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Research Article

Precise immobilization of metal single atoms into a porphyrinic metal-organic framework for an efficient alkene hydrosilylation

Chun-Ying Chen,§Qi-Jie Mo,§Fu-Zhen LiHai-Li SongLi Zhang( )
MOE Laboratory of Bioinorganic and Synthetic Chemistry, Lehn Institute of Functional Materials, School of Chemistry, Sun Yat-Sen University, Guangzhou 510006, China

§ Chun-Ying Chen and Qi-Jie Mo contributed equally to this work.

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Graphical Abstract

A platinum single atom based porphyrinic metal-organic framework composite (Pt-SAs@PCN-222) (PCN = porous coordination network) was prepared and acted as an efficient catalyst for alkene hydrosilylation, in which the precise immobilization of metal single atoms and the synergistic effects of the catalytically active site Pt-SAs and the porous support PCN-222 played important roles on the catalytic efficiency.

Abstract

Alkene hydrosilylation is one of the most concise and atom-economical methods to synthesize organosilicon molecules. Herein, we reported the precise immobilization of metal single atoms (M-SAs; M = Ru, Rh, Ir, Pd, Pt, and Au) into a porphyrinic metal-organic framework (MOF) of PCN-222 (PCN = porous coordination network), and then applied the resultant MOF composites of M-SAs@PCN-222 to alkene hydrosilylation. Under solvent-free conditions, Pt-SAs@PCN-222 displayed an especially high catalytic efficiency with the turnover frequency up to 119 s−1 and the maximum turnover number of 906,250 at room temperature. Experimental and theoretical studies revealed that there existed strong interactions between Pt-SAs@PCN-222 and the substrates, which helped to condense the substrates in the cavities of the porous catalysts. Further density functional theory calculations and molecular dynamics simulations disclosed that PCN-222 could transfer electrons to Pt-SAs to enhance the silane oxidative addition and drive the reaction to proceed smoothly via Chalk–Harrod pathway.

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Nano Research
Pages 5914-5921
Cite this article:
Chen C-Y, Mo Q-J, Li F-Z, et al. Precise immobilization of metal single atoms into a porphyrinic metal-organic framework for an efficient alkene hydrosilylation. Nano Research, 2024, 17(7): 5914-5921. https://doi.org/10.1007/s12274-024-6580-y
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Received: 12 December 2023
Revised: 31 January 2024
Accepted: 16 February 2024
Published: 11 April 2024
© Tsinghua University Press 2024
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