3D-printed graphene skeletons for highly-efficient thermal conductivity enhancement and superior compressibility of thermal interface composites

Abstract

Enhancing thermal conductivity of polymer-based composites while maintaining high compressibility remains a critical challenge in developing high-performance thermal interface materials (TIMs). In this study, we constructed multi-scale porous graphene skeletons using a 3D printing technique and subsequently infiltrated them with polydimethylsiloxane (PDMS) to first fabricate 3D-printed graphene/PDMS composites. The obtained composites achieved thermal conductivity of 0.83 W/m·K at a graphene loading of only 2.75 wt%, corresponding to an impressive thermal conductivity enhancement efficiency of 195 %. These results demonstrate the remarkable effectiveness of the 3D-printed graphene skeleton in greatly improving thermal conductivity at extremely low filler loadings. Furthermore, the composites exhibited excellent compressibility, with low compressive modulus of 0.42 MPa. These superior performances are attributed to the continuous heat transfer pathways, highly-integrated skeleton, low interfacial thermal resistance, and multi-scale porous structures of the skeleton. This work provides a novel strategy for fabricating high-performance TIMs with integrated structural and multifunctional properties.