The escalating power density of electronics demands thermal interface materials (TIMs) that simultaneously offer high thermal conductivity, strong adhesion, and environmental sustainability. Conventional thermally conductive adhesives (TCAs) face inherent trade-offs among these properties, often relying on non-recyclable thermosets. Here, we present a sustainable thermoplastic TCA composed of a poly(lipoic acid) (polyLA)-based dynamic polymer matrix integrated with polyvinylpyrrolidone-modified hexagonal boron nitride (BN@PVP). The polyLA matrix incorporates catechol moieties and reversible Fe3+-carboxyl/catechol coordination bonds, creating a dynamically reconfigurable network. This design yields an adhesive (LD50Fe100) with high toughness (1.52 MJ m-3), and strong lap shear adhesion (884 kPa on PMMA and 1210 kPa on steel). The dynamic bonds enable room-temperature self-healing (93.1% efficiency) and robust recyclability. At a BN@PVP loading of 40 wt %, the composite (BN@LD50Fe100) achieves a thermal conductivity of 1.2 W m-1 K-1 while maintaining enhanced mechanical properties. LED chip heat dissipation experiments demonstrate a 4 °C lower operating temperature compared to devices without a TIM, with stable thermal performance over multiple cycles. This work provides a promising material strategy to overcome the traditional trade-offs in TCAs, offering a path toward repairable, reusable, and efficient thermal management solutions for advanced electronic packaging.
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Chen et al. (2026) studied this question.
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