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Carbon Dioxide Conversion to Methanol over Size-Selected Cu_4 Clusters at Low Pressures

机译:在低压下按尺寸选择的Cu_4团簇将二氧化碳转化为甲醇

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摘要

The activation of CO_2 and its hydro-genation to methanol are of much interest as a way to utilize captured CO_2. Here, we investigate the use of size-selected Cu_4 dusters 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 dusters have a low activation barrier for conversion of CO_2 to CH_3OH. This study suggests that small Cu clusters may be excellent and efficient catalysts for the recycling of released CO_2.
机译:作为利用捕获的CO_2的一种方式,CO_2的活化及其加氢成甲醇是非常令人感兴趣的。在这里,我们研究了在氢气存在下,将选择的载于Al_2O_3薄膜上的Cu_4除尘器用于还原CO_2的用途。在接近大气的反应条件下以低的CO_2分压测量了催化活性,并通过原位掠入射X射线吸收光谱研究了簇的氧化态。结果表明,大小选择的Cu_4团簇是将CO_2催化转化为CH_3OH的最活跃的低压催化剂。密度泛函理论计算表明,Cu_4除尘器具有较低的活化势垒,可以将CO_2转化为CH_3OH。这项研究表明,小的铜团簇可能是释放释放的CO_2的优秀而有效的催化剂。

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  • 来源
    《Journal of the American Chemical Society》 |2015年第27期|8676-8679|共4页
  • 作者单位

    Materials Science Division, Argonne National Laboratory, 9700 S. Cass Ave., Lemont, Illinois 60439, United States;

    Materials Science Division, Argonne National Laboratory, 9700 S. Cass Ave., Lemont, Illinois 60439, United States;

    Materials Science Division, Argonne National Laboratory, 9700 S. Cass Ave., Lemont, Illinois 60439, United States;

    X-ray Science Division, Argonne National Laboratory, 9700 S. Cass Ave., Lemont, Illinois 60439, United States;

    X-ray Science Division, Argonne National Laboratory, 9700 S. Cass Ave., Lemont, Illinois 60439, United States;

    Physikalisches Institut, Universitaet Freiburg, Stefan-Meier-Strasse 21, 79104 Freiburg, Germany;

    Materials Science Division, Argonne National Laboratory, 9700 S. Cass Ave., Lemont, Illinois 60439, United States;

    Materials Science Division, Argonne National Laboratory, 9700 S. Cass Ave., Lemont, Illinois 60439, United States,Nanoscience and Technology Division, Argonne National Laboratory, 9700 S. Cass Ave., Lemont, Illinois 60439, United States,Department of Chemical and Environmental Engineering, School of Engineering & Applied Science, Yale University, 9 Hillhouse Avenue, New Haven, Connecticut 06520, United States,Institute for Molecular Engineering, University of Chicago, 5801 South Ellis Avenue, Chicago, Illinois 60637, United States;

    Materials Science Division, Argonne National Laboratory, 9700 S. Cass Ave., Lemont, Illinois 60439, United States;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
  • 原文格式 PDF
  • 正文语种 eng
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  • 入库时间 2022-08-18 03:09:44

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