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Title: Atomic-layered Au clusters on α-MoC as catalysts for the low-temperature water-gas shift reaction

Here, the water-gas shift (WGS) reaction (where carbon monoxide plus water yields dihydrogen and carbon dioxide) is an essential process for hydrogen generation and carbon monoxide removal in various energy-related chemical operations. This equilibrium-limited reaction is favored at a low working temperature. Potential application in fuel cells also requires a WGS catalyst to be highly active, stable, and energy-efficient and to match the working temperature of on-site hydrogen generation and consumption units. We synthesized layered gold (Au) clusters on a molybdenum carbide (α-MoC) substrate to create an interfacial catalyst system for the ultralow-temperature WGS reaction. Water was activated over α-MoC at 303 kelvin, whereas carbon monoxide adsorbed on adjacent Au sites was apt to react with surface hydroxyl groups formed from water splitting, leading to a high WGS activity at low temperatures.
Authors:
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  1. Peking Univ., Beijing (China)
  2. Dalian Univ. of Technology, Dalian (China)
  3. Univ. of Chinese Academy of Sciences, Beijing (China); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Chinese Academy of Sciences, Shanxi (China); Synfuels China, Beijing (China)
  5. Brookhaven National Lab. (BNL), Upton, NY (United States)
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  7. Taiyuan Univ. of Technology, Shanxi (China)
  8. Lehigh Univ., Bethlehem, PA (United States)
  9. Chinese Academy of Sciences (CAS), Beijing (China)
Publication Date:
Report Number(s):
BNL-114190-2017-JA
Journal ID: ISSN 0036-8075; R&D Project: CO040; KC0302010; TRN: US1800180
Grant/Contract Number:
SC0012704; AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Science
Additional Journal Information:
Journal Volume: 357; Journal Issue: 6349; Journal ID: ISSN 0036-8075
Publisher:
AAAS
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1418304
Alternate Identifier(s):
OSTI ID: 1411142

Yao, Siyu, Zhang, Xiao, Zhou, Wu, Gao, Rui, Xu, Wenqian, Ye, Yifan, Lin, Lili, Wen, Xiaodong, Liu, Ping, Chen, Bingbing, Crumlin, Ethan, Guo, Jinghua, Zuo, Zhijun, Li, Weizhen, Xie, Jinglin, Lu, Li, Kiely, Christopher J., Gu, Lin, Shi, Chuan, Rodriguez, Jose A., and Ma, Ding. Atomic-layered Au clusters on α-MoC as catalysts for the low-temperature water-gas shift reaction. United States: N. p., Web. doi:10.1126/science.aah4321.
Yao, Siyu, Zhang, Xiao, Zhou, Wu, Gao, Rui, Xu, Wenqian, Ye, Yifan, Lin, Lili, Wen, Xiaodong, Liu, Ping, Chen, Bingbing, Crumlin, Ethan, Guo, Jinghua, Zuo, Zhijun, Li, Weizhen, Xie, Jinglin, Lu, Li, Kiely, Christopher J., Gu, Lin, Shi, Chuan, Rodriguez, Jose A., & Ma, Ding. Atomic-layered Au clusters on α-MoC as catalysts for the low-temperature water-gas shift reaction. United States. doi:10.1126/science.aah4321.
Yao, Siyu, Zhang, Xiao, Zhou, Wu, Gao, Rui, Xu, Wenqian, Ye, Yifan, Lin, Lili, Wen, Xiaodong, Liu, Ping, Chen, Bingbing, Crumlin, Ethan, Guo, Jinghua, Zuo, Zhijun, Li, Weizhen, Xie, Jinglin, Lu, Li, Kiely, Christopher J., Gu, Lin, Shi, Chuan, Rodriguez, Jose A., and Ma, Ding. 2017. "Atomic-layered Au clusters on α-MoC as catalysts for the low-temperature water-gas shift reaction". United States. doi:10.1126/science.aah4321. https://www.osti.gov/servlets/purl/1418304.
@article{osti_1418304,
title = {Atomic-layered Au clusters on α-MoC as catalysts for the low-temperature water-gas shift reaction},
author = {Yao, Siyu and Zhang, Xiao and Zhou, Wu and Gao, Rui and Xu, Wenqian and Ye, Yifan and Lin, Lili and Wen, Xiaodong and Liu, Ping and Chen, Bingbing and Crumlin, Ethan and Guo, Jinghua and Zuo, Zhijun and Li, Weizhen and Xie, Jinglin and Lu, Li and Kiely, Christopher J. and Gu, Lin and Shi, Chuan and Rodriguez, Jose A. and Ma, Ding},
abstractNote = {Here, the water-gas shift (WGS) reaction (where carbon monoxide plus water yields dihydrogen and carbon dioxide) is an essential process for hydrogen generation and carbon monoxide removal in various energy-related chemical operations. This equilibrium-limited reaction is favored at a low working temperature. Potential application in fuel cells also requires a WGS catalyst to be highly active, stable, and energy-efficient and to match the working temperature of on-site hydrogen generation and consumption units. We synthesized layered gold (Au) clusters on a molybdenum carbide (α-MoC) substrate to create an interfacial catalyst system for the ultralow-temperature WGS reaction. Water was activated over α-MoC at 303 kelvin, whereas carbon monoxide adsorbed on adjacent Au sites was apt to react with surface hydroxyl groups formed from water splitting, leading to a high WGS activity at low temperatures.},
doi = {10.1126/science.aah4321},
journal = {Science},
number = 6349,
volume = 357,
place = {United States},
year = {2017},
month = {6}
}

Works referenced in this record:

Generalized Gradient Approximation Made Simple
journal, October 1996
  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Projector augmented-wave method
journal, December 1994

Shape and Crystal-Plane Effects of Nanoscale Ceria on the Activity of Au-CeO2 Catalysts for the Water–Gas Shift Reaction
journal, March 2008
  • Si, Rui; Flytzani-Stephanopoulos, Maria
  • Angewandte Chemie International Edition, Vol. 47, Issue 15, p. 2884-2887
  • DOI: 10.1002/anie.200705828

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996

From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999

Activity and stability of low-content gold–cerium oxide catalysts for the water–gas shift reaction
journal, March 2005
  • Fu, Qi; Deng, Weiling; Saltsburg, Howard
  • Applied Catalysis B: Environmental, Vol. 56, Issue 1-2, p. 57-68
  • DOI: 10.1016/j.apcatb.2004.07.015

A climbing image nudged elastic band method for finding saddle points and minimum energy paths
journal, December 2000
  • Henkelman, Graeme; Uberuaga, Blas P.; Jónsson, Hannes
  • The Journal of Chemical Physics, Vol. 113, Issue 22, p. 9901-9904
  • DOI: 10.1063/1.1329672