	English
Pages (from-to)	44-54
Number of pages	11
Journal	Materials Today
Volume	50
DOIs	https://doi.org/10.1016/j.mattod.2021.08.003
Publication status	Published - 2021 Nov

Bibliographical note

Funding Information:
T.F. acknowledges the UNSW Scientia Ph.D. Scholarship and SSEAU Scholarship. The authors also thank Abdul Hakim and Fei Wang for helpful discussion. R.D. and R.A. acknowledge funding from the Australian Research Council (ARC) Training Centre for Global Hydrogen Economy ( IC200100023 ). R.D., R.A., and R.J. acknowledge funding from Digital Futures Grid Institute at UNSW Sydney . The authors acknowledge the facilities and the scientific and technical assistance of Microscopy Australia at the Electron Microscope Unit (EMU) within the Mark Wainwright Analytical Centre (MWAC) at UNSW Sydney and at The University of Sydney. G.H.L. acknowledge supports from the National Research Foundation (NRF) of Korea ( 2016M3A7B4910940 , 2018M3D1A1058793 , 2017R1A5A1014862 (SRC Program: vdWMRC Center)) and Research Institute of Advanced Materials, Institute of Engineering Research, and Institute of Applied Physics, Seoul National University.

Funding Information:
T.F. acknowledges the UNSW Scientia Ph.D. Scholarship and SSEAU Scholarship. The authors also thank Abdul Hakim and Fei Wang for helpful discussion. R.D. and R.A. acknowledge funding from the Australian Research Council (ARC) Training Centre for Global Hydrogen Economy (IC200100023). R.D. R.A. and R.J. acknowledge funding from Digital Futures Grid Institute at UNSW Sydney. The authors acknowledge the facilities and the scientific and technical assistance of Microscopy Australia at the Electron Microscope Unit (EMU) within the Mark Wainwright Analytical Centre (MWAC) at UNSW Sydney and at The University of Sydney. G.H.L. acknowledge supports from the National Research Foundation (NRF) of Korea (2016M3A7B4910940, 2018M3D1A1058793, 2017R1A5A1014862 (SRC Program: vdWMRC Center)) and Research Institute of Advanced Materials, Institute of Engineering Research, and Institute of Applied Physics, Seoul National University.

Publisher Copyright:
© 2021 Elsevier Ltd

All Science Journal Classification (ASJC) codes

Materials Science(all)
Condensed Matter Physics
Mechanics of Materials
Mechanical Engineering

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10.1016/j.mattod.2021.08.003

Cite this

Foller, T., Daiyan, R., Jin, X., Leverett, J., Kim, H., Webster, R., Yap, J. E., Wen, X., Rawal, A., De Silva, K. K. H., Yoshimura, M., Bustamante, H., Chang, S. L. Y., Kumar, P., You, Y., Lee, G. H., Amal, R., & Joshi, R. (2021). Enhanced graphitic domains of unreduced graphene oxide and the interplay of hydration behaviour and catalytic activity. Materials Today, 50, 44-54. https://doi.org/10.1016/j.mattod.2021.08.003

@article{1f2abadcb73f41118f0c1826397f89e0,

title = "Enhanced graphitic domains of unreduced graphene oxide and the interplay of hydration behaviour and catalytic activity",

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.",

author = "Tobias Foller and Rahman Daiyan and Xiaoheng Jin and Joshua Leverett and Hangyel Kim and Richard Webster and Yap, {Jeaniffer E.} and Xinyue Wen and Aditya Rawal and {De Silva}, {K. Kanishka H.} and Masamichi Yoshimura and Heriberto Bustamante and Chang, {Shery L.Y.} and Priyank Kumar and Yi You and Lee, {Gwan Hyoung} and Rose Amal and Rakesh Joshi",

note = "Funding Information: T.F. acknowledges the UNSW Scientia Ph.D. Scholarship and SSEAU Scholarship. The authors also thank Abdul Hakim and Fei Wang for helpful discussion. R.D. and R.A. acknowledge funding from the Australian Research Council (ARC) Training Centre for Global Hydrogen Economy ( IC200100023 ). R.D., R.A., and R.J. acknowledge funding from Digital Futures Grid Institute at UNSW Sydney . The authors acknowledge the facilities and the scientific and technical assistance of Microscopy Australia at the Electron Microscope Unit (EMU) within the Mark Wainwright Analytical Centre (MWAC) at UNSW Sydney and at The University of Sydney. G.H.L. acknowledge supports from the National Research Foundation (NRF) of Korea ( 2016M3A7B4910940 , 2018M3D1A1058793 , 2017R1A5A1014862 (SRC Program: vdWMRC Center)) and Research Institute of Advanced Materials, Institute of Engineering Research, and Institute of Applied Physics, Seoul National University. Funding Information: T.F. acknowledges the UNSW Scientia Ph.D. Scholarship and SSEAU Scholarship. The authors also thank Abdul Hakim and Fei Wang for helpful discussion. R.D. and R.A. acknowledge funding from the Australian Research Council (ARC) Training Centre for Global Hydrogen Economy (IC200100023). R.D. R.A. and R.J. acknowledge funding from Digital Futures Grid Institute at UNSW Sydney. The authors acknowledge the facilities and the scientific and technical assistance of Microscopy Australia at the Electron Microscope Unit (EMU) within the Mark Wainwright Analytical Centre (MWAC) at UNSW Sydney and at The University of Sydney. G.H.L. acknowledge supports from the National Research Foundation (NRF) of Korea (2016M3A7B4910940, 2018M3D1A1058793, 2017R1A5A1014862 (SRC Program: vdWMRC Center)) and Research Institute of Advanced Materials, Institute of Engineering Research, and Institute of Applied Physics, Seoul National University. Publisher Copyright: {\textcopyright} 2021 Elsevier Ltd",

