Carbon Dioxide Conversion to Methanol over Size-Selected Cu4 Clusters at Low Pressures

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• 作者：Cong Liu ; Bing Yang ; Eric Tyo ; Soenke Seifert ; Janae DeBartolo ; Bernd von Issendorff ; Peter Zapol ; Stefan Vajda ; Larry A. Curtiss
• 刊名：Journal of the American Chemical Society
• 出版年：2015
• 出版时间：July 15, 2015
• 年：2015
• 卷：137
• 期：27
• 页码：8676-8679
• 全文大小：295K
• ISSN：1520-5126

文摘

The activation of CO₂ and its hydrogenation to methanol are of much interest as a way to utilize captured CO₂. Here, we investigate the use of size-selected Cu₄ 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 Cu₄ clusters are the most active low-pressure catalyst for catalytic CO₂ conversion to CH₃OH. Density functional theory calculations reveal that Cu₄ clusters have a low activation barrier for conversion of CO₂ to CH₃OH. This study suggests that small Cu clusters may be excellent and efficient catalysts for the recycling of released CO₂.