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

Jing Wang; Rui You; Chao Zhao; Wei Zhang; Wei Liu; Xin Pu Fu; Yangyang Li; Fangyao Zhou; Xusheng Zheng; Qian Xu; Tao Yao; Chun Jiang Jia; Yang Gang Wang; Weixin Huang; Yuen Wu

doi:10.1021/acscatal.0c00097

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

Jing Wang, Rui You, Chao Zhao, Wei Zhang, Wei Liu, Xin Pu Fu, Yangyang Li, Fangyao Zhou, Xusheng Zheng, Qian Xu, Tao Yao, Chun Jiang Jia, Yang Gang Wang^*, Weixin Huang, Yuen Wu

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

148 Citations (Scopus)

Abstract

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.

Original language	English
Pages (from-to)	2754-2761
Number of pages	8
Journal	ACS Catalysis
Volume	10
Issue number	4
DOIs	https://doi.org/10.1021/acscatal.0c00097
Publication status	Published - 21 Feb 2020
Externally published	Yes

Keywords

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

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10.1021/acscatal.0c00097

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@article{00e2db04986d4217a19b83005f6d4080,

title = "N-Coordinated Dual-Metal Single-Site Catalyst for Low-Temperature CO Oxidation",

abstract = "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.",

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

author = "Jing Wang and Rui You and Chao Zhao and Wei Zhang and Wei Liu and Fu, \{Xin Pu\} and Yangyang Li and Fangyao Zhou and Xusheng Zheng and Qian Xu and Tao Yao and Jia, \{Chun Jiang\} and Wang, \{Yang Gang\} and Weixin Huang and Yuen Wu",

note = "Publisher Copyright: Copyright {\textcopyright} 2020 American Chemical Society.",

year = "2020",

month = feb,

day = "21",

doi = "10.1021/acscatal.0c00097",

language = "English",

volume = "10",

pages = "2754--2761",

journal = "ACS Catalysis",

issn = "2155-5435",

publisher = "American Chemical Society",

number = "4",

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TY - JOUR

T1 - N-Coordinated Dual-Metal Single-Site Catalyst for Low-Temperature CO Oxidation

AU - Wang, Jing

AU - You, Rui

AU - Zhao, Chao

AU - Zhang, Wei

AU - Liu, Wei

AU - Fu, Xin Pu

AU - Li, Yangyang

AU - Zhou, Fangyao

AU - Zheng, Xusheng

AU - Xu, Qian

AU - Yao, Tao

AU - Jia, Chun Jiang

AU - Wang, Yang Gang

AU - Huang, Weixin

AU - Wu, Yuen

PY - 2020/2/21

Y1 - 2020/2/21

N2 - 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.

AB - 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.

KW - CO pulse-adsorption microcalorimetry

KW - Langmuir-Hinshelwood mechanism

KW - N-doped carbon

KW - dual-metal active site

KW - low-temperature CO oxidation

UR - https://www.scopus.com/pages/publications/85080980329

U2 - 10.1021/acscatal.0c00097

DO - 10.1021/acscatal.0c00097

M3 - Article

AN - SCOPUS:85080980329

SN - 2155-5435

VL - 10

SP - 2754

EP - 2761

JO - ACS Catalysis

JF - ACS Catalysis

IS - 4

ER -

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

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Keywords

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