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phosphine-built-in Porous Organic Cage Supported Ultrafine Pd Nanoclusters Enable Highly Efficient and Regioselective Hydrogenation of Epoxides

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CCS Chemistry 2024年第10期6卷 2476-2488页

作者： Xin Zhou Zhaozhan Wang Zhe-Ning Chen Yong Yang CAS Key Laboratory of Bio-Based Materials Qingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of SciencesQingdao 266101 Shandong Energy Institute Qingdao 266101 College of Environment and Safety Engineering Qingdao University of Science and TechnologyQingdao 266101 State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002 University of Chinese Academy of Sciences Beijing 100049 Fujian Provincial Key Laboratory of Theoretical and Computational Chemistry Xiamen UniversityXiamen 361005

Selective hydrogenation of epoxides has been regarded as an atom-economical and straightforward method for the synthesis of ***,it remains a big challenge in the precise control of *** date,the reaction enabled by a reusable and high-performance heterogeneous catalyst with excellent regioselectivity is very ***,we develop highly loaded and ultrafine Pd nanoclusters(NCs)encapsulated on a phosphinebuilt-in porous organic cage(FPPOC)for the catalytic hydrogenation of epoxides by molecular *** from the unique characters of uniform dispersion and strong interaction between Pd NCs and FPPOC,the resultant Pd NCs exhibited superior catalytic activity and excellent regioselectivity for the hydrogenation of epoxides under milder conditions.A diverse set of terminal and internal epoxides was efficiently reduced to the corresponding linear or branched alcohols in an extremely regioselective manner,well tolerating diverse functional ***,the catalyst demonstrates high stability and could be reused up to 10 times with marginal decay in activity and ***,the catalyst is applicable for scale-up synthesis with a record turnover number as high as 16,111,to the best of our knowledge,outperforming those previous state-of-the-art *** experiments and characterizations in combination with density functional theory calculations provide insight into the superior activity and excellent regioselectivity.

关键词： porous organic cage phosphine-built-in palladium nanoclusters regioselective hydrogenation epoxides

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