Exploring the potential of graphene oxide as a functional material to produce hydrocarbons via photocatalysis: Theory meets experiment

A systematic theoretical study on graphene oxide model systems was performed with Density Functional Theory (DFT), and supported by experimental evidence. The results revealed that graphene is highly susceptible to be decorated with organic functional groups, which induced the formation of a band gap, and the rising of a novel semiconducting character. This novel property was used to explore the possible photocatalytic potential in the model systems under study. That is, we evaluated work functions to theoretically obtain the energies of the valence band maximum and the conduction band minimum with respect to the normal hydrogen electrode potential. The assessment of UV-vis profile via Time-dependent DFT also showed the potential of the model systems to efficiently absorb sun light irradiation under photocatalytic conditions. Moreover, the results showed that it is possible to tune the photocatalytic potential of the graphene oxide models under study by interchanging the functional groups anchored on the graphene surface, and their corresponding contents ratio. Experimental evidence obtained via the measurement of optoelectronic properties, revealed that it is possible to classify a graphene oxide powder into one of the model systems under study, while a photocatalytic procedure performed in our laboratory, showed the facile photoreduction of formic acid into methanol with such a graphene oxide. Consequently, the prediction of the electronic structure properties is expected. This may represent a tool to design materials based on graphene oxide to be implemented in reactors for photocatalytic applications.