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氧化铟上乙炔的半氢化:提出的单集合催化作用。

Semihydrogenation of Acetylene on Indium Oxide: Proposed Single-Ensemble Catalysis.

机构信息

ETH Zurich, Department of Chemistry and Applied Biosciences, Institute for Chemical and Bioengineering, Vladimir-Prelog-Weg 1, 8093, Zurich, Switzerland.

Institute of Chemical Research of Catalonia (ICIQ) and, The Barcelona Institute of Science and Technology, Av. Països Catalans 16, 43007, Tarragona, Spain.

出版信息

Angew Chem Int Ed Engl. 2017 Aug 28;56(36):10755-10760. doi: 10.1002/anie.201704999. Epub 2017 Jul 25.

DOI:10.1002/anie.201704999
PMID:28696499
Abstract

Indium oxide catalyzes acetylene hydrogenation with high selectivity to ethylene (>85 %); even with a large excess of the alkene. In situ characterization reveals the formation of oxygen vacancies under reaction conditions, while an in depth theoretical analysis links the surface reduction with the creation of well-defined vacancies and surrounding In O ensembles, which are considered responsible for this outstanding catalytic function. This behavior, which differs from that of other common reducible oxides, originates from the presence of four crystallographically inequivalent oxygen sites in the indium oxide surface. These resulting ensembles are 1) stable against deactivation, 2) homogeneously and densely distributed, and 3) spatially isolated and confined against transport; thereby broadening the scope of oxides in hydrogenation catalysis.

摘要

氧化铟能高选择性地催化乙炔氢化为乙烯(>85%);即使烯烃过量也是如此。原位表征表明,在反应条件下形成了氧空位,而深入的理论分析将表面还原与明确定义的空位和周围的 In O 团簇的形成联系起来,这被认为是导致这种出色催化功能的原因。这种行为与其他常见的可还原氧化物不同,起源于氧化铟表面的四个晶相不等价的氧位。这些形成的团簇具有以下特点:1)稳定,不易失活;2)均匀且密集地分布;3)空间上相互隔离和限制,防止传输;从而拓宽了氧化物在加氢催化中的应用范围。

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