Synergistic Modulation at Atomically Dispersed Fe/Au Interface for Selective CO2 Electroreduction

被引：52

作者：

Shen, Xinyi ^{[1
]}

Liu, Xiaokang ^{[1
]}

Wang, Sicong ^{[1
]}

Chen, Tao ^{[1
,2
]}

Zhang, Wei ^{[1
,4
]}

Cao, Linlin ^{[1
]}

Ding, Tao ^{[1
]}

Lin, Yue ^{[3
]}

Liu, Dong ^{[1
]}

Wang, Lan ^{[1
,2
]}

Zhang, Wei ^{[1
,4
]}

Yao, Tao ^{[1
]}

机构：

[1] Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Peoples R China

[2] Southwest Univ Sci & Technol, Sch Natl Def Sci & Technol, Mianyang 621010, Sichuan, Peoples R China

[3] Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Hefei 230029, Peoples R China

[4] Chinese Acad Sci, Chongqing Inst Green & Intelligent Technol, Chongqing 400714, Peoples R China

来源：

NANO LETTERS | 2021年 / 21卷 / 01期

基金：

中国国家自然科学基金;

关键词：

Synergistic strategy; CO2; electroreduction; Operando XAFS; Interfacial sites; Dynamic structures; CARBON-DIOXIDE; ACTIVE-SITES; AU; REDUCTION; CATALYSTS; NANOPARTICLES;

D O I：

10.1021/acs.nanolett.0c04291

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The electrocatalytic carbon dioxide reduction reaction (CO2RR) offers an attractive route to fuels and feedstocks from renewable energy. Gold is active for the electrochemical CO2RR to CO, while the competing hydrogen evolution reaction is unavoidable. Here, we report a synergistic strategy, via introducing atomically dispersed Fe to tune the electronic structure of the Au nanoparticle, to improve the CO selectivity. By using operando X-ray absorption and infrared spectroscopies, we reveal the dynamic structural evolution and the adsorption of reactant intermediates at the single-atom Fe-1/Au interface. During the reaction, the interaction between Fe and Au atoms becomes stronger, and the Fe-1/Au synergies affect the adsorption of reaction intermediates, thus improving the selectivity of CO up to 96.3% with a mass activity of 399 mA mg(-1). These results highlight the significant importance of synergistic modulation for advancing the single-atom decorated nanoparticle catalysis.

引用

页码：686 / 692

页数：7

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