Modulation of d-orbital to realize enriched electronic cobalt sites in cobalt sulfide for enhanced hydrogen evolution in electrocatalytic water/seawater splitting

Jian-Peng Sun ¹Yu Zheng ²Zi-Sheng Zhang ³Xiang-Chao Meng ¹Zi-Zhen Li¹

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作者信息

1. Key Laboratory of Marine Chemistry Theory and Technology (Ministry of Education),College of Chemistry and Chemical Engineering,Ocean University of China,Qingdao 266100,China
2. Shanxi Institute of Energy,Taiyuan 030600,China
3. Department of Chemical and Biological Engineering,Faculty of Engineering,University of Ottawa,Ottawa,ON K1N6 N5,Canada
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Abstract

Herein,a novel single-atomic Pt doping and interface-rich CoS/Co(OH)2(Pt-CoS/Co(OH)2/C)electro-catalyst has been successfully prepared.Benefiting from precise regulation of d-orbital electronic structure modu-lation on Co site,Pt-CoS/Co(OH)2/C exhibited remarkable HER activity and high stability for hydrogen evolution in splitting both water(73 mV@10 mA.cm-2)and seawater(87 mV@10 mA.cm-2).Notably,atomic Pt doping was introduced into CoS/Co(OH)2,which could produce local unbalanced Coulombic force and significantly increased the number of S vacancies,and then expose abundant Co sites.Meantime,Co(OH)2 in Pt-CoS/Co(OH)2/C could act as the adsorption sites for H2O in hydrogen evolution reaction process.Density functional theory results also proved that atomic Pt doping,S vacancies and Co(OH)2 coupling could result in the formation of enriched elec-tronic Co sites and optimize dz2 orbital electronic structure,and then realize the depth upward shift of d-band center and enhance the adsorption of H*on Co sites.

Key words

Electrocatalysts/Hydrogen evolution reaction/Pt-CoS/Co(OH)2/d-band center/Electronic structure/Water/seawater electrolysis

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基金项目

山东省自然科学基金(ZR2021QB056)

Taishan Scholars Foundation of Shandong province(tsqn201909058)

Shiyanjia Lab()

出版年

2024

稀有金属(英文版)

中国有色金属学会

稀有金属(英文版)

CSTPCDEI

影响因子：0.801

ISSN：1001-0521

参考文献量47

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