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In the quest for sustainable and renewable energy sources, researchers and engineers have explored innovative technologies to harvest energy from various environmental sources. Dielectric elastomer generators (DEGs) with high energy harvesting performance have been proven to be promising energy collectors, but achieving a high dielectric constant (ε’) and low electrical conductivity (EC) under high electric fields of dielectric elastomer (DE) simultaneously is a struggle, which poses significant challenges. In this study, high-content carboxyl group-grafted liquid polybutadiene (HCPB) is synthesized and then adopted as an organic dielectric filler to blend and cocross-link with a butadiene rubber (BR) matrix to prepare DE composites with high energy harvesting performance. The introduction of carboxyl groups enhances polarization while trapping free Al3+in the matrix, which revolutionarily achieves a significant increase in ε’ under extremely low EC. Ultimately, the contradiction between increased ε’ and decreased ECunder high electric fields is reconciled, resulting in a 30 HCPB/BR composite with high energy density (w= 91.9 mJ/cm3) and fine power conversion efficiency (PCE= 24.1%). This advancement paves the way for the development of HCPB/BR composite-based DEGs with enhanced ε’ and energy harvesting performance.

The dynamic density functional theory has been applied to investigate diffusion dynamics in polymer nanocomposites under shear conditions. According to the time-dependent density relaxations of the test particle and polymer chains, the particle diffusion mode and polymer flow pattern have been quantitatively determined and examined by the reported experimental and computational data. It is shown that a suitable coupling of particle size and particle–polymer interaction can produce the maximum diffusion resistance. More importantly, shear stress can induce the microscopic structure transition in polymer nanocomposites from homogeneous dispersion to microphase separation or ordered layer arrangement. The influence extent of particle size, particle volume fraction, and particle–polymer interaction on the transition has been identified to find the optimum condition to minimize the damage to the overall structure.