Efficient, Robust, and Flame-Retardant Electrothermal Coatings Based on a Polyhedral Oligomeric Silsesquioxane-Functionalized Graphene/Multiwalled Carbon Nanotube Hybrid with a Dually Cross-Linking Structure

Graphene electrothermal coatings have attracted considerable attention in recent years due to their important application prospects in a broad range of areas. So far, lots of strategies have been explored for producing them. However, these strategies usually involve a complicated process with sophisticated conditions, limiting their scalable applications. Herein, we demonstrate a facile strategy for preparing efficient, robust, and flame-retardant electrothermal coatings from liquid-phase exfoliated graphene, by combining with multiwalled carbon nanotubes (MWCNTs) and polyhedral oligomeric silsesquioxane (POSS) nanoparticles. This relies on the use of a hyperbranched polyethylene copolymer that simultaneously bears UV-reactive moieties and POSS terminal groups. As a stabilizer, the copolymer can effectively promote the exfoliation of both graphite and MWCNTs in common organic solvents under sonication, rendering the POSS-functionalized graphene and MWCNTs well dispersible in the solvent. From their dispersions, POSS-functionalized graphene/MWCNT hybrid electrothermal coatings have been successfully prepared simply by vacuum filtration and UV irradiation under mild conditions. It has been confirmed that a dually cross-linking structure can be formed in the hybrid system. This significantly improves the thermal resistance of resultant coatings, which remain exhibiting a stable work state even at a temperature high as 280 °C without the occurrence of flammation. Meanwhile, this also endows them with excellent electrothermal performance and service stability. At a relatively low voltage, 15 V, the steady temperature can reach 188.4 °C, with a response time < 30 s; after being alternately folded for 2700 cycles or scraped 200 times, the coating still maintains a stable state. In particular, the process involved is relatively simple with mild conditions. With these features, the coatings obtained herein may find their important applications in the area of wearable devices and household heating systems.