Electronic metal-support interaction modulates single-atom platinum catalysis for hydrogen evolution reaction

被引：684

作者：

Shi, Yi ^{[1
]}

Ma, Zhi-Rui ^{[1
]}

Xiao, Yi-Ying ^{[1
]}

Yin, Yun-Chao ^{[2
]}

Huang, Wen-Mao ^{[3
]}

Huang, Zhi-Chao ^{[3
]}

Zheng, Yun-Zhe ^{[4
]}

Mu, Fang-Ya ^{[5
]}

Huang, Rong ^{[4
]}

Shi, Guo-Yue ^{[5
]}

Sun, Yi-Yang ^{[6
]}

Xia, Xing-Hua ^{[2
]}

Chen, Wei ^{[1
,3
,7
]}

机构：

[1] Natl Univ Singapore, Dept Chem, Singapore, Singapore

[2] Nanjing Univ, Sch Chem & Chem Engn, State Key Lab Analyt Chem Life Sci, Nanjing, Peoples R China

[3] Natl Univ Singapore, Dept Phys, Singapore, Singapore

[4] East China Normal Univ, Dept Elect, Key Lab Polar Mat & Devices MOE, Shanghai, Peoples R China

[5] East China Normal Univ, Sch Chem & Mol Engn, Shanghai, Peoples R China

[6] Chinese Acad Sci, Shanghai Inst Ceram, State Key Lab High Performance Ceram & Superfine, Shanghai, Peoples R China

[7] Tianjin Univ, Joint Sch Natl Univ Singapore & Tianjin Univ, Int Campus, Fuzhou, Peoples R China

来源：

NATURE COMMUNICATIONS | 2021年 / 12卷 / 01期

基金：

新加坡国家研究基金会; 中国国家自然科学基金;

关键词：

WATER; MOS2; ELECTROCATALYSIS; SURFACE; PHOTOELECTRON; SPECTROSCOPY; CHEMISTRY; DESIGN;

D O I：

10.1038/s41467-021-23306-6

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

Tuning metal-support interaction has been considered as an effective approach to modulate the electronic structure and catalytic activity of supported metal catalysts. At the atomic level, the understanding of the structure-activity relationship still remains obscure in heterogeneous catalysis, such as the conversion of water (alkaline) or hydronium ions (acid) to hydrogen (hydrogen evolution reaction, HER). Here, we reveal that the fine control over the oxidation states of single-atom Pt catalysts through electronic metal-support interaction significantly modulates the catalytic activities in either acidic or alkaline HER. Combined with detailed spectroscopic and electrochemical characterizations, the structure-activity relationship is established by correlating the acidic/alkaline HER activity with the average oxidation state of single-atom Pt and the Pt-H/Pt-OH interaction. This study sheds light on the atomic-level mechanistic understanding of acidic and alkaline HER, and further provides guidelines for the rational design of high-performance single-atom catalysts. Insights into the rational design of single-atom metal catalysts remains obscure in heterogeneous catalysis. Here, the authors establish the atomic-level structure-activity relationship for a wide-pH-range hydrogen evolution reaction through the electronic metal-support interaction modulation.

引用

页数：11

共 62 条

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