Reaction mechanisms of graphene oxide chemical reduction by sulfur-containing compounds

We used density functional theory to study the reaction mechanisms of chemical reduction of graphene oxide (GO) by the sulfur-containing compounds HSO3− and H2SO3. We studied the reaction energy profiles for the following reactions: dehydroxylation of GO with one and two hydroxyl groups, de-epoxidation of GO with one or two epoxy groups and decarboxylation and decarbonylation of GO with carboxyl and carbonyl groups. We found that hydroxyl and epoxide groups could be easily reduced because of the lower energy barriers, whereas decarboxylation and decarbonylation reactions are not kinetically and thermodynamically easy because of the higher energy barriers. These reaction mechanisms at the atomistic level are not only supported by Chen’s experimental results [J. Phys. Chem. C 2010, 114, 19885], but are also beneficial for the development of new agents that could efficiently reduce GO.