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<p>This study investigates the evolution of free-radical polymerization under spatially graded conditions by constructing a position-dependent reaction probability model. Given the strong temperature dependence of thermal initiators, spatial temperature variations significantly affect both local monomer reactivity and the macroscopic evolution of polymer structures. Understanding this coupling is crucial for designing gradient-controlled synthesis strategies. The dissipative particle dynamics (DPD) method was employed to investigate free radical polymerization under gradient temperature conditions. Increasing Δ<i>T</i> enhances spatial heterogeneity: high-temperature regions form dense networks with lower molecular weights (<i>M</i><sub>n</sub> and <i>M</i><sub>w</sub>) due to rapid initiation and frequent termination. In contrast, low-temperature regions yield higher molecular weights and expanded chain conformations (&lt;<i>R</i><Stack> <sub>g</sub> <sup>2</sup> </Stack>&gt;) resulting from longer radical lifetimes. These structural differences further govern pore evolution: porosity decreases rapidly and reaches lower final values in high-temperature zones, while low-temperature regions exhibit delayed evolution but higher final porosity. This study demonstrates that the precise control of polymer growth orientation, molecular weight distribution, and porous morphology can be achieved by incorporating gradient conditions, thereby establishing a new paradigm for the targeted synthesis of gradient functional materials.</p>

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Evolutionary Characteristics of Linear Free-radical Polymerization Behavior under Gradient Condition

  • 期刊论文

  • 发表日期：

    2026年7月1日

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  • Hui Li,
  • Bing-Bing Pan,
  • Yi-Yi Zhang,
  • Wen Li,
  • Zi-Jian Xue,
  • Zhen-Bin Chen,
  • Hong Liu

摘要

This study investigates the evolution of free-radical polymerization under spatially graded conditions by constructing a position-dependent reaction probability model. Given the strong temperature dependence of thermal initiators, spatial temperature variations significantly affect both local monomer reactivity and the macroscopic evolution of polymer structures. Understanding this coupling is crucial for designing gradient-controlled synthesis strategies. The dissipative particle dynamics (DPD) method was employed to investigate free radical polymerization under gradient temperature conditions. Increasing ΔT enhances spatial heterogeneity: high-temperature regions form dense networks with lower molecular weights (Mn and Mw) due to rapid initiation and frequent termination. In contrast, low-temperature regions yield higher molecular weights and expanded chain conformations (<R g 2 >) resulting from longer radical lifetimes. These structural differences further govern pore evolution: porosity decreases rapidly and reaches lower final values in high-temperature zones, while low-temperature regions exhibit delayed evolution but higher final porosity. This study demonstrates that the precise control of polymer growth orientation, molecular weight distribution, and porous morphology can be achieved by incorporating gradient conditions, thereby establishing a new paradigm for the targeted synthesis of gradient functional materials.