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

University of Science and Technology of China
Southern University of Science and Technology
Shandong University

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

160 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

Abstract

Keywords

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