Department of Chemical and Petroleum Engineering and Department of Chemistry, University of Kansas , Lawrence, Kansas 66045, United States.
Department of Physics, Yeshiva University , New York, New York 10016, United States.
Nano Lett. 2016 Aug 10;16(8):5001-9. doi: 10.1021/acs.nanolett.6b01718. Epub 2016 Jul 28.
Heterogeneous catalysis occurs at the interface between a solid catalyst and the reactants. The structure of metal catalyst nanoparticles at the metal-gas interface is a key factor that determines catalytic selectivity and activity. Here we report that second-generation nanoclusters are formed on the initial catalyst nanoparticles as a result of interaction with the reactant molecules when the nanoparticles are in a gas phase at Torr pressure or higher. The formation of the second-generation nanoclusters is manifested by a decrease of the average coordination number of the metal atoms and a shift of their core level energies in the presence of gases. The formation of second-generation nanoclusters increases the number of undercoordinated sites, which are the most active for catalysis in many cases.
多相催化发生在固体催化剂和反应物之间的界面上。金属催化剂纳米粒子在金属-气体界面上的结构是决定催化选择性和活性的关键因素。在这里,我们报道了当纳米粒子在托或更高的气压的气相中时,由于与反应物分子的相互作用,在初始催化剂纳米粒子上形成了第二代纳米团簇。第二代纳米团簇的形成表现为金属原子的平均配位数的降低,以及它们的芯能级能量在存在气体时的偏移。第二代纳米团簇的形成增加了低配位数的位点数,在许多情况下,这些位点数是催化反应最活跃的。