Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439, USA.
1] Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439, USA [2] Nanoscience and Technology Division, Argonne National Laboratory, Argonne, Illinois 60439, USA [3] Department of Chemical and Environmental Engineering, School of Engineering, Yale University, New Haven, Connecticut 06520, USA [4] Institute for Molecular Engineering, The University of Chicago, Chicago, Illinois 60637, USA.
Nat Nanotechnol. 2015 Jul;10(7):577-88. doi: 10.1038/nnano.2015.140.
Clusters that contain only a small number of atoms can exhibit unique and often unexpected properties. The clusters are of particular interest in catalysis because they can act as individual active sites, and minor changes in size and composition--such as the addition or removal of a single atom--can have a substantial influence on the activity and selectivity of a reaction. Here, we review recent progress in the synthesis and characterization of well-defined subnanometre clusters, and the understanding and exploitation of their catalytic properties. We examine work on size-selected supported clusters in ultrahigh-vacuum environments and under realistic reaction conditions, and explore the use of computational methods to provide a mechanistic understanding of their catalytic properties. We also highlight the potential of size-selected clusters to provide insights into important catalytic processes and their use in the development of novel catalytic systems.
只包含少量原子的团簇可以表现出独特且常常出人意料的性质。这些团簇在催化中特别有趣，因为它们可以充当单个活性位，而大小和组成的微小变化（例如添加或去除一个单个原子）可以对反应的活性和选择性产生实质性影响。在这里，我们综述了最近在合成和表征具有良好定义的亚纳米团簇方面的进展，以及对其催化性质的理解和利用。我们考察了在超高真空环境中和在实际反应条件下对尺寸选择的负载团簇的研究，并探讨了计算方法的使用，以提供对其催化性质的机械理解。我们还强调了尺寸选择的团簇在提供对重要催化过程的见解以及在开发新型催化系统中的应用的潜力。
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