何成

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教授

博士生导师

硕士生导师

性别:男

毕业院校:南京大学

学位:博士

所在单位:化工学院

电子邮箱:hecheng@dlut.edu.cn

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Polyoxometalate-based homochiral metal-organic frameworks for tandem asymmetric transformation of cyclic carbonates from olefins

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论文类型:期刊论文

发表时间:2015-12-01

发表刊物:NATURE COMMUNICATIONS

收录刊物:SCIE、PubMed、Scopus

卷号:6

页面范围:10007

ISSN号:2041-1723

摘要:Currently, great interest is focused on developing auto-tandem catalytic reactions; a substrate is catalytically transferred through mechanistically distinct reactions without altering any reaction conditions. Here by incorporating a pyrrolidine moiety as a chiral organocatalyst and a polyoxometalate as an oxidation catalyst, a powerful approach is devised to achieve a tandem catalyst for the efficient conversion of CO2 into value-added enantiomerically pure cyclic carbonates. The multi-catalytic sites are orderly distributed and spatially matched in the framework. The captured CO2 molecules are synergistically fixed and activated by well-positioned pyrrolidine and amine groups, providing further compatibility with the terminal W = O activated epoxidation intermediate and driving the tandem catalytic process in a single workup stage and an asymmetric fashion. The structural simplicity of the building blocks and the use of inexpensive and readily available chemical reagents render this approach highly promising for the development of practical homochiral materials for CO2 conversion.