Efficient thermal transportation in a preferred direction is highly favorable for thermal management issues. The combination of 3D printing and two-dimensional (2D) materials such as graphene, BN, and so on enables infinite possibilities for hierarchically aligned structure programming. In this work, we report the formation of the asymmetrically aligned structure of graphene filled thermoplastic polyurethane (TPU) composites during 3D printing process. The as-printed vertically aligned structure demonstrates a through-plane thermal conductivity (TC) up to 12 W m −1 K −1 at 45 wt % graphene content, which is ∼8 times of that of a horizontally printed structure and surpasses many of the traditional particle reinforced polymer composites. The superior TC is mainly attributed to the anisotropic structure design that benefited from the preferable degree of orientation of graphene and the multiscale dense structure realized by finely controlling the printing parameters. Finite element method (FEM) confirms the essential impact of anisotropic TC design for highly thermal conductive composites. This study provides an effective way to develop 3D printed graphene-based polymer composites for scalable thermal-related applications such as battery thermal management, electric packaging, and so on.

To meet the increasing demands for effective heat management of electronic devices, a graphene-based polymeric composite is considered to be one of the candidate materials owing to the ultrahigh thermal conductivity (TC) of graphene. However, poor graphene dispersion, low quality of exfoliated graphene, and strong phonon scattering at the graphene/matrix interface restrict the heat dissipation ability of graphene-filled composites. Here, a facile and versatile approach to bond graphene foam (GF) with polydimethylsiloxane (PDMS) is proposed, and the corresponding composite with considerable improvement in TC and insulativity is fabricated. First, three-dimensional GF was coated with polydopamine (PDA) via π-π stack and functional groups from PDA reacted with 3-aminopropyltriethoxysilane (APTS). Then, the modified GF was compressed (c-GF) to enhance density and infiltrated with PDMS to get the c-GF/PDA/APTS/PDMS composite. As a result, these processes endow the composite with high TC of in-plane 28.77 W m K and out-of-plane 1.62 W m K at 11.62 wt % GF loading. Besides, the composite manifests obvious improvement in mechanical properties, thermal stability, and insulativity compared to neat PDMS and GF/PDMS composite. An attempt to use the composite for cooling a ceramic heater is found to be successful. Above results open a way for such composites to be applied for the heat management of electronic devices.

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