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

被引:101
作者
Zhang, Xin [1 ]
Zhong, Haoyin [1 ]
Zhang, Qi [1 ]
Zhang, Qihan [1 ]
Wu, Chao [2 ,3 ]
Yu, Junchen [1 ]
Ma, Yifan [1 ]
An, Hang [1 ]
Wang, Hao [1 ]
Zou, Yiming [4 ]
Diao, Caozheng [5 ]
Chen, Jingsheng [1 ]
Yu, Zhi Gen [6 ]
Xi, Shibo [2 ]
Wang, Xiaopeng [1 ,3 ,7 ,8 ]
Xue, Junmin [1 ]
机构
[1] Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117575, Singapore
[2] ASTAR, Inst Sustainabil Chem Energy & Environm, Singapore 627833, Singapore
[3] Sichuan Univ, Coll Mat Sci & Engn, Chengdu 610065, Peoples R China
[4] Nanyang Technol Univ, Sch Mat Sci & Engn, Singapore 639798, Singapore
[5] Natl Univ Singapore, SSLS, Singapore 117603, Singapore
[6] ASTAR, IHPC, Singapore 138632, Singapore
[7] Sichuan Univ, State Key Lab Intelligent Construct & Hlth Operat, Chengdu 610065, Peoples R China
[8] Tefusen Semicond & Hydrogen Energy Technol Yunnan, Chengdu 663200, Wenshan Zhuang, Peoples R China
基金
新加坡国家研究基金会;
关键词
STATE; BULK;
D O I
10.1038/s41467-024-45702-4
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
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(2g)(6)e(g)(0)), with electron transfer occurring in face-to-face t(2g)(& lowast;) 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(g)(& lowast;) 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.
引用
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页数:10
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