Enhanced Fuel Cell Performance Using Ultrafast, Out-of-Plane Proton-Conducting, 3D Graphene Oxide as an Electrolyte

Despite the considerable in-plane proton conductivity of graphene oxide (GO) nanosheets, inadequate single-cell performance in a polymer exchange membrane fuel cell (PEMFC) occurred on incorporating a vacuum-filtration-prepared GO membrane between the electrodes. In particular, the proton transfer between the electrodes in the PEMFC single cell is in the out-of-plane direction of the GO membrane and was found to be significantly lower than for the in-plane direction due to the presence of proton conduction barriers arising from turbostratic stacking of the GO layers. Therefore, the structural transformation of GO nanosheets into an ultrafast, out-of-plane proton conductor is key to boosting GO-based PEMFC performance. Here, we report the use of a freeze-dried route to three-dimensional (3D) graphene oxide (3DGO) exhibiting a 3D interconnected network and significant interlayer void space. The out-of-plane direction proton conductivity of 3DGO was calculated to be 3.5 × 10–2 S cm–1 at 343 K and 100% relative humidity (RH), which is about 175 times higher than that for the GO membrane. The 3DGO was incorporated as a solid electrolyte in a PEMFC single cell, and a maximum power density of 60.2 mW cm–2 was obtained at 30 °C. This high proton conductivity and PEMFC performance of the 3DGO are correlated with the facile proton conduction pathway and higher water uptake in the 3D porous architecture of 3DGO.