Simultaneously achieving ultrahigh thermal conductivity and enhanced fluidity in Highly-Filled Polymer composites

The development of high-performance thermal conductive materials (TCMs) is fundamentally constrained by the intrinsic conflict between ultrahigh filler loading for thermal conductivity and the processability dictated by viscosity. While acrylate-based TCMs offer stability advantages in optical and silicon-sensitive electronics, their thermal conductivity remains inadequate (< 2 W·m−1·K−1). Herein, a synergistic centrifugation-driven densification strategy is introduced to decouple filler loading from viscosity constraints. This approach combines: (1) molecularly tailored surface modification of multi-scale Al2O3 to minimize interfacial thermal resistance; (2) formulation of a low-viscosity precursor with moderate initial filler loading; (3) controlled centrifugation to spatially concentrate fillers into shear-aligned percolation networks. This method achieves an ultrahigh localized Al2O3 loading of 78.57 vol% while maintaining exceptional macroscopic fluidity (viscosity < 100 Pa·s). The resultant acrylate-based TCM exhibits benchmark-level thermal conductivity of 4.96 W·m−1·K−1, surpassing commercial counterparts by a substantial margin.