Shuangshuang Wang, Dianying Feng, Zhiming Zhang, Xia Liu, Kunpeng Ruan, Yongqiang Guo* and Junwei Gu. Highly thermally conductive polydimethylsiloxane composites with controllable 3D GO@f-CNTs networks via self-sacrificing template method. Chinese Journal of Polymer Science, 2024, 10.1007/s10118-024-3098-4. 2022IF=4.3.（2區化學期刊，中國科技期刊卓越行動計劃-梯隊期刊類項目）
Abstract
Constructing controllable thermal conduction networks is the key to efficiently improve thermal conductivities of polymer composites. In this work, graphite oxide (GO) and functionalized carbon nanotubes (f-CNTs) are combined to prepare “Line-Plane”-like hetero-structured thermally conductive GO@f-CNTs fillers, which are then performed to construct controllable 3D GO@f-CNTs thermal conduction networks via self-sacrificing template method based on oxalic acid. Subsequently, thermally conductive GO@f-CNTs/polydimethylsiloxane (PDMS) composites are fabricated via casting method. When the size of oxalic acid is 0.24 mm and the volume fraction of GO@f-CNTs is 60 vol%, GO@f-CNTs/PDMS composites present the optimal thermal conductivity coefficient (λ, 4.00 W/(m·K)), about 20 times that of the λ of pure PDMS (0.20 W/(m·K)), also much higher than the λ (2.44 W/(m·K)) of GO/f-CNTs/PDMS composites with the same amount of randomly dispersed fillers. Meanwhile, the obtained GO@f-CNTs/PDMS composites have excellent thermal stability, whose λ deviation is onlyabout 3% after 500 thermal cycles (20~200oC).
可控導熱網絡的構筑是高效提升導熱填料/高分子復合材料導熱性能的關鍵。本文以氧化石墨（GO）和改性碳納米管（f-CNTs）構筑的“線-面”狀異質結構GO@f-CNTs為導熱填料，借助草酸為自犧牲模板構筑結構完整、形貌可控的GO@f-CNTs導熱網絡，經澆注聚二甲基硅氧烷（PDMS）制備GO@f-CNTs/PDMS導熱復合材料。結果表明，當草酸粒徑為0.24 mm且GO@f-CNTs體積分數為60 vol%時，GO@f-CNTs/PDMS導熱復合材料具有最優的導熱系數（λ，4.00 W/(m·K)），約為純PDMS的λ（0.20 W/(m·K)）的20倍，也遠高于同等GO和f-CNTs用量隨機分散的GO/f-CNTs/PDMS導熱復合材料的λ（2.44 W/(m·K)）。GO@f-CNTs/PDMS導熱復合材料兼具優異的導熱穩定性，經500次熱循環（20~200oC）后其λ的偏差約為3%。
論文亮點
1. 以草酸為自犧牲模板將化學接枝法制備的GO@f-CNTs異質結構導熱填料構筑成結構完整、形貌可控的三維GO@f-CNTs導熱網絡。
2. 當草酸粒徑為0.24 mm且GO@f-CNTs體積分數為60 vol%時，GO@f-CNTs/PDMS導熱復合材料具有最優的導熱系數（λ，4.00 W/(m·K)），遠高于同等GO和f-CNTs用量隨機分散的GO/f-CNTs/PDMS導熱復合材料的λ（2.44 W/(m·K)）。
3. GO@f-CNTs/PDMS導熱復合材料的微觀熱傳導有限元模擬揭示了粒徑為0.24 mm的草酸構筑的GO@f-CNTs導熱網絡具有最佳的熱傳導效率。
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