Influence of Coordination Environment of Anchored Single-Site Cobalt Catalyst on CO2 Hydrogenation
Abstract
Heterogeneous catalysts generally have a variety of active-site structures due to the innate heterogeneity of the surface,resulting in complicated correlations between activity and active-site structure. Single site heterogeneous cobalt catalysts with a uniform catalytic surface were utilized as a platform to probe surface sensitive reactions; in this case CO2 hydrogenation. It was found that atomically isolated cobalt single sites, which exist solely in the tetrahedral Co2+ coordination, exclusively form CO under typical CO2 methanation conditions,while cobalt clusters yielded the highest rate of CO2 reactionand began to form methane. Utilizing the principles of Ostwald Ripening to probe the ensemble effects for CO2 hydrogenation, the transition from atomic isolation to small clusters of atoms to nanoparticles was explored. Furthermore, the chemical structure of the cobalt was elucidated primarily via X-Ray Absorption Spectroscopy (XANES/EXAFS) and X-Ray Photoelectron Spectroscopy (XPS).
- Authors:
-
[1]
- Univ. of South Carolina, Columbia, SC (United States)
- Argonne National Lab. (ANL), Lemont, IL (United States)
- Argonne National Lab. (ANL), Lemont, IL (United States); Illinois Institute of Technology, Chicago, IL (United States). Center for Synchrotron Research and Instrumentation
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1763652
- Alternate Identifier(s):
- OSTI ID: 1579470
- Grant/Contract Number:
- AC02-06CH11357; DGE-1250052
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ChemCatChem
- Additional Journal Information:
- Journal Volume: 12; Journal Issue: 3; Journal ID: ISSN 1867-3880
- Publisher:
- ChemPubSoc Europe
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CO2 methanation; Cobalt single-site catalysts; XAFS; XPS; CO2 hydrogenation; Cobalt; Ensemble effects; Ostwald Ripening
Citation Formats
Jimenez, Juan D., Wen, Cun, Royko, Michael M., Kropf, Arthur J., Segre, Carlo, and Lauterbach, Jochen. Influence of Coordination Environment of Anchored Single-Site Cobalt Catalyst on CO2 Hydrogenation. United States: N. p., 2019.
Web. doi:10.1002/cctc.201901676.
Jimenez, Juan D., Wen, Cun, Royko, Michael M., Kropf, Arthur J., Segre, Carlo, & Lauterbach, Jochen. Influence of Coordination Environment of Anchored Single-Site Cobalt Catalyst on CO2 Hydrogenation. United States. https://doi.org/10.1002/cctc.201901676
Jimenez, Juan D., Wen, Cun, Royko, Michael M., Kropf, Arthur J., Segre, Carlo, and Lauterbach, Jochen. Mon .
"Influence of Coordination Environment of Anchored Single-Site Cobalt Catalyst on CO2 Hydrogenation". United States. https://doi.org/10.1002/cctc.201901676. https://www.osti.gov/servlets/purl/1763652.
@article{osti_1763652,
title = {Influence of Coordination Environment of Anchored Single-Site Cobalt Catalyst on CO2 Hydrogenation},
author = {Jimenez, Juan D. and Wen, Cun and Royko, Michael M. and Kropf, Arthur J. and Segre, Carlo and Lauterbach, Jochen},
abstractNote = {Heterogeneous catalysts generally have a variety of active-site structures due to the innate heterogeneity of the surface,resulting in complicated correlations between activity and active-site structure. Single site heterogeneous cobalt catalysts with a uniform catalytic surface were utilized as a platform to probe surface sensitive reactions; in this case CO2 hydrogenation. It was found that atomically isolated cobalt single sites, which exist solely in the tetrahedral Co2+ coordination, exclusively form CO under typical CO2 methanation conditions,while cobalt clusters yielded the highest rate of CO2 reactionand began to form methane. Utilizing the principles of Ostwald Ripening to probe the ensemble effects for CO2 hydrogenation, the transition from atomic isolation to small clusters of atoms to nanoparticles was explored. Furthermore, the chemical structure of the cobalt was elucidated primarily via X-Ray Absorption Spectroscopy (XANES/EXAFS) and X-Ray Photoelectron Spectroscopy (XPS).},
doi = {10.1002/cctc.201901676},
journal = {ChemCatChem},
number = 3,
volume = 12,
place = {United States},
year = {Mon Dec 16 00:00:00 EST 2019},
month = {Mon Dec 16 00:00:00 EST 2019}
}
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