Beehive-Inspired Aerogels with Self-Assembled Phase Change Walls for Thermal Regulation

Conventional phase change materials (PCMs) suffer from leakage and poor stability, driving the demand for advanced thermal regulation systems that combine high energy density, mechanical robustness, and structural integrity. Inspired by honeycomb architecture, we present a bioinspired self-assembly strategy to construct phase change aerogels (PCAs), where solid PCM particles function as both structural and functional units interconnected by minimal polymeric binders. This approach overcomes the intrinsic limitations of traditional “host–guest” and cross-linked polymeric PCMs by enabling direct PCM participation in aerogel network formation. The resulting PCAs exhibit high latent heat (208.1 J g–1), low thermal conductivity (0.1055 W m–1 K–1), excellent mechanical resilience (Young’s modulus of 17.9 MPa), and outstanding recyclability. Interfacial chemistry, binder selection, and the PCM-to-binder ratio prove crucial to forming robust yet flexible networks. This work establishes a new paradigm for high-performance thermal management materials and deepens our understanding of multiscale interfacial engineering in PCMs.