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通过配体调节活性位点以促进电催化析氧反应

Ligand Modulation of Active Sites to Promote Electrocatalytic Oxygen Evolution.

作者信息

Huang Wenzhong, Li Jiantao, Liao Xiaobin, Lu Ruihu, Ling Chaohong, Liu Xiong, Meng Jiashen, Qu Longbing, Lin Mengting, Hong Xufeng, Zhou Xunbiao, Liu Shanlin, Zhao Yan, Zhou Liang, Mai Liqiang

机构信息

State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan, Hubei, 430070, China.

State Key Laboratory of Silicate Materials for Architectures International School of Materials Science and Engineering, Wuhan University of Technology, Wuhan, Hubei, 430070, China.

出版信息

Adv Mater. 2022 May;34(18):e2200270. doi: 10.1002/adma.202200270. Epub 2022 Apr 4.

Abstract

Rationally designed catalysts hold the key to address the sluggish kinetics of oxygen evolution reaction (OER). However, engineering the active sites of such catalysts still faces grand challenges. This study proposes a feasible ligand modulation strategy to boost the OER catalytic activity of cobalt-iron oxyhydroxide ((Fe,Co)OOH). The 2-methylimidazole (MI) ligand coordination on (Fe,Co)OOH reduces the orbital overlap between the Fe/Co 3d and O 2p, which weakens the adsorption to oxygen-containing intermediates and thus facilitates the unfavorable O desorption. As a result, the MI ligand modulated (Fe,Co)OOH achieves an excellent OER performance with low overpotentials (230/290 mV at 10/100 mA cm ) and excellent durability (>155 h). This study provides a novel ligand modulation strategy for the design of OER catalysts.

摘要

合理设计的催化剂是解决析氧反应(OER)缓慢动力学问题的关键。然而,设计此类催化剂的活性位点仍面临巨大挑战。本研究提出了一种可行的配体调控策略,以提高氢氧化钴铁((Fe,Co)OOH)的OER催化活性。(Fe,Co)OOH上的2-甲基咪唑(MI)配体配位减少了Fe/Co 3d和O 2p之间的轨道重叠,削弱了对含氧中间体的吸附,从而促进了不利的O脱附。结果,MI配体调控的(Fe,Co)OOH在低过电位(10/100 mA cm²时为230/290 mV)下实现了优异的OER性能和出色的耐久性(>155小时)。本研究为OER催化剂的设计提供了一种新颖的配体调控策略。

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