Direct In Situ Raman Spectroscopic Evidence of Oxygen Reduction Reaction Intermediates at High-Index Pt(hkl) Surfaces

被引：225

作者：

Dong, Jin-Chao ^{[1
]}

Su, Min ^{[1
]}

Briega-Martos, Valentin ^{[2
]}

Li, Lang ^{[1
]}

Le, Jia-Bo ^{[1
]}

Radjenovic, Petar ^{[1
]}

Zhou, Xiao-Shun ^{[3
]}

Feliu, Juan Miguel ^{[2
]}

Tian, Zhong-Qun ^{[1
]}

Li, Jian-Feng ^{[1
]}

机构：

[1] Xiamen Univ, Coll Energy, Coll Chem & Chem Engn, State Key Lab Phys Chem Solid Surfaces,iChEM, Xiamen 361005, Peoples R China

[2] Univ Alicante, Inst Electroquim, E-03080 Alicante, Spain

[3] Zhejiang Normal Univ, Coll Chem & Life Sci, Minist Educ Adv Catalysis Mat, Key Lab, Jinhua 321004, Zhejiang, Peoples R China

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2020年 / 142卷 / 02期

基金：

中国博士后科学基金; 中国国家自然科学基金;

关键词：

PLATINUM STEPPED SURFACES; SINGLE-CRYSTAL SURFACES; APPARENT PH-DEPENDENCE; ELECTROCHEMICAL OXIDATION; ADSORPTION; HYDROGEN; NANOCRYSTALS; KINETICS; METHANOL; CATIONS;

D O I：

10.1021/jacs.9b12803

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The study of the oxygen reduction reaction (ORR) at high-index Pt(hkl) single crystal surfaces has received considerable interest due to their well-ordered, typical atomic structures and superior catalytic activities. However, it is difficult to obtain direct spectral evidence of ORR intermediates during reaction processes, especially at high-index Pt(hkl) surfaces. Herein, in situ Raman spectroscopy has been employed to investigate ORR processes at high-index Pt(hkl) surfaces containing the [01 (1) over bar] crystal zone-i.e., Pt(211) and Pt(311). Through control and isotope substitution experiments, in situ spectroscopic evidence of OH and OOH intermediates at Pt(211) and Pt(311) surfaces was successfully obtained. After detailed analysis based on the Raman spectra and theoretical simulation, it was deduced that the difference in adsorption of OOH at high-index surfaces has a significant effect on the ORR activity. This research illuminates and deepens the understanding of the ORR mechanism on high-index Pt(hkl) surfaces and provides theoretical guidance for the rational design of high activity ORR catalysts.

引用

页码：715 / 719

页数：5

共 34 条

[1] New understanding of the nature of OH adsorption on Pt(111) electrodes [J].