Zhang Xin, Zhong Haoyin, Zhang Qi, Zhang Qihan, Wu Chao, Yu Junchen, Ma Yifan, An Hang, Wang Hao, Zou Yiming, Diao Caozheng, Chen Jingsheng, Yu Zhi Gen, Xi Shibo, Wang Xiaopeng, Xue Junmin
Department of Materials Science and Engineering, National University of Singapore, Singapore, 117575, Singapore.
Institute of Sustainability for Chemical, Energy and Environment (ISCE), Agency for Science, Technology and Research (A*STAR), Singapore, 627833, Singapore.
Nat Commun. 2024 Feb 15;15(1):1383. doi: 10.1038/s41467-024-45702-4.
Cobalt oxyhydroxide (CoOOH) is a promising catalytic material for oxygen evolution reaction (OER). In the traditional CoOOH structure, Co exhibits a low-spin state configuration ([Formula: see text]), with electron transfer occurring in face-to-face [Formula: see text] orbitals. In this work, we report the successful synthesis of high-spin state Co 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 [Formula: see text] 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, which is 148 mV lower than that of the low-spin state CoOOH. This work emphasizes the effect of the spin state of Co on OER activity of CoOOH based electrocatalysts for water splitting, and thus provides a new strategy for designing highly efficient electrocatalysts.
羟基氧化钴（CoOOH）是一种很有前景的析氧反应（OER）催化材料。在传统的CoOOH结构中，Co呈现低自旋态构型（[化学式：见原文]），电子转移发生在面对面的[化学式：见原文]轨道上。在这项工作中，我们报告了通过引入配位不饱和Co原子成功合成了高自旋态Co CoOOH结构。与低自旋态CoOOH相比，高自旋态CoOOH中的电子转移发生在顶点对顶点的[化学式：见原文]轨道上，其电子转移能力更快。结果，高自旋态CoOOH在10 mA cm时过电位为226 mV，表现出优异的OER活性，比低自旋态CoOOH低148 mV。这项工作强调了Co的自旋态对基于CoOOH的水电解电催化剂OER活性的影响，从而为设计高效电催化剂提供了一种新策略。
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