N-Coordinated Dual-Metal Single-Site Catalyst for Low-Temperature CO Oxidation

Wang, Jing1; You, Rui2; Zhao, Chao1; Zhang, Wei3; Liu, Wei4; Fu, Xin-Pu5; Li, Yangyang2; Zhou, Fangyao1; Zheng, Xusheng4; Xu, Qian4; Yao, Tao4; Jia, Chun-Jiang5; Wang, Yang-Gang3; Huang, Weixin2; Wu, Yuen1

2020

10.1021/acscatal.0c00097

ACS Catalysis   影响因子和分区

21555435

Catalysts for CO oxidation reaction are mainly based on oxide/hydroxide materials with multicomponent active sites. Here, we report a nonoxide/hydroxide material, atomically dispersed dual-metal single sites (Fe-Co sites) on N-doped carbon support, as a highly active catalyst for CO oxidation. It can greatly lower the temperature for complete CO conversion as low as -73 °C with a turnover frequency of 0.096 s^-1. X-ray absorption near-edge structure spectra, pulse-adsorption microcalorimetry, and density functional theory studies show that the Fe-Co sites synergistically catalyze CO oxidation facilely following the Langmuir-Hinshelwood (L-H) mechanism with CO preferentially adsorbing at the Co sites and O2 adsorbing at the Fe sites. These results, for the first time, reveal that the dual-metal single site on N-doped carbon can efficiency catalyze low-temperature CO oxidation reaction without the involvement of supports, such as oxygen vacancies and surface hydroxyl groups.
Copyright © 2020 American Chemical Society.

dual-metal active site N-doped carbon CO pulse-adsorption microcalorimetry low-temperature CO oxidation Langmuir-Hinshelwood mechanism

SCI ; EI

英语

通讯

[0700100] ; National Natural Science Foundation of China[21521091] ; Fundamental Research Funds for the Central Universities[]

Chemistry

Chemistry, Physical

WOS:000516887400038

American Chemical Society

20201108276266

Binary alloys ; Calorimeters ; Carbon ; Catalyst activity ; Density functional theory ; Doping (additives) ; Metals ; Oxidation ; X ray absorption ; X ray absorption near edge structure spectroscopy

Thermodynamics:641.1 ; Electromagnetic Waves:711 ; Chemical Reactions:802.2 ; Chemical Products Generally:804 ; Atomic and Molecular Physics:931.3 ; Temperature Measuring Instruments:944.5

Web of Science

1.Hefei National Laboratory for Physical Sciences at the Microscale, Department of Applied Chemistry, IChEM (Collaborative Innovation Center of Chemistry for Energy Materials), University of Science and Technology of China, Hefei; 230026, China
2.Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, Key Lab. of Surf. and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, University of Science and Technology of China, Hefei; 230026, China
3.Department of Chemistry, Southern University of Science and Technology, Shenzhen; 518055, China
4.National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei; 230026, China
5.Key Laboratory for Colloid and Interface Chemistry, Key Laboratory of Special Aggregated Materials, School of Chemistry and Chemical Engineering, Shandong University, Jinan; 250100, China

Wang, Jing,You, Rui,Zhao, Chao,et al. N-Coordinated Dual-Metal Single-Site Catalyst for Low-Temperature CO Oxidation[J]. ACS Catalysis,2020,10(4):2754-2761.

Wang, Jing.,You, Rui.,Zhao, Chao.,Zhang, Wei.,Liu, Wei.,...&Wu, Yuen.(2020).N-Coordinated Dual-Metal Single-Site Catalyst for Low-Temperature CO Oxidation.ACS Catalysis,10(4),2754-2761.

Wang, Jing,et al."N-Coordinated Dual-Metal Single-Site Catalyst for Low-Temperature CO Oxidation".ACS Catalysis 10.4(2020):2754-2761.