Carbon Dioxide Conversion to Methanol over Size-Selected Cu 4 Clusters at Low Pressures
Abstract
In order to utilize the captured CO2, the activation of CO2 and its hydrogenation to methanol are of much interest . We investigate the use of size-selected Cu-4 clusters supported on Al2O3 thin films for CO2 reduction in the presence of hydrogen. The catalytic activity was measured under near-atmospheric reaction conditions with a low CO2 partial pressure, and the oxidation state of the clusters was investigated by in situ grazing incidence X-ray absorption spectroscopy. The results indicate that size-selected Cu-4 clusters are the most active low-pressure catalyst for catalytic CO2 conversion to CH3OH. Density functional theory calculations reveal that Cu-4 clusters have a low activation barrier for conversion of CO2 to CH3OH. Our study suggests that small Cu clusters may be excellent and efficient catalysts for the recycling of released CO2.
- Authors:
-
- Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
- Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
- Univ. of Freiburg (Germany). Physical Inst.
- Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division and Nanoscience and Technology Division; Yale Univ., New Haven, CT (United States). Dept. of Chemical and Environmental Engineering; Univ. of Chicago, IL (United States). Inst. for Molecular Engineering
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1355784
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 137; Journal Issue: 27; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 54 ENVIRONMENTAL SCIENCES
Citation Formats
Liu, Cong, Yang, Bing, Tyo, Eric, Seifert, Soenke, DeBartolo, Janae, von Issendorff, Bernd, Zapol, Peter, Vajda, Stefan, and Curtiss, Larry A. Carbon Dioxide Conversion to Methanol over Size-Selected Cu 4 Clusters at Low Pressures. United States: N. p., 2015.
Web. doi:10.1021/jacs.5b03668.
Liu, Cong, Yang, Bing, Tyo, Eric, Seifert, Soenke, DeBartolo, Janae, von Issendorff, Bernd, Zapol, Peter, Vajda, Stefan, & Curtiss, Larry A. Carbon Dioxide Conversion to Methanol over Size-Selected Cu 4 Clusters at Low Pressures. United States. https://doi.org/10.1021/jacs.5b03668
Liu, Cong, Yang, Bing, Tyo, Eric, Seifert, Soenke, DeBartolo, Janae, von Issendorff, Bernd, Zapol, Peter, Vajda, Stefan, and Curtiss, Larry A. Fri .
"Carbon Dioxide Conversion to Methanol over Size-Selected Cu 4 Clusters at Low Pressures". United States. https://doi.org/10.1021/jacs.5b03668. https://www.osti.gov/servlets/purl/1355784.
@article{osti_1355784,
title = {Carbon Dioxide Conversion to Methanol over Size-Selected Cu 4 Clusters at Low Pressures},
author = {Liu, Cong and Yang, Bing and Tyo, Eric and Seifert, Soenke and DeBartolo, Janae and von Issendorff, Bernd and Zapol, Peter and Vajda, Stefan and Curtiss, Larry A.},
abstractNote = {In order to utilize the captured CO2, the activation of CO2 and its hydrogenation to methanol are of much interest . We investigate the use of size-selected Cu-4 clusters supported on Al2O3 thin films for CO2 reduction in the presence of hydrogen. The catalytic activity was measured under near-atmospheric reaction conditions with a low CO2 partial pressure, and the oxidation state of the clusters was investigated by in situ grazing incidence X-ray absorption spectroscopy. The results indicate that size-selected Cu-4 clusters are the most active low-pressure catalyst for catalytic CO2 conversion to CH3OH. Density functional theory calculations reveal that Cu-4 clusters have a low activation barrier for conversion of CO2 to CH3OH. Our study suggests that small Cu clusters may be excellent and efficient catalysts for the recycling of released CO2.},
doi = {10.1021/jacs.5b03668},
journal = {Journal of the American Chemical Society},
number = 27,
volume = 137,
place = {United States},
year = {Fri Jun 26 00:00:00 EDT 2015},
month = {Fri Jun 26 00:00:00 EDT 2015}
}
Web of Science
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