Super-compressible and mechanically stable reduced graphene oxide aerogel for wearable functional devices.

The graphene-based aerogels with good electrical conductivity and compressibility have been reported. However, it is challenging to fabricate the graphene aerogel to have excellent mechanical stability for its application in wearable devices. Thus, inspired by macroscale arch-shaped elastic structures and the importance of crosslinking in microstructural stability, we synthesized the mechanically stable reduced graphene oxide aerogels with small elastic modulus by optimizing the reducing agent to make the aligned wrinkled microstructure in which physical crosslinking is dominant. We used L-ascorbic acid, urea, and hydrazine hydrate as reducing agents to synthesize the graphene aerogels rGO-LAA, rGO-Urea, and rGO-HH, respectively. Hydrazine hydrate was found to be best in enhancing the physical and ionic interaction among graphene nanoflakes to achieve a wavy structure with excellent fatigue resistance. Notably, the optimized rGO-HH aerogel maintained structural stability even after 1000 cycles of compression of 50% strain and decompression, showing 98.7% stress retention and 98.1% height retention. We also studied the piezoresistive properties of the rGO-HH aerogel and showed that the rGO-HH-based pressure sensor exhibited excellent sensitivity (~5.7 kPa^-1) with good repeatability. Hence, a super-compressible and mechanically stable piezoresistive material for wearable functional devices was demonstrated by controlling the microstructure and surface chemistry of the reduced graphene oxide aerogel.