skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Reaction of CO 2 with UO 3 Nanoclusters

Abstract

Adsorption of CO 2 to uranium oxide, (UO 3) n, clusters was modeled using density functional theory (DFT) and coupled cluster theory (CCSD(T)). Geometries and reaction energies were indicated for carbonate formation (chemisorption) and Lewis acid–base addition of CO 2 (physisorption) to these (UO 3) n clusters. Chemisorption of multiple CO 2 moieties was also modeled for dimer and trimer clusters. Physisorption and chemisorption were both predicted to be thermodynamically allowed for (UO 3) n clusters, with chemisorption being more thermodynamically favorable than physisorption. The most energetically favored (UO 3) 3(CO 2) m clusters contain tridentate carbonates, which is consistent with solid-state and solution structures for uranyl carbonates. The calculations show that CO 2 exposure is bound to convert (UO 3) n to uranyl carbonates.

Authors:
 [1];  [1];  [1]; ORCiD logo [1]
  1. Univ. of Alabama, Tuscaloosa, AL (United States)
Publication Date:
Research Org.:
Georgia Inst. of Technology, Atlanta, GA (United States). Energy Frontier Research Center (EFRC) Center for Understanding and Control of Acid Gas-induced Evolution of Materials for Energy (UNCAGE-ME)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1470291
Grant/Contract Number:  
[SC0012577]
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory
Additional Journal Information:
[ Journal Volume: 121; Journal Issue: 44; Related Information: UNCAGE-ME partners with Georgia Institute of Technology (lead); Lehigh University; Oak Ridge National Laboratory; University of Alabama; University of Florida; University of Wisconsin; Washington University in St. Louis]; Journal ID: ISSN 1089-5639
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Flores, Luis A., Murphy, Julia G., Copeland, William B., and Dixon, David A. Reaction of CO2 with UO3 Nanoclusters. United States: N. p., 2017. Web. doi:10.1021/acs.jpca.7b09107.
Flores, Luis A., Murphy, Julia G., Copeland, William B., & Dixon, David A. Reaction of CO2 with UO3 Nanoclusters. United States. doi:10.1021/acs.jpca.7b09107.
Flores, Luis A., Murphy, Julia G., Copeland, William B., and Dixon, David A. Fri . "Reaction of CO2 with UO3 Nanoclusters". United States. doi:10.1021/acs.jpca.7b09107. https://www.osti.gov/servlets/purl/1470291.
@article{osti_1470291,
title = {Reaction of CO2 with UO3 Nanoclusters},
author = {Flores, Luis A. and Murphy, Julia G. and Copeland, William B. and Dixon, David A.},
abstractNote = {Adsorption of CO2 to uranium oxide, (UO3)n, clusters was modeled using density functional theory (DFT) and coupled cluster theory (CCSD(T)). Geometries and reaction energies were indicated for carbonate formation (chemisorption) and Lewis acid–base addition of CO2 (physisorption) to these (UO3)n clusters. Chemisorption of multiple CO2 moieties was also modeled for dimer and trimer clusters. Physisorption and chemisorption were both predicted to be thermodynamically allowed for (UO3)n clusters, with chemisorption being more thermodynamically favorable than physisorption. The most energetically favored (UO3)3(CO2)m clusters contain tridentate carbonates, which is consistent with solid-state and solution structures for uranyl carbonates. The calculations show that CO2 exposure is bound to convert (UO3)n to uranyl carbonates.},
doi = {10.1021/acs.jpca.7b09107},
journal = {Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory},
number = [44],
volume = [121],
place = {United States},
year = {2017},
month = {10}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 1 work
Citation information provided by
Web of Science

Save / Share: