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The effect of electrostatic field on the catalytic properties of platinum clusters confined in zeolite for hydrogenation

机译：静电场对催化的影响白金集群在的属性沸石对加氢

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摘要

The electrostatic field of a dielectric cavity is powerful for modulating many aspects of confined metal clusters. Here we report that the catalytic properties of Pt-n clusters confined in X-zeolite cages are strongly tuned by altering the zeolitic field, which is achieved by using different cations (Na+, Cs+, Ca2+ or La3+) to balance the negative framework of the zeolite. Compared with Pt-n@LaX, for example, Pt-n@CsX shows a surprising approximate to 5500% enhancement in TOF value for phenol hydrogenation to cyclohexanol. Electrostatic field modulation leads to gradual changes of electronic properties such as the Fermi levels/d-band centers of the Pt-n clusters, as revealed by DFT calculations and experimental characterizations. The decreases in Fermi levels of the Pt-n clusters benefit the hydrogenation of -C?CH groups (phenylacetylene and acetylene) and -NO2 groups (nitrobenzene, o-nitroanisole and o-chloronitrobenzene) but are detrimental for aromatic ring hydrogenation (phenol). These findings are important for the design of high performance catalysts.
机译：静电场的介质腔强大的调制的许多方面的限制金属集群。关在X-zeolite Pt-n集群的属性笼子里改变沸石的强烈关注场,这是通过使用不同的实现阳离子(Na + Cs + Ca2 +或La3 +)平衡负面框架的沸石。例如,Pt-n@LaX Pt-n@CsX显示了令人惊讶的近似增强5500%苯酚加氢TOF值环己醇。导致逐步变化的电子性质如费米水平/ d带中心的Pt-n集群,揭示了DFT计算和实验特征。在费米水平Pt-n集群效益加氢- c ?和乙炔)和no2组(硝基苯,o-nitroanisole和o-chloronitrobenzene)有害的芳环加氢(苯酚)。设计高性能的催化剂。

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