Attributed to the intense development and complexity in electronic devices, energy dissipation is becoming more essential nowadays. The carbonaceous materials particularly graphene (Gr)-based thermal interface materials (TIMs) are exceptional in heat management. However, because of the anisotropic behavior of Gr in composites, the TIMs having outstanding through-plane thermal conductivity (^⊥TC) are needed to fulfill the upcoming innovation in numerous devices. In order to achieve this, herein, nano-urethane linkage-based modified Gr and carbon fibers architecture termed as nanourethane linkage (NUL)-Gr/carbon fibers (CFs) is fabricated. Wherein, toluene diisocyanate is utilized to develop a novel but simple NUL to shape a new interface between graphene sheets. Interestingly, the prepared composite of NUL-Gr/CFs with polyvinylidene fluoride matrix shows outstanding performance in heat management. Owing to the unique structure of NUL-Gr/CFs, an unprecedented value of ^⊥TC (∼ 7.96 W·m⁻¹·K⁻¹) is achieved at a low filler fraction of 13.8 wt.% which translates into an improvement of ∼ 3,980% of pristine polymer. The achieved outcomes elucidate the significance of the covalent interaction between graphene sheets as well as strong bonding among graphene and matrix in the composites and manifest the potential of proposed NUL-Gr/CFs architecture for practical applications.

由于电子设备的迅猛发展和复杂性，如今能源消耗变得越来越重要。碳质材料，特别是基于石墨烯（Gr）的热界面材料（TIMs）在热管理方面表现出色。但是，由于Gr在复合材料中的各向异性行为，TIM具有优异的贯穿面热导率（^⊥需要TC）才能在众多设备中实现即将到来的创新。为了实现这一点，在本文中，制造了被称为纳米氨基甲酸酯键（NUL）-Gr /碳纤维（CFs）的基于纳米氨基甲酸酯键的改性Gr和碳纤维结构。其中，甲苯二异氰酸酯用于开发新颖但简单的NUL，以在石墨烯片之间形成新的界面。有趣的是，制备的NUL-Gr / CFs与聚偏二氟乙烯基质的复合材料在热管理方面表现出出色的性能。由于NUL-Gr / CFs的独特结构，空前的^⊥TC（〜7.96 W·m ^-1 ·K ^-1）是在13.8 wt。％的低填料含量下实现的，这意味着约3,980％的原始聚合物得到了改善。所取得的成果阐明了石墨烯片之间共价相互作用的重要性以及复合材料中石墨烯与基质之间的牢固结合，并表明了拟议的NUL-Gr / CFs体系结构在实际应用中的潜力。