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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-MoCat 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 Lab. (LBNL), Berkeley, CA (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
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. 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., and Ma, Ding. Fri . "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, 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-MoCat 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 = {7}
}

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Works referenced in this record:

ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT
journal, June 2005


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

Water–gas shift catalysis over transition metals supported on molybdenum carbide
journal, November 2015


Stabilized Gold Nanoparticles on Ceria Nanorods by Strong Interfacial Anchoring
journal, December 2012

  • Ta, Na; Liu, Jingyue (Jimmy); Chenna, Santhosh
  • Journal of the American Chemical Society, Vol. 134, Issue 51
  • DOI: 10.1021/ja310341j

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


Tuning the electronic behavior of Au nanoparticles with capping molecules
journal, July 2002

  • Zhang, P.; Sham, T. K.
  • Applied Physics Letters, Vol. 81, Issue 4
  • DOI: 10.1063/1.1494120

Molybdenum Carbide as Alternative Catalysts to Precious Metals for Highly Selective Reduction of CO 2 to CO
journal, May 2014

  • Porosoff, Marc D.; Yang, Xiaofang; Boscoboinik, J. Anibal
  • Angewandte Chemie International Edition, Vol. 53, Issue 26
  • DOI: 10.1002/anie.201404109

Charge Polarization at a Au-TiC Interface and the Generation of Highly Active and Selective Catalysts for the Low-Temperature Water-Gas Shift Reaction
journal, September 2014

  • Rodriguez, José A.; Ramírez, Pedro J.; Asara, Gian Giacomo
  • Angewandte Chemie International Edition, Vol. 53, Issue 42
  • DOI: 10.1002/anie.201407208

Activity of CeOx and TiOx Nanoparticles Grown on Au(111) in the Water-Gas Shift Reaction
journal, December 2007


Catalytically active Au-O(OH) x - species stabilized by alkali ions on zeolites and mesoporous oxides
journal, November 2014


Water-Gas Shift Reaction on a Highly Active Inverse CeO x /Cu(111) Catalyst: Unique Role of Ceria Nanoparticles
journal, October 2009

  • Rodriguez, José A.; Graciani, Jesús; Evans, Jaime
  • Angewandte Chemie International Edition, Vol. 48, Issue 43
  • DOI: 10.1002/anie.200903918

The water-gas shift reaction: from conventional catalytic systems to Pd-based membrane reactors-a review
journal, January 2010

  • Mendes, D.; Mendes, A.; Madeira, L. M.
  • Asia-Pacific Journal of Chemical Engineering, Vol. 5, Issue 1
  • DOI: 10.1002/apj.364

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


High Activity Carbide Supported Catalysts for Water Gas Shift
journal, March 2011

  • Schweitzer, Neil M.; Schaidle, Joshua A.; Ezekoye, Obiefune K.
  • Journal of the American Chemical Society, Vol. 133, Issue 8
  • DOI: 10.1021/ja110705a

Homogeneous catalysis by ruthenium carbonyl in alkaline solution: the water gas shift reaction
journal, January 1977

  • Laine, Richard M.; Rinker, Robert G.; Ford, Peter C.
  • Journal of the American Chemical Society, Vol. 99, Issue 1
  • DOI: 10.1021/ja00443a049

Low-temperature water-gas shift reaction over Cu- and Ni-loaded cerium oxide catalysts
journal, August 2000


Atomically Dispersed Au–(OH) x Species Bound on Titania Catalyze the Low-Temperature Water-Gas Shift Reaction
journal, March 2013

  • Yang, Ming; Allard, Lawrence F.; Flytzani-Stephanopoulos, Maria
  • Journal of the American Chemical Society, Vol. 135, Issue 10
  • DOI: 10.1021/ja312646d

Active Nonmetallic Au and Pt Species on Ceria-Based Water-Gas Shift Catalysts
journal, August 2003


Low-Temperature Water–Gas Shift Reaction over Au/α-Fe2O3
journal, January 1996


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

Thermal stability and catalytic activity of gold nanoparticles supported on silica
journal, February 2009


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

Remarkable Performance of Ir 1 /FeO x Single-Atom Catalyst in Water Gas Shift Reaction
journal, October 2013

  • Lin, Jian; Wang, Aiqin; Qiao, Botao
  • Journal of the American Chemical Society, Vol. 135, Issue 41
  • DOI: 10.1021/ja408574m

Probing the Low-Temperature Water–Gas Shift Activity of Alkali-Promoted Platinum Catalysts Stabilized on Carbon Supports
journal, February 2014

  • Zugic, Branko; Zhang, Shiran; Bell, David C.
  • Journal of the American Chemical Society, Vol. 136, Issue 8
  • DOI: 10.1021/ja4123889

Water Gas Shift Catalysis
journal, September 2009


Catalytically active structures of SiO 2 -supported Au nanoparticles in low-temperature CO oxidation
journal, January 2013

