Study of deep oxidation and sulfonation of graphene oxide as low-temperature fuel cell electrolyte

Abstract In order improve the fuel cell performance of a free-standing graphene oxide (GO) membrane, the impacts of both the additional oxidation of GO and the modification with vinilsulfonic acid were investigated. The modification with vinilsulfonic acid was conducted with and without adding potassium persulfate, K2S2O8, which is a radical initiator for the polymerization of vinylsulfonate. A total of six types of free-standing GO membranes with and without the oxidation and/or the modification were prepared. The oxidation and the modification additively increased the proton conductivity, and the oxidation significantly improved the durability of the fuel cell performance at 30 °C. The membrane of GOhvsi, of which GO was oxidized and modified with the initiator, showed very high in-plane proton conductivities at 30 °C, i.e., 0.54 S cm−1 at RH 100%. The H2–O2 fuel cell using GOhvsi showed maximum power densities as high as 136 mW cm−2 and 184 mW cm−2 at 30 °C and 50 °C, respectively. The performance at 30 °C was stable for more than 20 h. The improved durability by the oxidation was attributed to the increased defects of carbon based on an XPS analysis. The TPD-MS analysis suggested that the oxygenated functional groups at the defects would increase the binding strength.