期刊
CHINESE JOURNAL OF POLYMER SCIENCE
卷 40, 期 11, 页码 1331-1348出版社
SPRINGER
DOI: 10.1007/s10118-022-2744-y
关键词
Epoxide; Ring-opening copolymerization; Synergistic catalysis; CO2; Stereochemistry control
资金
- National Natural Science Foundation of China [21920102006]
The ring-opening alternating copolymerization processes of epoxides with small-molecule monomers are powerful strategies for preparing polymeric materials with degradable main-chain backbone units. The catalysts selected for these processes play crucial roles in determining reaction rates, productivities, selectivity, regio- and stereochemistry, compositions, and molecular weights. This paper outlines the development of highly active metal catalysts based on synergistic strategies and provides a thorough mechanistic understanding of the copolymerization systems.
The ring-opening alternating copolymerization processes of epoxides with small-molecule monomers, such as carbon dioxide (CO2), carbonyl sulfide (COS) and cyclic anhydrides, are powerful strategies for preparing polymeric materials with degradable carbonate/ester/thiocarbonate main-chain backbone units. The catalysts selected for copolymerization processes play crucial roles in determining their reaction rates and productivities, as well as the selectivity, regio- and stereochemistry, compositions, and the molecular weights of their resultant copolymers. These processes often generate undesirable byproducts such as polyether or ether linkages dispersed randomly within the copolymer's chain, and/or more thermodynamically stable cyclic products. In this account, we outline our efforts of over a dozen years on developing highly active well-defined metal catalysts based on inter- and intra-molecular synergistic strategies to selectively produce completely alternating copolymers from epoxides and various small-molecule monomers. Much attention was paid to the enantioselective resolution copolymerization processes of racemic epoxides via regioselective ring-openings, and the asymmetric copolymerization processes of meso-epoxides with CO2, COS, or cyclic anhydrides via dissymmetrical ring-openings using multichiral catalytic systems, and affording isotactic copolymers with main-chain chirality. In addition, this account provides a thorough mechanistic understanding of the high reactivities, excellent selectivity, and unprecedented stereochemical controls of these copolymerization systems, mediated by inter-and intramolecular synergistic catalysis.
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