Efficient Electronic Modulation of g-C3N4 Photocatalyst by Implanting Atomically Dispersed Ag-1-N-3 for Extremely High Hydrogen Evolution Rates

Developing an efficient method to improve the photocatalytic efficiency of graphitic carbon nitride (g-C-3 N-4) is of great significance for solar H-2 production. Electronic structure modulation has been considered one of the most crucial strategies to improving the photocatalytic efficiency of g-C3N4, but how to efficiently modulate its electronic structure remains a huge challenge. Herein, we, for the first time, report a facile and highly-efficient approach to modulating the electronic structure of g-C3N4 through single Ag atom implantation with a Ag-1-N-3 coordination configuration into the g-C3N4 framework. Due to the remarkably promoted light absorption and notably improved charge separation resulting from efficient electronic structure modulation, the Ag-1-N-3 sites embedded hollow g-C3N4 sphere (Ag1N3-HCNS) shows an unprecedentedly high visible-light photocatalytic H-2 evolution rate (HER) of 17.95mmol g(-1) h(-1) under an atmospheric pressure with a remarkable apparent quantum yield (AQY) of 23.6% at 420 nm. Owing to different test apparatuses and conditions in different literature, neither the absolute HER value nor AQY could be used as a comparative indicator. Generally, times (ts(HER)) regarding the improvement in HER compared to bulk g-C3N4 under the same test apparatus and conditions are presented in the literature. Therefore, the tsHER can be used as an indicator for comparisons of the photocatalytic performance of the developed catalyst. Ag1N3-HCNS shows an unprecedented 193-fold higher HER than bulk g-C3N4 under the same measurement conditions, remarkably outperforming the previously reported g-C3N4 photocatalysts. This work presents a new horizon for designing excellent g-C3N4 photocatalysts through efficient electronic structure modulation of tri-s-triazine by implanting single-atom metals with strong metal-N bonding. [GRAPHICS] .