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通过在Co(OH)纳米针阵列上引入S和FeOOH诱导分子间氧耦合用于工业水氧化

Inducing Intermolecular Oxygen Coupling by Introducing S and FeOOH on Co(OH) Nanoneedle Arrays for Industrial Water Oxidation.

作者信息

Zhang Yijie, Zhang Weiyi, Zhang Xiaowen, Gao Yuan, Zhao Qiang, Li Jinping, Liu Guang

机构信息

Shanxi Key Laboratory of Gas Energy Efficient and Clean Utilization, College of Chemical Engineering and Technology, Taiyuan University of Technology, Taiyuan, Shanxi, 030024, P. R. China.

Shanxi Research Institute of HuaiRou Laboratory, Taiyuan, Shanxi, 030031, P. R. China.

出版信息

Small. 2024 Nov;20(46):e2405080. doi: 10.1002/smll.202405080. Epub 2024 Jul 28.

Abstract

The design of electrocatalysts for oxygen evolution reaction (OER) remains a limitation of industrial hydrogen production by electrolysis of water. Excellent and stable OER catalysts can be developed by activating lattice oxygen and changing the reaction path. Herein, S and FeOOH on the Co(OH) nanoneedle arrays are introduced to construct a heterostructure (S-FeOOH/Co(OH)/NF) as a proof of concept. Theoretical calculations and experimental suggest that the Co-O-Fe motif formed at the heterogeneous interface with the introduction of FeOOH, inducing electron transfer from Co to Fe, enhancing Co─O covalency and reducing intramolecular charge transfer energy, thereby stimulating direct intramolecular lattice oxygen coupling. Doping of S in FeOOH further accelerates electron transfer, improves lattice oxygen activity, and prevents dissolution of FeOOH. Consequently, the overpotential of S-FeOOH/Co(OH)/NF is only 199 mV at 10 mA cm, and coupled with the Pt/C electrode can be up to 1 A cm under 1.79 V and remain stable for over 120 h in an anion exchange membrane water electrolyzer (AEMWE). This work proposes a strategy for the design of efficient and stable electrocatalysts for industrial water electrolysis and promotes the commercialization of AEMWE.

摘要

用于析氧反应(OER)的电催化剂设计仍然是水电解制氢工业化的一个限制因素。通过激活晶格氧和改变反应路径,可以开发出优异且稳定的OER催化剂。在此,将S和FeOOH引入到Co(OH)纳米针阵列上,构建异质结构(S-FeOOH/Co(OH)/NF)作为概念验证。理论计算和实验表明,引入FeOOH后在异质界面形成的Co-O-Fe基序,诱导电子从Co转移到Fe,增强了Co─O共价性并降低了分子内电荷转移能量,从而促进了分子内直接晶格氧耦合。在FeOOH中掺杂S进一步加速了电子转移,提高了晶格氧活性,并防止了FeOOH的溶解。因此,S-FeOOH/Co(OH)/NF在10 mA cm时的过电位仅为199 mV,与Pt/C电极耦合在1.79 V下可达1 A cm,并在阴离子交换膜水电解槽(AEMWE)中保持稳定超过120小时。这项工作提出了一种设计用于工业水电解的高效稳定电催化剂的策略,并推动了AEMWE的商业化。

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