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

Journal Article · · Journal of the American Chemical Society
DOI:https://doi.org/10.1021/jacs.5b03668· OSTI ID:1355784
 [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
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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.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1355784
Journal Information:
Journal of the American Chemical Society, Vol. 137, Issue 27; ISSN 0002-7863
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 247 works
Citation information provided by
Web of Science

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Combined CO 2 Capture and Hydrogenation to Methanol: Amine Immobilization Enables Easy Recycling of Active Elements journal April 2019
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Reversing Size-Dependent Trends in the Oxidation of Copper Clusters through Support Effects: Reversing Size-Dependent Trends in the Oxidation of Copper Clusters through Support Effects journal December 2017
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Efficient Visible-Light-Driven Carbon Dioxide Reduction by a Single-Atom Implanted Metal-Organic Framework journal October 2016
Copper Catalysts Unleashing the Potential for Hydrogenation of Carbon−Oxygen Bonds journal September 2018
Performance of Preformed Au/Cu Nanoclusters Deposited on MgO Powders in the Catalytic Reduction of 4-Nitrophenol in Solution journal February 2018
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