Application of three-dimensional (3D) carbon framework in phase change material (PCM) has aroused a tremendous interest. However, implementing a high alignment carbon framework with low interfacial thermal resistance (ITR) remain challenging. Herein, we demonstrated a synergetic effect strategy by Ti3C2Tx MXene and graphene nanoplate (GNP) to achieve a 3D thermally conductive framework with high alignment skeleton and low filler-to-filler ITR. Typically, the 3D anisotropic carbon framework is fabricated by unidirectional ice template freezing cellulose nanofibers (CNF)/GNP solution with the assistance of MXene. The abundant functional groups of MXene and the similar layered structure promote the dispersion stability of GNP in CNF aqueous solution, resulting in the significant improvement in GNP alignment and the filler-to-filler ITR. Therefore, the final phase change composites obtained by impregnating polyethylene glycol (PEG) into the framework achieves a satisfactory thermal conductivity (TC) of up to 3.49 W/m K at only 6.25 vol% filler loading. Combining the solar-thermal conversion ability of graphene and MXene, the PCM reveals a rapid energy conversion, transfer and storage capability. More importantly, the phase change enthalpy of the PCM can be as high as 164.3 J/g, with little change even after 50 heating-cooling cycles, and the existence of carbon framework can effectively prevent the leakage phenomenon in solid-liquid conversion process, ensuring its shape stability.
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