High-spin Co3+ in cobalt oxyhydroxide for efficient water oxidation

Xin Zhang, Haoyin Zhong, Qi Zhang, Qihan Zhang, Chao Wu, Junchen Yu, Yifan Ma, Hang An, Hao Wang, Yiming Zou, Caozheng Diao, Jingsheng Chen, Zhi Gen Yu, Shibo Xi (), Xiaopeng Wang () and Junmin Xue ()
Additional contact information
Xin Zhang: National University of Singapore
Haoyin Zhong: National University of Singapore
Qi Zhang: National University of Singapore
Qihan Zhang: National University of Singapore
Chao Wu: Technology and Research (A*STAR)
Junchen Yu: National University of Singapore
Yifan Ma: National University of Singapore
Hang An: National University of Singapore
Hao Wang: National University of Singapore
Yiming Zou: Nanyang Technological University
Caozheng Diao: National University of Singapore
Jingsheng Chen: National University of Singapore
Zhi Gen Yu: Technology and Research (A*STAR)
Shibo Xi: Technology and Research (A*STAR)
Xiaopeng Wang: National University of Singapore
Junmin Xue: National University of Singapore

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Cobalt oxyhydroxide (CoOOH) is a promising catalytic material for oxygen evolution reaction (OER). In the traditional CoOOH structure, Co3+ exhibits a low-spin state configuration ( $${t}_{2{{{{{\rm{g}}}}}}}^{6}{e}_{{{{{{\rm{g}}}}}}}^{0}$$ t 2 g 6 e g 0 ), with electron transfer occurring in face-to-face $${t}_{2{{{{{\rm{g}}}}}}}^{*}$$ t 2 g * orbitals. In this work, we report the successful synthesis of high-spin state Co3+ CoOOH structure, by introducing coordinatively unsaturated Co atoms. As compared to the low-spin state CoOOH, electron transfer in the high-spin state CoOOH occurs in apex-to-apex $${e}_{{{{{{\rm{g}}}}}}}^{*}$$ e g * orbitals, which exhibits faster electron transfer ability. As a result, the high-spin state CoOOH performs superior OER activity with an overpotential of 226 mV at 10 mA cm−2, which is 148 mV lower than that of the low-spin state CoOOH. This work emphasizes the effect of the spin state of Co3+ on OER activity of CoOOH based electrocatalysts for water splitting, and thus provides a new strategy for designing highly efficient electrocatalysts.

Date: 2024
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DOI: 10.1038/s41467-024-45702-4

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