Pyrimidine-assisted synthesis of S, N-codoped few-layered graphene for highly efficient hydrogen peroxide production in acid

H2O2 production by electroreduction of oxygen is an attractive alternative to replace the current complex anthraquinone method. However, it is still challenging to realize efficient electrochemical H2O2 production in acid by using cost- effective catalysts. Herein, we report a pyrimidine-assisted chemical-vapor-deposition method to synthesize sulfur-and-nitrogen-codoped few-layered graphene (SNGL) with exceptional activity and selectivity for two-electron oxygen reduction reaction (2e(-) ORR) in acidic electrolyte ( pH = 1). The H2O2 selectivity reaches 90%-100% over a potential range of 0.200.55 V, and the maximum H2O2 production rate (4.8 mol g (-1)h(-1)) exceeds all of the reported H2O2 production performance for carbon-material-based catalysts. Experiments and density functional theory (DFT) simulations reveal that the synergy effect of the combined oxidized sulfur and pyridinic N functional motif can lower the Fermi level of valence electronic states of active edge carbon sites and thus leads to suitable binding strength of *OOH intermediate for high selectivity and performance 2e(-) ORR for H2O2 formation.

Automated summary

Sulfur-and-nitrogen-codoped few-layered graphene synthesized by a pyrimidine-assisted chemical-vapor-deposition method exhibits exceptional activity and selectivity for two-electron oxygen reduction reaction (2e(-) ORR) in acidic electrolyte, leading to efficient production of H2O2.