4.8 Article

A Topology-Defined Polyester Elastomer from CO2 and 1,3-Butadiene: A One-Pot-One-Step Scrambling Polymerizations Strategy

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 46, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202213028

Keywords

Carbon Dioxide Fixation; Copolymerization; Polyester Elastomer; Ring-Opening Polymerization

Funding

  1. Zhejiang Provincial Natural Science Foundation of China [LZ22B040001]
  2. National Natural Science Foundation of China [21674089, 21871232]
  3. State Key Lab of CAD&CG in Zhejiang University
  4. Key Laboratory of Medical Electronics and Digital Health of Zhejiang Province in Jiaxing University

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We designed and performed a novel strategy to produce polyesters using CO2 and olefins, by individually synthesizing PCL and EVL oligomers through anionic ring-opening polymerization and conjugated addition oligomerization, and then inserting EVL oligomers into PCL by transesterification, resulting in polyesters with tunable topology and composition.
It is significant and challenging to use CO2 to produce polymeric materials, especially with olefins. Here, a novel strategy named scrambling polymerizations is designed and performed for the copolymerization of a CO2-and-1,3-butadiene-derived valerolactone, 3-ethylidene-6-vinyltetrahydro-2H-pyran-2-one (EVL), with epsilon-caprolactone (CL) to prepare polyesters. Anionic ring-opening polymerization of CL and conjugated addition oligomerization of EVL take place individually to form PCL and EVL oligomers, respectively. Then EVL oligomers insert into PCL by transesterification resulting in polyester P(CL-co-EVL) with a tunable topology and composition. The non-cytotoxic and degradable polyester network with elongation at break of >600 % can be used as an elastomer. We propose a method to provide polyester elastomers from CO2 and olefins for the first time, and expand the potential of transformation from sustainable feedstocks to polymeric materials.

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