Department of Chemical and Biomolecular Engineering, National University of Singapore, 4 Engineering Drive 4, Singapore, 117585, Singapore.
Department of Molecular Engineering, Graduate School of Engineering; Japan and Elements Strategy Initiative for Catalysts & Batteries (ESICB), Kyoto University, Kyotodaigaku Katsura, Nishikyo-ku, Kyoto, 615-8510; 615-8245, Japan.
Angew Chem Int Ed Engl. 2016 Jul 11;55(29):8319-23. doi: 10.1002/anie.201602801. Epub 2016 May 30.
In coordination chemistry, catalytically active metal complexes in a zero- or low-valent state often adopt four-coordinate square-planar or tetrahedral geometry. By applying this principle, we have developed a stable Pt1 single-atom catalyst with a high Pt loading (close to 1 wt %) on phosphomolybdic acid(PMA)-modified active carbon. This was achieved by anchoring Pt on the four-fold hollow sites on PMA. Each Pt atom is stabilized by four oxygen atoms in a distorted square-planar geometry, with Pt slightly protruding from the oxygen planar surface. Pt is positively charged, absorbs hydrogen easily, and exhibits excellent performance in the hydrogenation of nitrobenzene and cyclohexanone. It is likely that the system described here can be extended to a number of stable SACs with superior catalytic activities.
在配位化学中，处于零价或低价态的催化活性金属配合物通常采用四配位的平面正方形或四面体几何构型。基于这一原理，我们开发了一种负载量高（接近 1wt%）的磷钼酸（PMA）改性活性炭负载的稳定的 Pt1 单原子催化剂。该催化剂是通过将 Pt 锚定在 PMA 的四配位空穴位点上实现的。每个 Pt 原子由扭曲的平面正方形结构中的四个氧原子稳定，Pt 略微突出于氧平面表面。Pt 带正电荷，易吸收氢，在硝基苯和环己酮的加氢反应中表现出优异的性能。很可能这里所描述的体系可以扩展到许多具有优越催化活性的稳定 SACs。
