Shape Memory Multidimensional Microsphere Network for Thermal Energy Storage and Intelligent Sensing

Phase change materials (PCMs) exhibit high energy density, reversibility, and broad temperature selectivity. Unfortunately, the inherent trade-off between functionality and mechanical strength inevitably arises during application, necessitating the breakthrough of the thermal-mechanical-functional coupling bottleneck to establish an efficient thermal storage system. This work innovatively designs a multi-dimensional composite PCMs based on supramolecular polymers and graphene-encapsulated paraffin microspheres, achieving cross-scale synergy between thermal conduction networks, energy storage units, mechanical support structures, and functional design. The multi-level strong-weak hydrogen bond interactions within the supramolecular construct a physically cross-linked framework that combines toughness and stability, while paraffin-graphene microspheres enhance energy storage density. The three-dimensional thermally conductive and electrically conductive framework endows PCMs with photo/electro-thermal energy conversion and response capabilities. Simultaneously achieving high phase change enthalpy (190.2 J g −1 ), ultra-low leakage rate (<0.47 wt%), and high strength ranging from 16.0 to 29.6 MPa, with programmable shape memory and recyclable molding capabilities, overcoming the bottleneck of synergistically suppressing thermal hysteresis and mechanical fatigue in PCMs. Further construction of intelligent temperature sensing arrays enables interaction between high and low-temperature environments. This work proposes a feasible strategy to promote the evolution of PCMs from passive thermal storage media to embodied intelligent components.