CO oxidation activity of non-reducible oxide-supported mass-selected few-atom Pt single-clusters.,Nature Communications

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CO oxidation activity of non-reducible oxide-supported mass-selected few-atom Pt single-clusters.
Nature Communications ( IF 14.7 ) Pub Date : 2020-04-20 , DOI: 10.1038/s41467-020-15850-4
Atsushi Beniya ₁ , Shougo Higashi ₁ , Nobuko Ohba ₁ , Ryosuke Jinnouchi ₁ , Hirohito Hirata ₂ , Yoshihide Watanabe ₁

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Platinum nanocatalysts play critical roles in CO oxidation, an important catalytic conversion process. As the catalyst size decreases, the influence of the support material on catalysis increases which can alter the chemical states of Pt atoms in contact with the support. Herein, we demonstrate that under-coordinated Pt atoms at the edges of the first cluster layer are rendered cationic by direct contact with the Al2O3 support, which affects the overall CO oxidation activity. The ratio of neutral to cationic Pt atoms in the Pt nanocluster is strongly correlated with the CO oxidation activity, but no correlation exists with the total surface area of surface-exposed Pt atoms. The low oxygen affinity of cationic Pt atoms explains this counterintuitive result. Using this relationship and our modified bond-additivity method, which only requires the catalyst-support bond energy as input, we successfully predict the CO oxidation activities of various sized Pt clusters on TiO2.

中文翻译：

不可还原氧化物负载的质量选择的少原子 Pt 单团簇的 CO 氧化活性。

铂纳米催化剂在 CO 氧化这一重要的催化转化过程中发挥着关键作用。随着催化剂尺寸的减小，载体材料对催化作用的影响增加，这可以改变与载体接触的 Pt 原子的化学状态。在此，我们证明第一簇层边缘的配位不足的 Pt 原子通过与 Al2O3 载体直接接触而呈现出阳离子，从而影响整体 CO 氧化活性。 Pt纳米团簇中中性与阳离子Pt原子的比例与CO氧化活性密切相关，但与表面暴露的Pt原子的总表面积不存在相关性。阳离子 Pt 原子的低氧亲和力解释了这一违反直觉的结果。利用这种关系和我们改进的键加成方法（仅需要催化剂载体键能作为输入），我们成功预测了 TiO2 上各种尺寸的 Pt 簇的 CO 氧化活性。

更新日期：2020-04-24

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