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

发表时间:2019-03-09
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论文类型:
期刊论文
第一作者:
Han, Qiuxia
通讯作者:
Duan, CY (reprint author), Dalian Univ Technol, State Key Lab Fine Chem, Dalian 116024, Peoples R China.
合写作者:
Qi, Bo,Ren, Weimin,He, Cheng,Niu, Jingyang,Duan, Chunying
发表时间:
2015-12-01
发表刊物:
NATURE COMMUNICATIONS
收录刊物:
SCIE、PubMed、Scopus
文献类型:
J
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.
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