Strongly anisotropic thermal conductivity and adequate breathability of bilayered films for heat management of on-skin electronics

Thin-film wearable electronics are required to be directly laminated on to human skin for reliable, sensitive bio-sensing but with minimal irritation to the user after long-time use. Excellent heat management films with strongly anisotropic thermal conductivity (K) and adequate breathability are increasingly desirable for shielding the skin from heating while allowing the skin to breathe properly. Here, interfacial self-assembly of a graphene oxide (GO) film covering an ambient-dried bacterial cellulose aerogel (AD-BCA) film followed by laser reduction was proposed to prepare laser-reduced GO (L-rGO)/AD-BCA bilayered films. The AD-BCA substrate provides low cross-plane K (K ⊥ ≈ 0.052 W mK−1), high breathability, and high compressive and tensile resistance by 'partially' inheriting the pore structure from bacterial cellulose (BC) gel. The introduction of an upper L-rGO film, which is only 0.31 wt% content, dramatically increases the in-plane K (K // ) from 0.3 W mK−1 in AD-BCA to 10.72 W mK−1 owing to the highly in-plane oriented, continuous, uniform assembling geometry of the GO film; while K ⊥ decreases to a lower value of 0.033 W mK−1, mainly owing to the air pockets between L-rGO multilayers caused by the laser reduction. The bilayered films achieve a K // /K ⊥ of 325, which is substantially larger even than that of graphite and similar polymer composites. They permit high transmission rates for water vapor (416.78 g/m2/day, >204 g/m2/day of normal skin) and O2 (449.35 cm3/m2/day). The combination of strongly anisotropic thermal conductivity and adequate breathability facilitates applications in heat management in on-skin electronics.