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Title: Water-gas-shift over metal-free nanocrystalline ceria: An experimental and theoretical study

Abstract

Abstract A tandem experimental and theoretical investigation of a mesoporous ceria catalyst reveals the properties of the metal oxide are conducive for activity typically ascribed to metals, suggesting reduced Ce 3+ and oxygen vacancies are responsible for the inherent bi‐functionality of CO oxidation and dissociation of water required for facilitating the production of H 2 . The degree of reduction of the ceria, specifically the (1 0 0) face, is found to significantly influence the binding of reagents, suggesting reduced surfaces harbor the necessary reactive sites. The metal‐free catalysis of the reaction is significant for catalyst design considerations, and the suite of in situ analyses provides a comprehensive study of the dynamic nature of the high surface area catalyst system. This study postulates feasible improvements in catalytic activity may redirect the purpose of the water‐gas shift reaction from CO purification to primary hydrogen production.

Authors:
 [1];  [2];  [1];  [3];  [3];  [4];  [5];  [6];  [1];  [5];  [5];  [1]
+ Show Author Affiliations
  1. Univ. of Connecticut, Storrs, CT (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States); State Univ. of New York at Stony Brook, Stony Brook, NY (United States)
  3. Aarhus Univ. (Denmark)
  4. Technical Univ. of Catalonia- BarcelonaTech, Barcelona (Spain)
  5. Brookhaven National Lab. (BNL), Upton, NY (United States)
  6. Univ. of Connecticut, Storrs, CT (United States); Tanta Univ., Tanta (Egypt)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1368675
Alternate Identifier(s):
OSTI ID: 1401890
Report Number(s):
BNL-114017-2017-JA
Journal ID: ISSN 1867-3880; R&D Project: CO040; KC0302010
Grant/Contract Number:  
SC00112704; SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
ChemCatChem
Additional Journal Information:
Journal Volume: 9; Journal Issue: 8; Journal ID: ISSN 1867-3880
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; ceria; water-gas-shift; hydrogen; fuel cells; metal-free catalysis

Citation Formats

Guild, Curtis J., Vovchok, Dimitriy, Kriz, David A., Bruix, Albert, Hammer, Bjørk, Llorca, Jordi, Xu, Wenqian, El-Sawy, Abdelhamid, Biswas, Sourav, Rodriguez, Jose A., Senanayake, Sanjaya D., and Suib, Steven L. Water-gas-shift over metal-free nanocrystalline ceria: An experimental and theoretical study. United States: N. p., 2017. Web. doi:10.1002/cctc.201700081.
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Guild, Curtis J., Vovchok, Dimitriy, Kriz, David A., Bruix, Albert, Hammer, Bjørk, Llorca, Jordi, Xu, Wenqian, El-Sawy, Abdelhamid, Biswas, Sourav, Rodriguez, Jose A., Senanayake, Sanjaya D., & Suib, Steven L. Water-gas-shift over metal-free nanocrystalline ceria: An experimental and theoretical study. United States. https://doi.org/10.1002/cctc.201700081
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Guild, Curtis J., Vovchok, Dimitriy, Kriz, David A., Bruix, Albert, Hammer, Bjørk, Llorca, Jordi, Xu, Wenqian, El-Sawy, Abdelhamid, Biswas, Sourav, Rodriguez, Jose A., Senanayake, Sanjaya D., and Suib, Steven L. Mon . "Water-gas-shift over metal-free nanocrystalline ceria: An experimental and theoretical study". United States. https://doi.org/10.1002/cctc.201700081. https://www.osti.gov/servlets/purl/1368675.
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@article{osti_1368675,
title = {Water-gas-shift over metal-free nanocrystalline ceria: An experimental and theoretical study},
author = {Guild, Curtis J. and Vovchok, Dimitriy and Kriz, David A. and Bruix, Albert and Hammer, Bjørk and Llorca, Jordi and Xu, Wenqian and El-Sawy, Abdelhamid and Biswas, Sourav and Rodriguez, Jose A. and Senanayake, Sanjaya D. and Suib, Steven L.},
abstractNote = {Abstract A tandem experimental and theoretical investigation of a mesoporous ceria catalyst reveals the properties of the metal oxide are conducive for activity typically ascribed to metals, suggesting reduced Ce 3+ and oxygen vacancies are responsible for the inherent bi‐functionality of CO oxidation and dissociation of water required for facilitating the production of H 2 . The degree of reduction of the ceria, specifically the (1 0 0) face, is found to significantly influence the binding of reagents, suggesting reduced surfaces harbor the necessary reactive sites. The metal‐free catalysis of the reaction is significant for catalyst design considerations, and the suite of in situ analyses provides a comprehensive study of the dynamic nature of the high surface area catalyst system. This study postulates feasible improvements in catalytic activity may redirect the purpose of the water‐gas shift reaction from CO purification to primary hydrogen production.},
doi = {10.1002/cctc.201700081},
journal = {ChemCatChem},
number = 8,
volume = 9,
place = {United States},
year = {Mon Jan 23 00:00:00 EST 2017},
month = {Mon Jan 23 00:00:00 EST 2017}
}
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https://doi.org/10.1002/cctc.201700081
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