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掺杂铬以调节铜和钴的价态有助于高效水分解。

Doping of Cr to Regulate the Valence State of Cu and Co Contributes to Efficient Water Splitting.

作者信息

Mu Xiaoming, Wang Kai, Lv Keyi, Feng Bo, Yu Xiaofei, Li Lanlan, Zhang Xinghua, Yang Xiaojing, Lu Zunming

机构信息

School of Materials Science and Engineering, Hebei University of Technology, Tianjin 300130, PR China.

出版信息

ACS Appl Mater Interfaces. 2023 Apr 5;15(13):16552-16561. doi: 10.1021/acsami.2c18799. Epub 2023 Mar 24.

Abstract

Water electrolysis in alkaline media is the most promising technology for hydrogen production, but efficient electrocatalysts are required to reduce the overpotential in HER and OER processes. In this work, the multicomponent transition metal catalyst Cr-Cu/CoO was loaded on copper foam by electrodeposition and annealing, and the catalyst exhibited excellent electrochemical activity. The HER overpotential is 21 mV and the OER overpotential is 252 mV at a current density of 10 mA cm. The overall water splitting voltage is 1.51 V, even better than the Pt/C//RuO two-electrode system (1.61 V). The excellent performance of this catalyst is mainly derived from the close synergistic interaction among Cu, Co, and Cr. The doping of Cr modulates the valence states of Cu and Co at the active sites and improves the adsorption of various reaction intermediates. Density functional theory (DFT) calculations show that the doping of Cr can optimize the adsorption of the reaction intermediate H*. Meanwhile, the high-valent Cr and Co promote hydrolysis through strong adsorption with OH. The present work provides a reasonable strategy for designing low-cost transition metals as efficient catalysts for water electrolysis.

摘要

碱性介质中的水电解是最具前景的制氢技术,但需要高效的电催化剂来降低析氢反应(HER)和析氧反应(OER)过程中的过电位。在这项工作中,通过电沉积和退火将多组分过渡金属催化剂Cr-Cu/CoO负载在泡沫铜上,该催化剂表现出优异的电化学活性。在电流密度为10 mA cm时,HER过电位为21 mV,OER过电位为252 mV。整体水分解电压为1.51 V,甚至优于Pt/C//RuO双电极体系(1.61 V)。该催化剂的优异性能主要源于Cu、Co和Cr之间紧密的协同相互作用。Cr的掺杂调节了活性位点处Cu和Co的价态,提高了各种反应中间体的吸附。密度泛函理论(DFT)计算表明,Cr的掺杂可以优化反应中间体H*的吸附。同时,高价态的Cr和Co通过与OH的强吸附促进水解。本工作为设计低成本过渡金属作为水电解的高效催化剂提供了合理策略。

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