  • Qian, Kun; Luo, Liangfeng; Bao, Huizhi
  • Catal. Sci. Technol., Vol. 3, Issue 3
  • DOI: 10.1039/C2CY20481A

Molybdenum carbide catalysts I. Synthesis of unsupported powders
journal, July 1987


Preparation and catalytic properties of transition metal carbides and nitrides
journal, June 1992


Alkali-Stabilized Pt-OHx Species Catalyze Low-Temperature Water-Gas Shift Reactions
journal, September 2010


EXAFS as a tool to interrogate the size and shape of mono and bimetallic catalyst nanoparticles
journal, January 2010

  • Beale, Andrew M.; Weckhuysen, Bert M.
  • Physical Chemistry Chemical Physics, Vol. 12, Issue 21
  • DOI: 10.1039/b925206a

Comparison of the activity of Au/CeO2 and Au/Fe2O3 catalysts for the CO oxidation and the water-gas shift reactions
journal, June 2007


    Works referencing / citing this record:

    Confined Pt 1 1+ Water Clusters in a MOF Catalyze the Low-Temperature Water-Gas Shift Reaction with both CO 2 Oxygen Atoms Coming from Water
    journal, November 2018

    • Rivero-Crespo, Miguel A.; Mon, Marta; Ferrando-Soria, Jesús
    • Angewandte Chemie International Edition, Vol. 57, Issue 52
    • DOI: 10.1002/anie.201810251

    New Strategies for the Preparation of Sinter‐Resistant Metal‐Nanoparticle‐Based Catalysts
    journal, July 2019

    • Wang, Lingxiang; Wang, Liang; Meng, Xiangju
    • Advanced Materials, Vol. 31, Issue 50
    • DOI: 10.1002/adma.201901905

    Supported Noble‐Metal Single Atoms for Heterogeneous Catalysis
    journal, July 2019

    • Li, Xuning; Yang, Xiaofeng; Huang, Yanqiang
    • Advanced Materials, Vol. 31, Issue 50
    • DOI: 10.1002/adma.201902031

    Highly Selective Photoreduction of CO 2 with Suppressing H 2 Evolution over Monolayer Layered Double Hydroxide under Irradiation above 600 nm
    journal, July 2019

    • Tan, Ling; Xu, Si-Min; Wang, Zelin
    • Angewandte Chemie International Edition, Vol. 58, Issue 34
    • DOI: 10.1002/anie.201904246

    Carbon vacancy defect-activated Pt cluster for hydrogen generation
    journal, January 2019

    • Bao, Xiaobing; Gong, Yutong; Chen, Yuzhuo
    • Journal of Materials Chemistry A, Vol. 7, Issue 25
    • DOI: 10.1039/c9ta04010b

    Controlled synthesis of 2D Mo 2 C/graphene heterostructure on liquid Au substrates as enhanced electrocatalytic electrodes
    journal, July 2019


    New Strategies for the Preparation of Sinter‐Resistant Metal‐Nanoparticle‐Based Catalysts
    journal, July 2019

    • Wang, Lingxiang; Wang, Liang; Meng, Xiangju
    • Advanced Materials, Vol. 31, Issue 50
    • DOI: 10.1002/adma.201901905

    Supported Noble‐Metal Single Atoms for Heterogeneous Catalysis
    journal, July 2019

    • Li, Xuning; Yang, Xiaofeng; Huang, Yanqiang
    • Advanced Materials, Vol. 31, Issue 50
    • DOI: 10.1002/adma.201902031

    Confined Pt 1 1+ Water Clusters in a MOF Catalyze the Low-Temperature Water-Gas Shift Reaction with both CO 2 Oxygen Atoms Coming from Water
    journal, November 2018

    • Rivero-Crespo, Miguel A.; Mon, Marta; Ferrando-Soria, Jesús
    • Angewandte Chemie International Edition, Vol. 57, Issue 52
    • DOI: 10.1002/anie.201810251

    Highly Selective Photoreduction of CO 2 with Suppressing H 2 Evolution over Monolayer Layered Double Hydroxide under Irradiation above 600 nm
    journal, July 2019

    • Tan, Ling; Xu, Si-Min; Wang, Zelin
    • Angewandte Chemie International Edition, Vol. 58, Issue 34
    • DOI: 10.1002/anie.201904246

    Carbon vacancy defect-activated Pt cluster for hydrogen generation
    journal, January 2019

    • Bao, Xiaobing; Gong, Yutong; Chen, Yuzhuo
    • Journal of Materials Chemistry A, Vol. 7, Issue 25
    • DOI: 10.1039/c9ta04010b

    Controlled synthesis of 2D Mo 2 C/graphene heterostructure on liquid Au substrates as enhanced electrocatalytic electrodes
    journal, July 2019