year = "2021",

month = nov,

doi = "10.1016/j.mattod.2021.08.003",

language = "English",

volume = "50",

pages = "44--54",

journal = "Materials Today",

issn = "1369-7021",

publisher = "Elsevier",

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Foller, T, Daiyan, R, Jin, X, Leverett, J, Kim, H, Webster, R, Yap, JE, Wen, X, Rawal, A, De Silva, KKH, Yoshimura, M, Bustamante, H, Chang, SLY, Kumar, P, You, Y, Lee, GH, Amal, R & Joshi, R 2021, 'Enhanced graphitic domains of unreduced graphene oxide and the interplay of hydration behaviour and catalytic activity', Materials Today, vol. 50, pp. 44-54. https://doi.org/10.1016/j.mattod.2021.08.003

TY - JOUR

T1 - Enhanced graphitic domains of unreduced graphene oxide and the interplay of hydration behaviour and catalytic activity

AU - Foller, Tobias

AU - Daiyan, Rahman

AU - Jin, Xiaoheng

AU - Leverett, Joshua

AU - Kim, Hangyel

AU - Webster, Richard

AU - Yap, Jeaniffer E.

AU - Wen, Xinyue

AU - Rawal, Aditya

AU - De Silva, K. Kanishka H.

AU - Yoshimura, Masamichi

AU - Bustamante, Heriberto

AU - Chang, Shery L.Y.

AU - Kumar, Priyank

AU - You, Yi

AU - Lee, Gwan Hyoung

AU - Amal, Rose

AU - Joshi, Rakesh

N1 - Funding Information: T.F. acknowledges the UNSW Scientia Ph.D. Scholarship and SSEAU Scholarship. The authors also thank Abdul Hakim and Fei Wang for helpful discussion. R.D. and R.A. acknowledge funding from the Australian Research Council (ARC) Training Centre for Global Hydrogen Economy ( IC200100023 ). R.D., R.A., and R.J. acknowledge funding from Digital Futures Grid Institute at UNSW Sydney . The authors acknowledge the facilities and the scientific and technical assistance of Microscopy Australia at the Electron Microscope Unit (EMU) within the Mark Wainwright Analytical Centre (MWAC) at UNSW Sydney and at The University of Sydney. G.H.L. acknowledge supports from the National Research Foundation (NRF) of Korea ( 2016M3A7B4910940 , 2018M3D1A1058793 , 2017R1A5A1014862 (SRC Program: vdWMRC Center)) and Research Institute of Advanced Materials, Institute of Engineering Research, and Institute of Applied Physics, Seoul National University. Funding Information: T.F. acknowledges the UNSW Scientia Ph.D. Scholarship and SSEAU Scholarship. The authors also thank Abdul Hakim and Fei Wang for helpful discussion. R.D. and R.A. acknowledge funding from the Australian Research Council (ARC) Training Centre for Global Hydrogen Economy (IC200100023). R.D. R.A. and R.J. acknowledge funding from Digital Futures Grid Institute at UNSW Sydney. The authors acknowledge the facilities and the scientific and technical assistance of Microscopy Australia at the Electron Microscope Unit (EMU) within the Mark Wainwright Analytical Centre (MWAC) at UNSW Sydney and at The University of Sydney. G.H.L. acknowledge supports from the National Research Foundation (NRF) of Korea (2016M3A7B4910940, 2018M3D1A1058793, 2017R1A5A1014862 (SRC Program: vdWMRC Center)) and Research Institute of Advanced Materials, Institute of Engineering Research, and Institute of Applied Physics, Seoul National University. Publisher Copyright: © 2021 Elsevier Ltd

PY - 2021/11

Y1 - 2021/11

N2 - 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.

AB - 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.

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Enhanced graphitic domains of unreduced graphene oxide and the interplay of hydration behaviour and catalytic activity

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