In-situ ECSTM investigation of H2O2 production in cobalt- porphyrin-catalyzed oxygen reduction reaction

被引：10

作者：

Feng, Ya-Chen ^{[1
,2
]}

Wang, Xiang ^{[1
]}

Yi, Zhen-Yu ^{[1
,2
]}

Wang, Yu-Qi ^{[1
,2
]}

Yan, Hui-Juan ^{[1
,2
]}

Wang, Dong ^{[1
,2
]}

机构：

[1] Chinese Acad Sci, CAS Res Educ Ctr Excellence Mol Sci, CAS Key Lab Mol Nanostruct & Nanotechnol, Beijing Natl Lab Mol Sci BNLMS,Inst Chem, Beijing 100190, Peoples R China

[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China

来源：

SCIENCE CHINA-CHEMISTRY | 2023年 / 66卷 / 01期

基金：

国家重点研发计划; 中国国家自然科学基金;

关键词：

electrochemical scanning tunnelling microscopy; H2O2; production; cobalt-porphyrin; oxygen reduction reaction; SCANNING-TUNNELING-MICROSCOPY; IRON-PHTHALOCYANINE; HYDROGEN-PEROXIDE; AU(111); O-2; MOLECULE; SURFACE; ELECTROCATALYST; IDENTIFICATION; KINETICS;

D O I：

10.1007/s11426-022-1465-8

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

We report the in-situ investigation of the production of H2O2 in 5,10,15,20-tetra(4-methoxyphenyl)-21H,23H-porphyrin cobalt(II) (CoTMPP)-catalyzed oxygen reduction reaction (ORR) in neutral electrolytes by electrochemical scanning tunneling microscopy (ECSTM) at the molecular scale. The adsorption of 00H on active sites can be observed in STM images and is found to be correlated with the pH value of the electrolyte. The thermodynamic parameters of the formation of CoTMPP-OOH- complex are extracted by the quantitative analysis of the STM images. Two stages of the ORR including the formation of H2O2 and further reduction of H2O2 at different reduction potentials can be revealed by electrochemical measurements. In-situ ECSTM experiments unambiguously identify the formation of the CoTMPP-OOH- complex as the high contrast species and its reduction and oxidation process. This work provides the direct evidence for understanding the formation and transformation process of H2O2 at the molecular scale, which benefits the rational design of the high-efficiency electrocatalysts for ORR and H2O2 production.

引用

页码：273 / 278

页数：6

共 44 条

[1] Oxygen reduction reaction in acid medium at iron phthalocyanine dispersed on high surface area carbon substrate:: tolerance to methanol, stability and kinetics [J].