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Nano Research 2021, 14(9): 3329-3336 https://doi.org/10.1007/s12274-021-3358-3
Research Article | Issue | Published: 24 February 2021

Carbon-supported layered double hydroxide nanodots for efficient oxygen evolution: Active site identification and activity enhancement

Show Author's Information Shenlong Zhao1,3,§,  Detao Zhang2,4,§,  Shuai Jiang5,  Yanglansen Cui6,  Haijing Li5,  Juncai Dong5,  Zhirun Xie6,  Da-Wei Wang6,  Rose Amal6,  Zhenhai Xia4,  Liming Dai1( )
Australian Carbon Materials Centre (A-CMC), School of Chemical Engineering, The University of New South Wales, Sydney, NSW 2052, Australia
Center of Advanced Science and Engineering for Carbon (Case4Carbon), Department of Macromolecular Science and Engineering, Case Western Reserve University (CWRU), 10900 Euclid Avenue, Cleveland, OH 44106, USA
School of Chemical and Biomolecular Engineering, The University of Sydney, Sydney, NSW 2006, Australia
Department of Materials Science and Engineering, University of North Texas, Denton, TX 76203, USA
Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China
School of Chemical Engineering, The University of New South Wales, Sydney, NSW 2052, Australia

§ Shenlong Zhao and Detao Zhang contributed equally to this work.

Keywords:
oxygen evolution reaction, carbon nanomaterials, layered double hydroxide (LDH) nanodots, metal-organic framework (MOF) derivatives
Topics:
Electrocatalysts
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Zhao S, Zhang D, Jiang S, et al. Carbon-supported layered double hydroxide nanodots for efficient oxygen evolution: Active site identification and activity enhancement. Nano Research, 2021, 14(9): 3329-3336. https://doi.org/10.1007/s12274-021-3358-3
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Abstract Full text Electronic supplementary material About this article

In this study, we developed a novel confinement-synthesis approach to layered double hydroxide nanodots (LDH-NDs) anchored on carbon nanoparticles, which formed a three-dimensional (3D) interconnected network within a porous carbon support derived from pyrolysis of metal-organic frameworks (C-MOF). The resultant LDH-NDs@C-MOF nonprecious metal catalysts were demonstrated to exhibit super-high catalytic performance for oxygen evolution reaction (OER) with excellent operation stability and low overpotential (~ 230 mV) at an exchange current density of 10 mA·cm-2. The observed overpotential for the LDH-NDs@C-MOF is much lower than that of large-sized LDH nanosheets (321 mV), pure carbonized MOF (411 mV), and even commercial RuO2 (281 mV). X-ray absorption measurements and density functional theory (DFT) calculations revealed partial charge transfer from Fe3+ through an O bridge to Ni2+ at the edge of LDH-NDs supported by C-MOF to produce the optimal binding energies for OER intermediates. This, coupled with a large number of exposed active sides and efficient charge and electrolyte/reactant/product transports associated with the porous 3D C-MOF support, significantly boosted the OER performance of the LDH-ND catalyst with respect to its nanosheet counterpart. Apart from the fact that this is the first active side identification for LDH-ND OER catalysts, this work provides a general strategy to enhance activities of nanosheet catalysts by converting them into edge-rich nanodots to be supported by 3D porous carbon architectures.


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Electronic supplementary material
About this article

Carbon-supported layered double hydroxide nanodots for efficient oxygen evolution: Active site identification and activity enhancement

Show Author's information Shenlong Zhao1,3,§, Detao Zhang2,4,§, Shuai Jiang5, Yanglansen Cui6, Haijing Li5, Juncai Dong5, Zhirun Xie6, Da-Wei Wang6, Rose Amal6, Zhenhai Xia4, Liming Dai1( )
Australian Carbon Materials Centre (A-CMC), School of Chemical Engineering, The University of New South Wales, Sydney, NSW 2052, Australia
Center of Advanced Science and Engineering for Carbon (Case4Carbon), Department of Macromolecular Science and Engineering, Case Western Reserve University (CWRU), 10900 Euclid Avenue, Cleveland, OH 44106, USA
School of Chemical and Biomolecular Engineering, The University of Sydney, Sydney, NSW 2006, Australia
Department of Materials Science and Engineering, University of North Texas, Denton, TX 76203, USA
Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China
School of Chemical Engineering, The University of New South Wales, Sydney, NSW 2052, Australia

§ Shenlong Zhao and Detao Zhang contributed equally to this work.

Abstract

In this study, we developed a novel confinement-synthesis approach to layered double hydroxide nanodots (LDH-NDs) anchored on carbon nanoparticles, which formed a three-dimensional (3D) interconnected network within a porous carbon support derived from pyrolysis of metal-organic frameworks (C-MOF). The resultant LDH-NDs@C-MOF nonprecious metal catalysts were demonstrated to exhibit super-high catalytic performance for oxygen evolution reaction (OER) with excellent operation stability and low overpotential (~ 230 mV) at an exchange current density of 10 mA·cm-2. The observed overpotential for the LDH-NDs@C-MOF is much lower than that of large-sized LDH nanosheets (321 mV), pure carbonized MOF (411 mV), and even commercial RuO2 (281 mV). X-ray absorption measurements and density functional theory (DFT) calculations revealed partial charge transfer from Fe3+ through an O bridge to Ni2+ at the edge of LDH-NDs supported by C-MOF to produce the optimal binding energies for OER intermediates. This, coupled with a large number of exposed active sides and efficient charge and electrolyte/reactant/product transports associated with the porous 3D C-MOF support, significantly boosted the OER performance of the LDH-ND catalyst with respect to its nanosheet counterpart. Apart from the fact that this is the first active side identification for LDH-ND OER catalysts, this work provides a general strategy to enhance activities of nanosheet catalysts by converting them into edge-rich nanodots to be supported by 3D porous carbon architectures.

Keywords: oxygen evolution reaction, carbon nanomaterials, layered double hydroxide (LDH) nanodots, metal-organic framework (MOF) derivatives

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Publication history
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Acknowledgements

Publication history

Received: 20 December 2020
Revised: 19 January 2021
Accepted: 21 January 2021
Published: 24 February 2021
Issue date: September 2021

Copyright

© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021

Acknowledgements

S. L. Z. and L. M. D. conceived and designed the project. S. L. Z., D. T. Z., S. J., Y. C. and J. C. D. performed the experiments. S. L. Z., H. J. L., J. C. D., and Z. R. X. analysed and discussed the experimental results. L. M. D. and S. L. Z. drafted the manuscript. D.-W. W., R. A., Z. H. X., and L. M. D. joined the discussion of data and gave useful suggestions. This work was supported by The ARC (Nos. DP190103881 and FL190100126).

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