Graphene-based phase change composites hold significant potential for solar energy utilization, but their poor thermal conductivity hinders their practical applications. In this work, an air-dried graphene skeleton (AGS) with excellent thermal conductivity enhancement efficiency was constructed by the ice templating method and syneresis, and the air-dried graphene phase change composite (AGP) was subsequently obtained through vacuum-impregnating n-Docosane (C22) into AGS. The syneresis effectively reduced the phonon scattering between graphene sheets within AGS and increased the density of AGS to 0.1701 g/cm³. Therefore, with a graphene skeleton loading of 23.82 wt.%, AGP exhibited excellent thermal conductivity of 9.867 W/(m K), outstanding electrical conductivity of 68.08 S/cm, and remarkable shape stability. Additionally, AGP demonstrated a melting enthalpy of 188.5 J/g and an outstanding solar-thermal conversion efficiency of 93.98%, showing enormous potential for the utilization of solar energy.
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