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

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 Tang

doi:10.1038/s41560-020-00709-1

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

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 Tang

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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 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

Original language	English (US)
Journal	Nature Energy
DOIs	https://doi.org/10.1038/s41560-020-00709-1
State	Published - Oct 26 2020

Bibliographical note

KAUST Repository Item: Exported on 2020-11-02
Acknowledgements: We appreciate financial support from the Strategic Priority Research Program of Chinese Academy of Sciences (XDB36000000, Z.T.), the National Key Basic Research Program of China (2016YFA0200700, Z.T.), the National Natural Science Foundation of China (21890381 and 21721002, Z.T.; 11605225, J.D.), the Frontier Science Key Project of Chinese Academy of Sciences (QYZDJ-SSW-SLH038, Z.T.) and K.C. Wong Education Foundation (Z.T.). S.Z. acknowledges financial support from the FH Loxton fellowship of the USYD. J.D. acknowledges support from the Youth Innovation Promotion Association, CAS. C.-T.H. acknowledges support from the Young Elite Scientists Sponsorship Program by CAST. J.Z. thanks the National Key Research and Development Program of China (2017YFA0403400). We sincerely appreciate V. Yachandra and B. Lassalle providing the XAS data for Ni(OH)2 and NiOOH references. We thank R. Chen for help and suggestions.

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@article{111291a4d2d244adaccf85b84ee4d5a5,

title = "Structural transformation of highly active metal–organic framework electrocatalysts during the oxygen evolution reaction",

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",

author = "Shenlong Zhao and Chunhui Tan and Chun-Ting He and Pengfei An and Feng Xie and Shuai Jiang and Yanfei Zhu and Kuang-Hsu Wu and Binwei Zhang and Haijing Li and Jing Zhang and Yuan Chen and Shaoqin Liu and Juncai Dong and Zhiyong Tang",

note = "KAUST Repository Item: Exported on 2020-11-02 Acknowledgements: We appreciate financial support from the Strategic Priority Research Program of Chinese Academy of Sciences (XDB36000000, Z.T.), the National Key Basic Research Program of China (2016YFA0200700, Z.T.), the National Natural Science Foundation of China (21890381 and 21721002, Z.T.; 11605225, J.D.), the Frontier Science Key Project of Chinese Academy of Sciences (QYZDJ-SSW-SLH038, Z.T.) and K.C. Wong Education Foundation (Z.T.). S.Z. acknowledges financial support from the FH Loxton fellowship of the USYD. J.D. acknowledges support from the Youth Innovation Promotion Association, CAS. C.-T.H. acknowledges support from the Young Elite Scientists Sponsorship Program by CAST. J.Z. thanks the National Key Research and Development Program of China (2017YFA0403400). We sincerely appreciate V. Yachandra and B. Lassalle providing the XAS data for Ni(OH)2 and NiOOH references. We thank R. Chen for help and suggestions.",

year = "2020",

month = oct,

day = "26",

doi = "10.1038/s41560-020-00709-1",

language = "English (US)",

journal = "Nature Energy",

issn = "2058-7546",

publisher = "Nature Publishing Group",

}

TY - JOUR

T1 - Structural transformation of highly active metal–organic framework electrocatalysts during the oxygen evolution reaction

AU - Zhao, Shenlong

AU - Tan, Chunhui

AU - He, Chun-Ting

AU - An, Pengfei

AU - Xie, Feng

AU - Jiang, Shuai

AU - Zhu, Yanfei

AU - Wu, Kuang-Hsu

AU - Zhang, Binwei

AU - Li, Haijing

AU - Zhang, Jing

AU - Chen, Yuan

AU - Liu, Shaoqin

AU - Dong, Juncai

AU - Tang, Zhiyong

N1 - KAUST Repository Item: Exported on 2020-11-02 Acknowledgements: We appreciate financial support from the Strategic Priority Research Program of Chinese Academy of Sciences (XDB36000000, Z.T.), the National Key Basic Research Program of China (2016YFA0200700, Z.T.), the National Natural Science Foundation of China (21890381 and 21721002, Z.T.; 11605225, J.D.), the Frontier Science Key Project of Chinese Academy of Sciences (QYZDJ-SSW-SLH038, Z.T.) and K.C. Wong Education Foundation (Z.T.). S.Z. acknowledges financial support from the FH Loxton fellowship of the USYD. J.D. acknowledges support from the Youth Innovation Promotion Association, CAS. C.-T.H. acknowledges support from the Young Elite Scientists Sponsorship Program by CAST. J.Z. thanks the National Key Research and Development Program of China (2017YFA0403400). We sincerely appreciate V. Yachandra and B. Lassalle providing the XAS data for Ni(OH)2 and NiOOH references. We thank R. Chen for help and suggestions.

PY - 2020/10/26

Y1 - 2020/10/26

N2 - 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

AB - 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

UR - http://hdl.handle.net/10754/665735

UR - http://www.nature.com/articles/s41560-020-00709-1

U2 - 10.1038/s41560-020-00709-1

DO - 10.1038/s41560-020-00709-1

M3 - Article

SN - 2058-7546

JO - Nature Energy

JF - Nature Energy

ER -

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

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