Understanding the Atomic and Defective Interface Effect on Ruthenium Clusters for the Hydrogen Evolution Reaction

被引：95

作者：

Gao, Taotao ^{[1
]}

Tang, Xiangmin ^{[2
]}

Li, Xiaoqin ^{[1
]}

Wu, Shuaiwei ^{[2
]}

Yu, Shumin ^{[2
]}

Li, Panpan ^{[3
]}

Xiao, Dan ^{[1
,4
]}

Jin, Zhaoyu ^{[5
]}

机构：

[1] Chengdu Univ, Inst Adv Study, Chengdu 610106, Peoples R China

[2] Chengdu Univ, Sch Mech Engn, Chengdu 610106, Peoples R China

[3] Sichuan Univ, Coll Mat Sci & Engn, Chengdu 610065, Peoples R China

[4] Sichuan Univ, Coll Chem Engn, Chengdu 610065, Peoples R China

[5] Univ Elect Sci & Technol China, Inst Fundamental & Frontier Sci, Chengdu 610054, Peoples R China

来源：

ACS CATALYSIS | 2023年 / 13卷 / 01期

关键词：

electrocatalysis; single-atomic site; substrate effect; vacancy defect; hydrogen evolution reaction; DENSITY-FUNCTIONAL THEORY; UNDERPOTENTIAL DEPOSITION; OXYGEN; ENERGY; ELECTROCATALYSTS; NANOPARTICLES; EFFICIENT; CATALYST;

D O I：

10.1021/acscatal.2c04586

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Water electrolysis powered by renewable electric energy is a promising technology for green hydrogen production without carbon emissions, while highly efficient and cost-effective electrocatalysts with long durability are urgently needed. Here, we demonstrate oxygen-coordinated single-atom iron sites (Fe-O-4) decorated carbon nanotubes with abundant vacancies as the substrate for stabilizing Ru clusters (CNT-V-Fe-Ru). The catalyst shows high performance for the hydrogen evolution reaction (HER) in both acidic and alkaline media, respectively. The HER kinetics analysis demonstrates that the defective substrate with single-atomic sites could significantly improve the intrinsic activity of Ru species. Theoretical calculations also support the superior HER behavior of CNT-V-Fe-Ru with fundamental insights into metal-substrate interactions. The present study highlights a unique feature of single-atom catalysts for serving as advanced supporting materials, which offers tremendous opportunities to adequately regulate electronic structures of metal-substrate interfaces at the atomic level.

引用

页码：49 / 59

页数：11

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