Transparent and Stretchable Graphene Electrode by Intercalation Doping for Epidermal Electrophysiology

Epidermal electronics is regarded as the next-generation technology, and graphene is a promising electrode, which is a key building block of such devices. However, graphene has a tendency to crack at small strains with a rapidly increased resistance upon stretching. Here, to enable graphene applicable in epidermal electronics, we designed a novel graphene structure that is molybdenum chloride (MoCl5)-intercalated few-layer graphene (Mo-FLG) fabricated in a confined environment. In the case of bilayer graphene (BLG), MoCl5-intercalated bilayer graphene (Mo-BLG) exhibited a low sheet resistance of 40 Ω/square (sq) at a transmittance of 80%. Due to the self-barrier doping effect, the sheet resistance increased to only 60 Ω/sq after exposing to the atmosphere over 1 month. Transferred onto elastomer substrates, Mo-BLG can work as an electrode up to 80% strain and maintain a high conductivity that is durable over 2000 cycles at 30% strain. This mechano-electrostability is attributed to the special intercalated structure where the intercalated dopants act as lubricants to weaken the layer–layer interaction and allow a certain degree of sliding, as well as electrical crack-connectors to bridge the cracked domains at a high strain. Mo-BLG can be applied as epidermal electrodes to monitor electrophysiological signals such as electrocardiogram (ECG), electrooculogram (EOG), electroencephalography (EEG), and surface electromyogram (sEMG) with high signal-to-noise ratios (SNRs) comparable to commercial Ag/AgCl electrode. This is the first demonstration of epidermal electrodes based on intercalation-doped graphene applied in health monitoring, shedding light on the future development of graphene-based epidermal electronics.