Highly thermally conductive, electrically insulating, and flexible nanocellulose composite films are crucially significant for the thermal management of next-generation green electronics. However, the intrinsic hygroscopicity of nanocellulose poses a daunting challenge to the reliability and structural stability of electronic products. To address these issues, herein, a dual bio-inspired design was innovatively introduced to fabricate highly thermally conductive and superhydrophobic nanocellulose-based composite films via vacuum-assisted self-assembly of cellulose nanofibers (CNFs) and hydroxylated boron nitride nanosheets (OH-BNNS) and subsequent hydrophobic modification. Driven by the highly orderly hierarchical architecture and a strong hydrogen bonding interaction, the laminated CNF-based composite films with 50 wt % OH-BNNS show a high in-plane thermal conductivity (15.13 W/mK), which results in a 505% enhancement compared with the pure CNF films. On the other hand, the rough surface combined with a low surface energy modifier endows CNF/OH-BNNS composite films with unique superhydrophobicity (contact angle over 155°) and a simultaneous self-cleaning function. Furthermore, the as-fabricated multifunctional CNF/OH-BNNS composite films were designed as a flexible printed circuit board to simulate the potential applications in the field of cooling electronic devices. The development of CNF/OH-BNNS composite films with synergetic properties of high thermal conductivity and superhydrophobicity may shed light on the functional thermal management materials and offer an innovative insight toward fabricating multifunctional nanocomposites via a dual bio-inspired design.
Keywords: bio-inspired; boron nitride nanosheets; cellulose nanofibers; composite films; superhydrophobicity; thermal conductivity.