Theoretical insight on transition metal cluster-loaded crystalline carbon nitride for hydrogen evolution reactions

Increasing the active sites upon single-atom catalysts is an optional strategy to increase the catalyst efficiency. In this study, the loading of three and four Group VIII and Group IB transition metal (TM) atoms on poly(triazine imide) (PTI) nanosheets was firstly explored. Meanwhile, comprehensive first-principles investigations were carried out to explore their structural stability, electronic properties, and catalytic performances in the context of the hydrogen evolution reaction (HER). Our results indicate that 11 catalysts are suitable candidates for HER applicability among the total 38 catalysts. Notably, the 4TM@H-PTI catalysts have more active sites than 3TM@H-PTI and show more effective electron transfer with the substrate. Consequently, the 4TM@H-PTI catalysts can be regarded as novel and highly prospective candidates for HER applications. The present work provides valuable insights and paves the way for the design of co-catalysts on PTI that are both low-cost and high-performance, potentially creating novel opportunities for progress within the realm of photocatalysis and sustainable energy.