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Abstract
Effecting the synergistic function of single metal atom sites and their supports is of great importance to achieve high-performance catalysts. Herein, we successfully fabricate polyoxometalates (POMs)-stabilized atomically dispersed platinum sites by employing three-dimensional metal-organic frameworks (MOFs) as the finite spatial skeleton to govern the accessible quantity, spatial dispersion, and mobility of metal precursors around each POM unit. The isolated single platinum atoms (Pt1) are steadily anchored in the square-planar sites on the surface of monodispersed Keggin-type phosphomolybdic acid (PMo) in the cavities of various MOFs, including MIL-101, HKUST-1, and ZIF-67. In contrast, either the absence of POMs or MOFs yielded only platinum nanoparticles. Pt1-PMo@MIL-101 are seven times more active than the corresponding nanoparticles in the diboration of phenylacetylene, which can be attributed to the synergistic effect of the preconcentration of organic reaction substrates by porous MOFs skeleton and the decreased desorption energy of products on isolated Pt atom sites.
It is of great significance to exert the synergistic effect between single atom and support. Here, the authors prepare polyoxometalates-stabilized single-atom site catalysts in confined space with enhanced activity for alkynes diboration.
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1 Tsinghua University, Department of Chemistry, Beijing, China (GRID:grid.12527.33) (ISNI:0000 0001 0662 3178); Dalian University of Technology, Zhang Dayu School of Chemistry, Dalian, China (GRID:grid.30055.33) (ISNI:0000 0000 9247 7930)
2 Tsinghua University, Shenzhen Geim Graphene Center and Institute of Materials Research, Tsinghua Shenzhen International Graduate School, Shenzhen, China (GRID:grid.12527.33) (ISNI:0000 0001 0662 3178)
3 Tsinghua University, Department of Chemistry, Beijing, China (GRID:grid.12527.33) (ISNI:0000 0001 0662 3178)
4 Northeast Normal University, Key Laboratory of Polyoxometalate Science of the Ministry of Education, College of Chemistry, Changchun, China (GRID:grid.27446.33) (ISNI:0000 0004 1789 9163)
5 Anhui Normal University, College of Chemistry and Materials Science, Wuhu, China (GRID:grid.440646.4) (ISNI:0000 0004 1760 6105)
6 Chinese Academy of Sciences, Institute of Physics, Beijing, China (GRID:grid.9227.e) (ISNI:0000000119573309)
7 Chinese Academy of Sciences, Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Beijing, China (GRID:grid.9227.e) (ISNI:0000000119573309)