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Title: Carbon Dioxide Conversion to Methanol over Size-Selected Cu 4 Clusters at Low Pressures

In order to utilize the captured CO 2, the activation of CO 2 and its hydrogenation to methanol are of much interest . We investigate the use of size-selected Cu-4 clusters supported on Al 2O 3 thin films for CO 2 reduction in the presence of hydrogen. The catalytic activity was measured under near-atmospheric reaction conditions with a low CO 2 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 CO 2 conversion to CH 3OH. Density functional theory calculations reveal that Cu-4 clusters have a low activation barrier for conversion of CO 2 to CH 3OH. Our study suggests that small Cu clusters may be excellent and efficient catalysts for the recycling of released CO 2.
Authors:
 [1] ;  [1] ;  [1] ;  [2] ;  [2] ;  [3] ;  [1] ;  [4] ;  [1]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
  2. Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
  3. Univ. of Freiburg (Germany). Physical Inst.
  4. 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:
Grant/Contract Number:
AC02-06CH11357
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)
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 54 ENVIRONMENTAL SCIENCES
OSTI Identifier:
1355784

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., 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. doi: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. 2015. "Carbon Dioxide Conversion to Methanol over Size-Selected Cu 4 Clusters at Low Pressures". United States. doi: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 = {2015},
month = {6}
}