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Non-linear Radical Additions-Coupling Polymerization of monovinyl monomers towards Polymer Networks: Theory, Tunability and Heritable Architecture

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Chinese Journal of Polymer Science 2022年第12期40卷 1623-1630,I0008页

作者： Li-Mei Ren Cheng-Lin Li Qi Wang MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science&Engineering Zhejiang UniversityHangzhou 310027China Current address:Zhejiang University-University of Edinburgh Institute Zhejiang University School of Medicineand Key Laboratory of Tissue Engineering and Regenerative Medicine of Zhejiang ProvinceZhejiang University School of MedicineHangzhou 310027China

Exploring new polymerization strategy for current available monomers is a big challenge in polymer science. Here we re-investigate radical polymerization of monovinyl monomer(MVM) initiated by uniform branched polyfunctional initiator(PFI), which is termed non-linear radical additions-coupling polymerization(NLRAs CP). In NLRAs CP, both addition and coupling reactions of radical contribute to the construction of the polymer chains, which leads to continuous growth of branch topology. Theoretical analysis of NLRAs CP predicts that the gelation is determined by the functionality of PFI(a), the extent of initiation of the PFI(q) and the termination factor of radical(φ). NLRAs CPs of styrene and methyl methacrylate promoted by Cu(0)/MeTREN or Mn_(2)(CO)_(10)/visible light were conducted. After the cleavage of incorporated PFI fragment or junctions in the network, the network was transformed to linear chains having almost the same structure as segmental chains in the precursor network. This allows the reverse deducing the network structure from its cleaved products. It has been proven that NLRAs CP includes stepwise initiation of PFI, chain-growth of segmental chains and successive endlinking of macroradicals derived from PFI. The three parameters related to the gelation process, a, q and φ, were adjusted via binary PFI, the feed ratio of [Mn_(2)(CO)_(10)]/[PFI] and addition of non-homopolymerizable comonomer respectively. The minimum values of a and q, and the minimum amount of comonomer required for gelation were determined,which can be applied to estimate φ of various macroradicals. NLRAs CP opens a general and facile strategy for synthesis of a variety of polymer networks with heritable architecture by one-pot polymerization of various MVMs.

关键词： Non-linear radical additions-coupling polymerization monovinyl monomer Polyfunctional initiator Polymer network Theory

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