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

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. Finally, 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]
  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) (SC-22)
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:
Journal Article: 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.
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. doi:10.1002/cctc.201700081.
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. doi:10.1002/cctc.201700081. https://www.osti.gov/servlets/purl/1368675.
@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 = {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 Ce3+ and oxygen vacancies are responsible for the inherent bi-functionality of CO oxidation and dissociation of water required for facilitating the production of H2. 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. Finally, 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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