Applied Catalysis2022,Vol.31212.DOI:10.1016/j.apcatb.2022.121383

Rational synthesis of ruthenium-based metallo-supramolecular polymers as heterogeneous catalysts for catalytic transfer hydrogenation of carbonyl compounds

Gong, Zi-Jie Narayana, Yemineni S. L., V Lin, Yen-Chun Huang, Wei-Hsiang Su, Wei-Nien Li, Yi-Pei Higuchi, Masayoshi Yu, Wen-Yueh
Applied Catalysis2022,Vol.31212.DOI:10.1016/j.apcatb.2022.121383

Rational synthesis of ruthenium-based metallo-supramolecular polymers as heterogeneous catalysts for catalytic transfer hydrogenation of carbonyl compounds

Gong, Zi-Jie 1Narayana, Yemineni S. L., V 2Lin, Yen-Chun 1Huang, Wei-Hsiang 3Su, Wei-Nien 3Li, Yi-Pei 1Higuchi, Masayoshi 2Yu, Wen-Yueh1
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作者信息

  • 1. Natl Taiwan Univ
  • 2. Natl Inst Mat Sci
  • 3. Natl Taiwan Univ Sci & Technol
  • 折叠

Abstract

Ruthenium-based metallo-supramolecular polymers (Ru-MSPs) were synthesized by complexing Ru ions with 1,4-bis(1,10-phenanthrolin-5-yl)benzene ligands for heterogeneously catalytic transfer hydrogenation of carbonyl compounds with formate. The degree of polymerization and the local environment of Ru atoms in RuMSP were tailored by tuning the ligand/metal ratio and the synthesis temperature/period. The coordinativelyunsaturated Ru atoms are identified as the active centers in Ru-MSP for carbonyl reduction. Ru-MSP is much more active than Ru-based counterparts including its monomeric analogue, which is attributed to (1) the higher electron density in Ru atoms that facilitates the selective dehydrogenation of formate via C-H dissociation, and (2) the lower LUMO of ligand moieties that activates the carbonyl oxygen via Lewis acid-base interactions. Furthermore, Ru-MSP displays high reusability and capability of catalyzing a wide scope of carbonyl compounds. These findings demonstrate that the rationally-designed polymerization is a promising approach to heterogenize the catalytically active metal complexes with enhanced performance.

Key words

Metallo-supramolecular polymer/Heterogeneous catalyst/Catalytic transfer hydrogenation/Carbonyl reduction/FORMIC-ACID/POTASSIUM FORMATE/WATER OXIDATION/RU/COMPLEXES/EFFICIENT/NANOPARTICLES/DESIGN/IMMOBILIZATION/COORDINATION

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出版年

2022
Applied Catalysis

Applied Catalysis

ISSN:0926-3373
被引量5
参考文献量65
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