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Simulating molecular structures and dynamic behaviors offers critical insights into the microscopic mechanisms governing variations in charge transport properties. In this work, molecular dynamics (MD) simulations integrated with the Compass II force field and molecular modeling (including geometry optimization, annealing, and dynamic equilibration) were systematically conducted to analyze intermolecular interaction energy, free volume distribution, electronic density of states (DOS), charge differential density, and trap energy levels. This comprehensive approach aims to unravel the regulatory role of hydrogen bonds in the structural evolution and charge transport dynamics of polypropylene (PP)/polyvinylidene fluoride (PVDF) composite systems. A quantitative framework was further established to correlate hydrogen bond density with key material performance metrics, such as free volume fraction, bandgap energy, and trap energy depth. This elucidates the hydrogen bond-mediated modulation of molecular architecture and charge transport behavior in PP/PVDF composites. Simulation results reveal a pronounced dependence of hydrogen bond formation on MA grafting content. At an MA mass fraction of 36.22wt.%, the hydrogen bond count reaches a maximum of 20, coinciding with a peak intermolecular interaction energy of 2171.63kcal·mol-1 and a minimized free volume fraction of 16.03%, indicative of a highly compact molecular packing structure and further increasing the MA content to 52.97wt.% induces a notable reduction in the composite’s bandgap to 3.13eV (minimum) and a concurrent deepening of trap energy levels to 3.06eV (maximum). Spatial charge differential density analysis demonstrates enhanced electron density localization near hydrogen-bonded regions, suppressing electron escape probability by over 40% compared to non-bonded domains. These findings collectively highlight a dual mechanism: hydrogen bonds not only reconfigure the molecular topology but also reshape localized charge distribution, directly impeding carrier mobility and altering charge transport pathways. The findings establish a robust structure-property relationship, demonstrating that hydrogen bond engineering serves as a pivotal strategy to tailor dielectric performance in polymer composites. By optimizing hydrogen bond density, the trade-off between structural compactness and electronic confinement can be strategically balanced, enabling the design of PP-based dielectrics with low carbon footprints and superior insulating properties. This mechanistic understanding provides actionable guidelines for advancing high-performance insulating materials in energy storage systems, aerospace components, and next-generation electrical devices, where precise control over charge transport is paramount.
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Keywords:
- polypropylene /
- hydrogen bond /
- molecular dynamics /
- charge transport
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