Structural transformation of highly active metal–organic framework electrocatalysts during the oxygen evolution reaction
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...
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| Published in | Nature energy Vol. 5; no. 11; pp. 881 - 890 |
|---|---|
| Main Authors | , , , , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
London
Nature Publishing Group UK
01.11.2020
Nature Publishing Group |
| Subjects | |
| Online Access | Get full text |
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| 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 Ni
0.5
Co
0.5
-MOF-74 during the OER by operando X-ray absorption spectroscopy analysis and high-resolution transmission electron microscopy imaging. We suggest that Ni
0.5
Co
0.5
OOH
0.75
, 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 Ni
0.9
Fe
0.1
-MOF that delivers low overpotentials of 198 mV and 231 mV at 10 mA cm
−2
and 20 mA cm
−2
, respectively.
Metal–organic frameworks (MOFs) are increasingly being explored for electrocatalytic oxygen evolution, which is half of the water splitting reaction. Here the authors show that, under reaction conditions, mixed metal oxyhydroxides form at the nodes of bimetallic MOFs, which are highly catalytically active. |
|---|---|
| AbstractList | 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.Metal–organic frameworks (MOFs) are increasingly being explored for electrocatalytic oxygen evolution, which is half of the water splitting reaction. Here the authors show that, under reaction conditions, mixed metal oxyhydroxides form at the nodes of bimetallic MOFs, which are highly catalytically active. 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 Ni 0.5 Co 0.5 -MOF-74 during the OER by operando X-ray absorption spectroscopy analysis and high-resolution transmission electron microscopy imaging. We suggest that Ni 0.5 Co 0.5 OOH 0.75 , 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 Ni 0.9 Fe 0.1 -MOF that delivers low overpotentials of 198 mV and 231 mV at 10 mA cm −2 and 20 mA cm −2 , respectively. Metal–organic frameworks (MOFs) are increasingly being explored for electrocatalytic oxygen evolution, which is half of the water splitting reaction. Here the authors show that, under reaction conditions, mixed metal oxyhydroxides form at the nodes of bimetallic MOFs, which are highly catalytically active. |
| Author | Tang, Zhiyong Zhang, Binwei Wu, Kuang-Hsu Chen, Yuan An, Pengfei Liu, Shaoqin He, Chun-Ting Tan, Chunhui Xie, Feng Zhang, Jing Jiang, Shuai Dong, Juncai Zhao, Shenlong Zhu, Yanfei Li, Haijing |
| Author_xml | – sequence: 1 givenname: Shenlong surname: Zhao fullname: Zhao, Shenlong organization: CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, School of Chemical and Biomolecular Engineering, The University of Sydney – sequence: 2 givenname: Chunhui surname: Tan fullname: Tan, Chunhui organization: Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology – sequence: 3 givenname: Chun-Ting surname: He fullname: He, Chun-Ting organization: Key Laboratory of Functional Small Organic Molecule, Ministry of Education, College of Chemistry and Chemical Engineering, Jiangxi Normal University – sequence: 4 givenname: Pengfei surname: An fullname: An, Pengfei organization: Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences – sequence: 5 givenname: Feng surname: Xie fullname: Xie, Feng organization: Advanced Membranes and Porous Materials Center, Physical Sciences and Engineering Division, King Abdullah University of Science and Technology – sequence: 6 givenname: Shuai surname: Jiang fullname: Jiang, Shuai organization: CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology – sequence: 7 givenname: Yanfei surname: Zhu fullname: Zhu, Yanfei organization: CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology – sequence: 8 givenname: Kuang-Hsu surname: Wu fullname: Wu, Kuang-Hsu organization: School of Chemical and Biomolecular Engineering, The University of Sydney – sequence: 9 givenname: Binwei orcidid: 0000-0002-7023-5986 surname: Zhang fullname: Zhang, Binwei organization: School of Chemical and Biomolecular Engineering, The University of Sydney – sequence: 10 givenname: Haijing surname: Li fullname: Li, Haijing organization: Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences – sequence: 11 givenname: Jing surname: Zhang fullname: Zhang, Jing organization: Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences – sequence: 12 givenname: Yuan orcidid: 0000-0001-9059-3839 surname: Chen fullname: Chen, Yuan organization: School of Chemical and Biomolecular Engineering, The University of Sydney – sequence: 13 givenname: Shaoqin surname: Liu fullname: Liu, Shaoqin email: shaoqinliu@hit.edu.cn organization: State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology – sequence: 14 givenname: Juncai orcidid: 0000-0001-8860-093X surname: Dong fullname: Dong, Juncai email: dongjc@ihep.ac.cn organization: Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences – sequence: 15 givenname: Zhiyong orcidid: 0000-0003-0610-0064 surname: Tang fullname: Tang, Zhiyong email: zytang@nanoctr.cn organization: CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology |
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| Snippet | Metal–organic frameworks (MOFs) are increasingly being investigated as electrocatalysts for the oxygen evolution reaction (OER). Despite their promising... |
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| Title | Structural transformation of highly active metal–organic framework electrocatalysts during the oxygen evolution reaction |
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