Investigation of the Stability and Hydrogen Evolution Activity of Dual-Atom Catalysts on Nitrogen-Doped Graphene

Single atom catalysts (SACs) have received a lot of attention in recent years for their high catalytic activity, selectivity, and atomic utilization rates. Two-dimensional N-doped graphene has been widely used to stabilize transition metal (TM) SACs in many reactions. However, the anchored SAC could lose its activity because of the too strong metal-N interaction. Alternatively, we studied the stability and activity of dual-atom catalysts (DACs) for 24 TMs on N-doped graphene, which kept the dispersion state but had different electronic structures from SACs. Our results show that seven DACs can be formed directly compared to the SACs. The others can form stably when the number of TMs is slightly larger than the number of vacancies. We further show that some of the DACs present better catalytic activities in hydrogen evolution reaction (HER) than the corresponding SACs, which can be attributed to the optimal charge transfer that is tuned by the additional atom. After the screening, the DAC of Re is identified as the most promising catalyst for HER. This study provides useful information for designing atomically-dispersed catalysts on N-doped graphene beyond SACs.