Soft gels with high toughness have drawn tremendous attention recently due to their potential applications in flexible electronic fields. The miniaturization and high‐power density of electronic devices require soft gels with both high toughness and low thermal resistance; however, it is difficult to achieve these properties simultaneously. Herein, a simple design strategy is reported for constructing soft (high stretchability of 6.91 and low Young's modulus of 340 kPa), tough (4741.48 J m−2) and thermal conductive (low thermal resistance of 0.14 cm2 K W−1, under 10 psi pressure) polydimethylsiloxane/aluminum composite gel. This is realized by precisely lengthening polymer strands between the chemical cross‐linked points and controlling the aluminum content in the composite gels. The symbiosis of this combination involves: lengthening the polymer strands facilitates its unfolding to increase the softness and intrinsic toughness; the thermally conductive spherical aluminum enables low thermal resistance and increases the intrinsic toughness and stress dissipation. By utilizing this gel as a thermal interface material, effective heat dissipation is demonstrated in electronic devices operating under high‐power conditions over numerous cycles. These results demonstrate the application potential of composite gels in meeting the performance maintenance and heat dissipation, which are needed for modern electronic devices.

Thermal conductive polymer-based composites with the combination of superior stretchable, efficient self-healing, recyclable and high thermal conductivity have long been pursued in modern electronics industry. However, integrating these attractive properties...

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.

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Thermal resistance at a soft/hard material interface plays an undisputed role in the development of electronic packaging, sensors, and medicine. Adhesion energy and phonon spectra match are two crucial parameters in determining the interfacial thermal resistance (ITR), but it is difficult to simultaneously achieve these two parameters in one system to reduce the ITR at the soft/hard material interface. Here, we report a design of an elastomer composite consisting of a polyurethane−thioctic acid copolymer and microscale spherical aluminum, which exhibits both high phonon spectra match and high adhesion energy (>1000 J/m 2 ) with hard materials, thus leading to a low ITR of 0.03 mm 2 •K/W. We further develop a quantitative physically based model connecting the adhesion energy and ITR, revealing the key role the adhesion energy plays. This work serves to engineer the ITR at the soft/hard material interface from the aspect of adhesion energy, which will prompt a paradigm shift in the development of interface science.

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Thermal interface materials (TIMs) used between the chip and the heat spreader play an indispensable role in effective heat removal to ensure the chip's performance and reliability. As they suffer from stresses in practical applications, TIMs need to have high toughness to resist fracture. The notch sensitivity of TIMs is considered an important parameter to evaluate its toughness. However, the notch sensitivity of TIMs is seldom mentioned, and the mechanism to enhance the toughness is still unclear. Here, using polymer-based TIMs consisting of polydimethylsiloxane/aluminum as a model, we specifically investigate notch sensitivity of TIMs and analyze the mechanical mechanism in detail from the macroscopic and microscopic scales. It was found that a transition from notch insensitive to notch sensitive will happen with a notch length of 2.0 mm, which is much higher than typical soft materials, such as hydrogels. We interpret the notch sensitivity of the TIM by finite element analysis at macroscopic scales and the Lake–Thomas theory at microcosmic scales. The relationship between the area of the strain concentration region to the notch length in finite element analysis is in good agreement with the fracture stretch ratio with different notch lengths measured in a uniaxial tensile experiment. This investigation gives an insight into designing notch-insensitivity TIM and understanding their fracture behavior.