Emerging biocomposites with excellent heat dissipation capabilities and inherent sustainability are urgently needed to address the cooling issues of modern electronics and growing environmental concerns. However, the moisture stability, mechanical performance, thermal conductivity, and even flame retardancy of biomass-based materials are generally insufficient for practical thermal management applications. Herein, we present a high-performance graphene biocomposite consisting of carboxylated cellulose nanofibers and graphene nanosheets through an evaporation-induced self-assembly and subsequent Fe3+ cross-linking strategy. The Fe3+ coordination plays a critical role in stabilizing the material structure, thereby improving the mechanical strength and water stability of the biocomposite films, and its effect is revealed by density functional theory calculations. The hierarchical structure of the biocomposite films also leads to a high in-plane thermal conductivity of 42.5 W m-1 K-1, enabling a superior heat transfer performance. Furthermore, the resultant biocomposite films exhibit outstanding Joule heating performance with a fast thermal response and long-term stability, improved thermal stability, and flame retardancy. Therefore, such a general strategy and the desired overall properties of the biocomposite films offer wide application prospects for functional and safe thermal management.
Keywords: biocomposites; cellulose nanofibers; graphene; thermal conductivity; thermal management.