Crystallization Energetics and Regime Transitions in Graphene-Reinforced Polyethylene/Oligomeric Oxidized Polyethylene Blends: A Lauritzen- Hoffman Analysis
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This study provides a systematic investigation into the isothermal crystallization kinetics and crystallization regime transitions of linear low-density polyethylene (PE) blended with oligomeric oxidized polyethylene (OPE) and reinforced with thermally reduced graphene (TRG) nanosheets. By varying the PE/OPE ratios (100/0, 80/20, and 60/40) and TRG loadings (0.5 to 3 wt%), we demonstrate that OPE and TRG synergistically accelerate crystallization, as evidenced by a marked reduction in crystallization half-time (t 1/2 ). An energetic evaluation via the Hoffman-Lauritzen theory reveals a clear transition from Regime III to Regime I crystallization behavior across the matrix configurations. The fold surface free energy (σ e ) calculated for both regimes reveals that while OPE enhances matrix mobility, the addition of TRG nanosheets functions as a dual-action agent: inducing strong heterogeneous nucleation at low concentrations (0.5 wt% to 1 wt%) while imposing confinement effects at higher loadings (3 wt%). Derived effective activation energies (E a ) confirm that TRG lowers the energetic barrier for molecular folding during crystal growth, offering a tunable pathway to control morphological development in polyolefin nanocomposites.
