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<p>The use of renewable bio-based monomers to prepare polyisobutylene-based polymers can not only reduce the dependence on petroleum resources but also promote the green transformation of the cationic polymerization industry. Herein, 2-chloro-2,4,4-trimethylpentane (TMPCl) was synthesized as the main initiator and then cooperated with co-initiator TiCl<sub>4</sub> to construct a cationic initiation system, which was successfully used in preparing poly(isobutylene-<i>co</i>-<i>β</i>-myrcene). The effects of co-initiator concentration, monomer concentration and monomer feed ratio on the copolymerization of isobutylene (IB) and <i>β</i>-myrcene were investigated. The results showed that the molecular weight (M<sub>n</sub>) first increased and then decreased with elevating the concentration of TiCl<sub>4</sub>. When the monomer concentration was 15 wt% and the monomer feed ratio (mole ratio between IB and <i>β</i>-myrcene) was 98:2, an IB-<i>co</i>-<i>β</i>-myrcene random copolymer with a molecular weight of 7.3 × 10<sup>3</sup> g/mol and a lower T<sub>g</sub> (-67.97 ℃) was obtained. According to the <sup>1</sup>H NMR analysis of the polymer structure and terminal groups, it was suggested that IB and <i>β</i>-myrcene mainly formed the copolymer with 1,4 structural unit under this initiation system, thus the cationic polymerization mechanism of IB and <i>β</i>-myrcene was further proposed. This work can provide basic data and theoretical guidance for the manufacture of greener polyisobutylene-based polymers in the future.&#xa0;</p>

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Cationic copolymerization of isobutylene and bio-renewable β-myrcene towards sustainable elastomers: synthesis and mechanism

  • 期刊论文

  • 发表日期：

    2025年2月25日

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  • Yanqing Feng,
  • Penghui Guo,
  • Wei Ding,
  • Yushun Jin,
  • Ruofan Liu,
  • Yibo Wu

摘要

The use of renewable bio-based monomers to prepare polyisobutylene-based polymers can not only reduce the dependence on petroleum resources but also promote the green transformation of the cationic polymerization industry. Herein, 2-chloro-2,4,4-trimethylpentane (TMPCl) was synthesized as the main initiator and then cooperated with co-initiator TiCl4 to construct a cationic initiation system, which was successfully used in preparing poly(isobutylene-co-β-myrcene). The effects of co-initiator concentration, monomer concentration and monomer feed ratio on the copolymerization of isobutylene (IB) and β-myrcene were investigated. The results showed that the molecular weight (Mn) first increased and then decreased with elevating the concentration of TiCl4. When the monomer concentration was 15 wt% and the monomer feed ratio (mole ratio between IB and β-myrcene) was 98:2, an IB-co-β-myrcene random copolymer with a molecular weight of 7.3 × 103 g/mol and a lower Tg (-67.97 ℃) was obtained. According to the 1H NMR analysis of the polymer structure and terminal groups, it was suggested that IB and β-myrcene mainly formed the copolymer with 1,4 structural unit under this initiation system, thus the cationic polymerization mechanism of IB and β-myrcene was further proposed. This work can provide basic data and theoretical guidance for the manufacture of greener polyisobutylene-based polymers in the future.