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Structural transformation of highly active metal–organic framework electrocatalysts during the oxygen evolution reaction

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  • Shenlong Zhao

    (CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology
    The University of Sydney)

  • Chunhui Tan

    (Institute of High Energy Physics, Chinese Academy of Sciences
    Harbin Institute of Technology)

  • Chun-Ting He

    (Jiangxi Normal University)

  • Pengfei An

    (Institute of High Energy Physics, Chinese Academy of Sciences)

  • Feng Xie

    (King Abdullah University of Science and Technology)

  • Shuai Jiang

    (CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology)

  • Yanfei Zhu

    (CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology)

  • Kuang-Hsu Wu

    (The University of Sydney)

  • Binwei Zhang

    (The University of Sydney)

  • Haijing Li

    (Institute of High Energy Physics, Chinese Academy of Sciences)

  • Jing Zhang

    (Institute of High Energy Physics, Chinese Academy of Sciences)

  • Yuan Chen

    (The University of Sydney)

  • Shaoqin Liu

    (Harbin Institute of Technology)

  • Juncai Dong

    (Institute of High Energy Physics, Chinese Academy of Sciences)

  • Zhiyong Tang

    (CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology)

Abstract

Metal–organic frameworks (MOFs) are increasingly being investigated as electrocatalysts for the oxygen evolution reaction (OER). Despite their promising catalytic activity, many fundamental questions concerning their structure−performance relationships—especially those regarding the roles of active species—remain to be answered. Here we show the structural transformation of a Ni0.5Co0.5-MOF-74 during the OER by operando X-ray absorption spectroscopy analysis and high-resolution transmission electron microscopy imaging. We suggest that Ni0.5Co0.5OOH0.75, with abundant oxygen vacancies and high oxidation states, forms in situ and is responsible for the high OER activity observed. The ratio of Ni to Co in the bimetallic centres alters the geometric and electronic structure of as-formed active species and in turn the catalytic activity. Based on our understanding of this system, we fabricate a Ni0.9Fe0.1-MOF that delivers low overpotentials of 198 mV and 231 mV at 10 mA cm−2 and 20 mA cm−2, respectively.

Suggested Citation

  • Shenlong Zhao & Chunhui Tan & Chun-Ting He & Pengfei An & Feng Xie & Shuai Jiang & Yanfei Zhu & Kuang-Hsu Wu & Binwei Zhang & Haijing Li & Jing Zhang & Yuan Chen & Shaoqin Liu & Juncai Dong & Zhiyong , 2020. "Structural transformation of highly active metal–organic framework electrocatalysts during the oxygen evolution reaction," Nature Energy, Nature, vol. 5(11), pages 881-890, November.
    • Handle: RePEc:nat:natene:v:5:y:2020:i:11:d:10.1038_s41560-020-00709-1
    DOI: 10.1038/s41560-020-00709-1
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    Citations

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    Cited by:

    1. Zilong Wu & Xiangyu Liu & Haijing Li & Zhiyi Sun & Maosheng Cao & Zezhou Li & Chaohe Fang & Jihan Zhou & Chuanbao Cao & Juncai Dong & Shenlong Zhao & Zhuo Chen, 2023. "A semiconductor-electrocatalyst nano interface constructed for successive photoelectrochemical water oxidation," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    2. Daying Zheng & Kaijie Liu & Zeshu Zhang & Qi Fu & Mengyao Bian & Xinyu Han & Xin Shen & Xiaohui Chen & Haijiao Xie & Xiao Wang & Xiangguang Yang & Yibo Zhang & Shuyan Song, 2024. "Essential features of weak current for excellent enhancement of NOx reduction over monoatomic V-based catalyst," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    3. Zuyun He & Jun Zhang & Zhiheng Gong & Hang Lei & Deng Zhou & Nian Zhang & Wenjie Mai & Shijun Zhao & Yan Chen, 2022. "Activating lattice oxygen in NiFe-based (oxy)hydroxide for water electrolysis," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    4. Xingkun Wang & Liangliang Xu & Cheng Li & Canhui Zhang & Hanxu Yao & Ren Xu & Peixin Cui & Xusheng Zheng & Meng Gu & Jinwoo Lee & Heqing Jiang & Minghua Huang, 2023. "Developing a class of dual atom materials for multifunctional catalytic reactions," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    5. Xiang Liu & Yu-Quan Zhu & Jing Li & Ye Wang & Qiujin Shi & An-Zhen Li & Kaiyue Ji & Xi Wang & Xikang Zhao & Jinyu Zheng & Haohong Duan, 2024. "Electrosynthesis of adipic acid with high faradaic efficiency within a wide potential window," Nature Communications, Nature, vol. 15(1), pages 1-16, December.
    6. Yingying Zou & Chao Liu & Chaoqi Zhang & Ling Yuan & Jiaxin Li & Tong Bao & Guangfeng Wei & Jin Zou & Chengzhong Yu, 2023. "Epitaxial growth of metal-organic framework nanosheets into single-crystalline orthogonal arrays," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    7. Zheao Huang & Zhouzhou Wang & Hannah Rabl & Shaghayegh Naghdi & Qiancheng Zhou & Sabine Schwarz & Dogukan Hazar Apaydin & Ying Yu & Dominik Eder, 2024. "Ligand engineering enhances (photo) electrocatalytic activity and stability of zeolitic imidazolate frameworks via in-situ surface reconstruction," Nature Communications, Nature, vol. 15(1), pages 1-14, December.

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