Spatiotemporally and Chemically Resolved Imaging of Electrocatalytic Oxygen Evolution on Single Nanoplates of Cobalt-Layered Hydroxide

Zhao, Xin1; Li, Yanyan1,2,3; Cui, Yu1; Saqib, Muhammad1; Zhang, Xinyu1,2,3; Hao, Rui1,4; Zheng, Zhiping1,2,3

2023-09-01

10.1021/jacs.3c06062

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY   影响因子和分区

0002-7863

1520-5126

Transition metal-layered hydroxides have been extensively studied in order to address the key challenge of slow kinetics of the oxygen evolution reaction (OER). However, how the catalytically active sites are evolved and the corresponding heterogeneous structure-property relationship remain unclear. Herein, using cobalt-layered hydroxide as a representative catalyst, we report a strategy for the comprehensive in situ investigation of the electrocatalytic OER process at the single electrocatalyst level using combined electrochemiluminescence (ECL) and visabsorption microscopy. The stepwise heterogeneous electrocatalytic responses of single-cobalt hydroxide nanoplates are unveiled with ECL imaging, and the corresponding valence state changes are revealed by vis-absorption imaging. The correlated in situ and ex situ multimode analyses indicate that, during the oxidation process, the Co2+ cations in the tetrahedral sites (Co-Td(2+)) turned into Co-Td(3+) and even the highly unstable Co-Td(4+), assisted by the interlayer water in a metastable CoOOH center dot xH(2)O phase. Crucially, the Co-Td(4+) sites are mainly distributed in the inner part of the nanoplates and show superior electrocatalytic properties. The correlative single-particle imaging approach for electrocatalytic process analysis with high spatiotemporal and chemical resolution enables in-depth mechanistic insights to be generated and, in turn, will benefit the rational design of electrocatalysts with enhanced performance.

SCI ; EI

英语

NI论文

第一 ; 通讯

National Natural Science Foundation of China["22074059","22150410330"] ; Shenzhen Nobel Prize Scientists Laboratory Project[C17783101] ; Guangdong Provincial Key Laboratory of Catalysis[2020B121201002] ; Guangdong Provincial Key Laboratory of Energy Materials for Electric Power[2018B030322001] ; SUSTech["Y01216127","Y01216227","Y01216142","Y01216242"] ; Postdoctorate Scientific Research Fund for staying (coming to) Shenzhen[K21217502]

Chemistry

Chemistry, Multidisciplinary

WOS:001068634500001

AMER CHEMICAL SOC

20234214921716

Electrocatalysts ; Image processing ; Nanostructures ; Oxygen ; Reaction kinetics ; Transition metals

Metallurgy and Metallography:531 ; Data Processing and Image Processing:723.2 ; Nanotechnology:761 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Solid State Physics:933

Web of Science

1.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China
2.Southern Univ Sci & Technol, Dept Chem, Guangdong Prov Key Lab Energy Mat Elect Power, Shenzhen 518055, Peoples R China
3.Southern Univ Sci & Technol, Key Lab Energy Convers & Storage Technol, Minist Educ, Shenzhen 518055, Peoples R China
4.Southern Univ Sci & Technol, Res Ctr Chem Biol & Om Anal, Shenzhen 518055, Peoples R China

Zhao, Xin,Li, Yanyan,Cui, Yu,et al. Spatiotemporally and Chemically Resolved Imaging of Electrocatalytic Oxygen Evolution on Single Nanoplates of Cobalt-Layered Hydroxide[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2023,145(38):20897-20906.

Zhao, Xin.,Li, Yanyan.,Cui, Yu.,Saqib, Muhammad.,Zhang, Xinyu.,...&Zheng, Zhiping.(2023).Spatiotemporally and Chemically Resolved Imaging of Electrocatalytic Oxygen Evolution on Single Nanoplates of Cobalt-Layered Hydroxide.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,145(38),20897-20906.

Zhao, Xin,et al."Spatiotemporally and Chemically Resolved Imaging of Electrocatalytic Oxygen Evolution on Single Nanoplates of Cobalt-Layered Hydroxide".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 145.38(2023):20897-20906.