Electrically Detachable Multifunctional Thermal Interface Materials Based on Pickering Emulsion Architectures

As next-generation electronic devices become increasingly integrated and power-dense, thermal interface materials (TIMs) are essential for efficient heat transfer between heat-generating components and heat spreaders. Although TIM research has primarily focused on enhancing thermal conductivity, practical applications increasingly require interfacial compliance, transient heat buffering, and clean reworkability. Polymer-based TIMs often require high filler loadings; however, excessive filler incorporation reduces interfacial wetting and mechanical recoverability, making stable contact at device interfaces difficult. In addition, most TIMs are difficult to remove cleanly after assembly, limiting repair and recycling.

Here, we propose an ionically detachable multifunctional TIM based on a Pickering emulsion composed of a covalent adaptable network (CAN), phase-change domains, thermally conductive ceramic fillers, and an ionic liquid. During emulsion formation, the fillers selectively localize at the interface between the phase-change domains and the CAN matrix, stabilizing the dispersed phase while forming thermally conductive pathways. The CAN provides mechanical stability and interfacial compliance, whereas the phase-change domains absorb latent heat during phase transition and mitigate transient temperature spikes. The ionic liquid preferentially partitions into the continuous CAN phase, forming ion-conduction pathways.

Upon voltage application, mobile ions migrate and accumulate near the electrode/TIM interface, inducing interfacial polarization and weakening adhesion between the TIM and substrate. This enables electrically triggered detachment without excessive mechanical force. Overall, the proposed TIM combines thermal conduction, phase-change heat buffering, interfacial compliance, and electrically triggered detachability, providing a promising strategy for adaptive and reworkable thermal management materials.