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Modifying electrocatalysts nanostructures and tuning their electronic properties through defects-oriented synthetic strategies are essential to improve the oxygen evolution reaction (OER) performance of electrocatalysts. Current synthetic strategies about electrocatalysts mainly target the single or double structural defects, while the researches about the synergistic effect of multiple structural defects are rare. In this work, the ultrathin NiFe layered double hydroxide nanosheets with a holey structure, oxygen vacancies and Ni3+ defects on nickel foam (NiFe-LDH-NSs/NF) are prepared by employing a simple and green H2O2-assisted etching method. The synergistic effect of the above three defects leads to the exposure of more active sites and significant improvement of the intrinsic activity. The optimized catalyst exhibits an excellent OER performance with an extraordinarily low overpotential of 170 mV at 10 mA·cm−2 and a small Tafel slope of 39.3 mV·dec−1 in 1 M KOH solution. Density functional theory calculations reveal this OER performance arises from pseudo re-oxidized metal-stable Ni3+ near oxygen vacancies (Ovac), which suppresses 3d-eg of Ni-site and elevates d-band center towards the competitively low electron-transfer barrier. This work provides a new insight to fabricate advanced electrocatalysts for renewable energy conversion technologies.


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Multiple structural defects in ultrathin NiFe-LDH nanosheets synergistically and remarkably boost water oxidation reaction

Show Author's information Zhongyin Zhao1,2Qi Shao1Jiangyan Xue1Bolong Huang3( )Zheng Niu1( )Hongwei Gu1Xiaoqing Huang1( )Jianping Lang1,2( )
College of Chemistry, Chemical Engineering and Materials Science Soochow UniversitySuzhou 215123 China
State Key Laboratory of Organometallic Chemistry, Shanghai Institute of Organic Chemistry Chinese Academy of SciencesShanghai 200032 China
Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic UniversityHung Hom, Kowloon, Hong Kong SAR China

Abstract

Modifying electrocatalysts nanostructures and tuning their electronic properties through defects-oriented synthetic strategies are essential to improve the oxygen evolution reaction (OER) performance of electrocatalysts. Current synthetic strategies about electrocatalysts mainly target the single or double structural defects, while the researches about the synergistic effect of multiple structural defects are rare. In this work, the ultrathin NiFe layered double hydroxide nanosheets with a holey structure, oxygen vacancies and Ni3+ defects on nickel foam (NiFe-LDH-NSs/NF) are prepared by employing a simple and green H2O2-assisted etching method. The synergistic effect of the above three defects leads to the exposure of more active sites and significant improvement of the intrinsic activity. The optimized catalyst exhibits an excellent OER performance with an extraordinarily low overpotential of 170 mV at 10 mA·cm−2 and a small Tafel slope of 39.3 mV·dec−1 in 1 M KOH solution. Density functional theory calculations reveal this OER performance arises from pseudo re-oxidized metal-stable Ni3+ near oxygen vacancies (Ovac), which suppresses 3d-eg of Ni-site and elevates d-band center towards the competitively low electron-transfer barrier. This work provides a new insight to fabricate advanced electrocatalysts for renewable energy conversion technologies.

Keywords: oxygen evolution reaction, layered double hydroxide, oxygen vacancies, holey structures, Ni3+ defects

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Acknowledgements

Publication history

Received: 04 January 2021
Revised: 24 February 2021
Accepted: 25 March 2021
Published: 03 June 2021
Issue date: January 2022

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

Acknowledgements

Acknowledgements

We thank financial supports from the National Natural Science Foundation of China (Nos. 21531006 and 21773163), the State Key Laboratory of Organometallic Chemistry of Shanghai Institute of Organic Chemistry (No. KF2021005), Collaborative Innovation Center of Suzhou Nano Science and Technology, the "Priority Academic Program Development" of Jiangsu Higher Education Institutions, and the Project of Scientific and Technologic Infrastructure of Suzhou (No. SZS201905). We are grateful to the editor and the reviewers for their useful comments and suggestions.

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