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<p>Polybutene-1 (PB-1) is a semi-crystalline polymer with excellent mechanical properties. However, its practical application is significantly hindered by the slow Form II-I transition, which can take up to several days to complete. While prior research established that long-chain branching (LCB) structures synthesized <i>via ω</i>-alkenylmethyldichlorosilane copolymerization-hydrolysis (ACH) chemistry markedly accelerate this transition, this work demonstrates that H-shaped LCB structures constructed through copolymerization with 1,9-decadiene exhibit the capability to facilitate Form II-I transition in most systems evaluated herein. However, low branching efficiency concurrently generates extended alkyl pendant chains, which impose pronounced steric-hindrance-driven suppression on the transition kinetics, thereby substantially diminishing the net acceleration effect of the LCB structures, even resulting in a net retardation effect in certain systems. Notably, a significant synergistic acceleration effect emerged between the H-shaped LCB structures and propylene comonomer units. These findings confirm that the H-shaped LCB structures play a role in promoting the Form II-I transformation process, which is independent of the synthetic pathways, thereby providing more strategies for addressing the long-standing processing problems of PB-1.</p>

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Acceleration of Form II-I Transition in Polybutene-1 by H-shape Long-chain Branching: Critical Role of 1,9-Decadiene as Branching Agent and Synergy with Comonomer

  • 期刊论文

  • 发表日期：

    2025年11月12日

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  • Hui-Ping Yu,
  • Jin-Yong Dong

摘要

Polybutene-1 (PB-1) is a semi-crystalline polymer with excellent mechanical properties. However, its practical application is significantly hindered by the slow Form II-I transition, which can take up to several days to complete. While prior research established that long-chain branching (LCB) structures synthesized via ω-alkenylmethyldichlorosilane copolymerization-hydrolysis (ACH) chemistry markedly accelerate this transition, this work demonstrates that H-shaped LCB structures constructed through copolymerization with 1,9-decadiene exhibit the capability to facilitate Form II-I transition in most systems evaluated herein. However, low branching efficiency concurrently generates extended alkyl pendant chains, which impose pronounced steric-hindrance-driven suppression on the transition kinetics, thereby substantially diminishing the net acceleration effect of the LCB structures, even resulting in a net retardation effect in certain systems. Notably, a significant synergistic acceleration effect emerged between the H-shaped LCB structures and propylene comonomer units. These findings confirm that the H-shaped LCB structures play a role in promoting the Form II-I transformation process, which is independent of the synthetic pathways, thereby providing more strategies for addressing the long-standing processing problems of PB-1.