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铂单原子与二氧化钛之间强烈的金属-载体相互作用

Strong Metal-Support Interactions between Pt Single Atoms and TiO.

作者信息

Han Bing, Guo Yalin, Huang Yike, Xi Wei, Xu Jie, Luo Jun, Qi Haifeng, Ren Yujing, Liu Xiaoyan, Qiao Botao, Zhang Tao

机构信息

CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.

University of Chinese Academy of Sciences, Beijing, 100049, China.

出版信息

Angew Chem Int Ed Engl. 2020 Jul 13;59(29):11824-11829. doi: 10.1002/anie.202003208. Epub 2020 May 11.

Abstract

Strong metal-support interaction (SMSI) has gained great attention in the field of heterogeneous catalysis. However, whether single-atom catalysts can exhibit SMSI remains unknown. Here, we demonstrate that SMSI can occur on TiO -supported Pt single atoms but at a much higher reduction temperature than that for Pt nanoparticles (NPs). Pt single atoms involved in SMSI are not covered by the TiO support nor do they sink into its subsurface. The suppression of CO adsorption on Pt single atoms stems from coordination saturation (18-electron rule) rather than the physical coverage of Pt atoms by the support. Based on the new finding it is revealed that single atoms are the true active sites in the hydrogenation of 3-nitrostyrene, while Pt NPs barely contribute to the activity since the NP sites are selectively encapsulated. The findings in this work provide a new approach to study the active sites by tuning SMSI.

摘要

强金属-载体相互作用(SMSI)在多相催化领域受到了广泛关注。然而,单原子催化剂是否能表现出SMSI仍不清楚。在此,我们证明了SMSI可以发生在TiO负载的Pt单原子上,但还原温度比Pt纳米颗粒(NPs)高得多。参与SMSI的Pt单原子既没有被TiO载体覆盖,也没有沉入其亚表面。CO在Pt单原子上吸附的抑制源于配位饱和(18电子规则),而不是载体对Pt原子的物理覆盖。基于这一新发现,揭示了单原子是3-硝基苯乙烯加氢反应中的真正活性位点,而Pt NPs对活性的贡献很小,因为NP位点被选择性地包裹了。这项工作中的发现为通过调节SMSI来研究活性位点提供了一种新方法。

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