Interfacial Coordination Interaction Enables Soft Elastomer Composites High Thermal Conductivity and High Toughness

Soft elastomers have attracted wide applications, such as soft electronic devices and soft robotics, due to their ability to undergo large deformation with a small external force. Most elastomers suffer from poor toughness and thermal conductivity, which limits their use. The addition of inorganic fillers can enhance the thermal conductivity and toughness, but it deteriorates the softness (low Young's modulus and high stretchability). Integrating thermal conductivity, toughness, and softness into one elastomer is still a challenge. Here, we report a strategy of interfacial coordination interaction to achieve soft elastomer composites with high thermal conductivity and high toughness. We demonstrate the strategy by using poly(lipoic acid) elastomer and silver-coated aluminum filler as model, where silver-sulfur coordination cross-links are formed at the interface. The resultant elastomer composite shows high streachability (450%), high thermal conductivity (2.35 W m^-1 K^-1), low modulus (321 kPa), and high toughness (3496 J m^-2), which cannot be achieve in existing elastomers. The time domain thermoreflectance technique demonstrates that the silver-sulfur coordination interaction lowers the interfacial thermal resistance, resulting in enhanced thermal conductivity of the elastomer composites. The excellent softness stems from lower bonding energy of the silver-sulfur coordination cross-links compared with covalent chemical cross-links. The high toughness also benefits from the interfacial silver-sulfur coordination interaction that can dissipate more energy upon deformation. We further demonstrate the potential application of the thermally conductive, tough, and soft elastomer composites for thermal management of chip and soft electronic devices.