Key Lab of Applied Chemistry of Zhejiang Province and Department of Chemistry & Key Lab of Biomass Chemical Engineering of Ministry of Education and College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027, China.
National Center for Magnetic Resonance in Wuhan, State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics and Mathematics, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan, 430071, China.
Nat Commun. 2023 May 3;14(1):2531. doi: 10.1038/s41467-023-38181-6.
Hydroformylation is one of the largest industrially homogeneous processes that strongly relies on catalysts with phosphine ligands such as the Wilkinson's catalyst (triphenylphosphine coordinated Rh). Heterogeneous catalysts for olefin hydroformylation are highly desired but suffer from poor activity compared with homogeneous catalysts. Herein, we demonstrate that rhodium nanoparticles supported on siliceous MFI zeolite with abundant silanol nests are very active for hydroformylation, giving a turnover frequency as high as ~50,000 h that even outperforms the classical Wilkinson's catalyst. Mechanism study reveals that the siliceous zeolite with silanol nests could efficiently enrich olefin molecules to adjacent rhodium nanoparticles, enhancing the hydroformylation reaction.
氢甲酰化反应是工业上最大的均相过程之一，强烈依赖于膦配体的催化剂，如威尔金森催化剂（三苯基膦配位的 Rh）。烯烃氢甲酰化的多相催化剂虽然具有很高的需求，但与均相催化剂相比，活性较差。在此，我们证明了负载在富含硅醇窝的硅质 MFI 沸石上的铑纳米粒子对于氢甲酰化反应具有很高的活性，其转化频率高达~50000 h，甚至超过了经典的威尔金森催化剂。机理研究表明，具有硅醇窝的硅质沸石可以有效地将烯烃分子富集到相邻的铑纳米粒子上，从而增强氢甲酰化反应。
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