Ultralight Pt-ALD-modified graphene aerogel achieving aluminum-class thermal resistance at 12% mass

Graphene aerogels (GAs), a class of three-dimensional porous structures, are limited by a fundamental challenge: low thermal conductivity stemming from high interfacial resistance between constituent layers and structural defects. This study systematically investigates a strategy to enhance thermal transport properties by engineering the interlayer bonding via platinum atomic layer deposition (Pt-ALD) and compares it with conventional high-temperature annealing (1873 K). The Pt-ALD-modified graphene aerogel (GA-ALD) exhibited a 199 % increase in thermal conductivity, significantly surpassing the 113 % enhancement from heat treatment. SEM, Raman, XRD, XPS, and FTIR data explicitly indicate that Pt-ALD forms covalent PtOC bonds that bridge adjacent graphene layers while preserving the original porous morphology. Owing to the synergistic effect of enhanced solid-phase thermal conductivity and efficient convective heat transfer through the preserved porous structure, the GA-ALD sample achieved a total thermal resistance comparable to that of an equal-sized aluminum heat sink under identical forced-convection conditions, while weighing only ∼12 % of its aluminum counterpart. Moreover, cyclic compressive tests confirmed GA-ALD durability, retaining 99.5 % height and 94.7 % stress after 1000 cycles. These findings demonstrate that interfacial bond engineering via ALD is a powerful route to ultralight, high-performance carbon aerogels for weight-sensitive thermal-management applications.