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

Abstract

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:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3];  [4]; ORCiD logo [5];  [6]; ORCiD logo [1];  [4]; ORCiD logo [5]; ORCiD logo [2]; ORCiD logo [6]; ORCiD logo [6];  [7];  [1]; ORCiD logo [1]; ORCiD logo [8]; ORCiD logo [8]; ORCiD logo [9]; ORCiD logo [2]; ORCiD logo [5] more »; ORCiD logo [1] « less
  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:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1418304
Alternate Identifier(s):
OSTI ID: 1411142
Report Number(s):
BNL-114190-2017-JA
Journal ID: ISSN 0036-8075; ark:/13030/qt92s96063; TRN: US1801262
Grant/Contract Number:  
AC02-05CH11231; SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Science
Additional Journal Information:
Journal Volume: 357; Journal Issue: 6349; Journal ID: ISSN 0036-8075
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

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, José 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., 2017. 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, José A., & Ma, Ding. Atomic-layered Au clusters on α-MoC as catalysts for the low-temperature water-gas shift reaction. United States. https://doi.org/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, José A., and Ma, Ding. Fri . "Atomic-layered Au clusters on α-MoC as catalysts for the low-temperature water-gas shift reaction". United States. https://doi.org/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, José 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 = {Fri Jul 28 00:00:00 EDT 2017},
month = {Fri Jul 28 00:00:00 EDT 2017}
}

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