Synergistic 2-D cobalt di-tert-butyl phosphate grid graphitic carbon nitride (gC3N4) hybrids for rapid photocatalytic hydrogen evolution

Present day energy demands require greener, cleaner, scalable and high-rate hydrogen production by employing abundant solar energy-driven catalysis. Amongst emerging low cost photocatalysts, graphitic carbon nitrides (gC 3 N 4 ) have emerged as exciting platforms for hydrogen production using sunlight due to their interesting semiconducting properties with the unique band structure. However, the fast electron-hole recombination in g-C 3 N 4 restricts their high performance in producing hydrogen which limits its wider applicability for large scale H 2 production. Synergistic hybridization of gC 3 N 4 with two-dimensional (2D) transition metal organo-phosphates can potentially ensure swift charge transfer, which however has never been realized. Keeping in mind the urgency, we herein report the first demonstration of the synthesis of gC 3 N 4 -2D cobalt di-tert-butyl phosphate bipyridine (gC 3 N 4 -CDTBP) hybrids for facile and enhanced H 2 production under visible light. Further analysis with the transmission electron microscopic imaging (HRTEM), X-ray photoelectron spectroscopy (XPS), and ultraviolet photoelectron spectroscopy (UPS) reveal the inter-layer coupling and bond alignment, confirming the synergistic hybridization between the component layers. This novel hybrid nanosystem achieves a hydrogen evolution rate of 682.4 μmol h -1 g -1 , outperforming state-of-the-art g-C 3 N 4 –based photocatalysts such as CoPi/ g-C 3 N 4 (234 μmol h -1 g -1 ) and cobalt phosphate hydroxide/ g-C 3 N 4 (254 μmol h -1 g -1 ), demonstrating the strong synergistic effect of the 2D–2D CDTBP-g-C 3 N 4 interface. Suppression of exciton recombination in gCDTBP- gC 3 N 4 as compared to pristine gC 3 N 4, and consequent 25-fold enhancement in photoelectric current upon hybridization reveals the swift charge transfer. The findings of the present study highlight the importance of developing advanced hybrid nanocatalysts for scalable hydrogen production. With the push for green energy, scalable hydrogen production using solar-driven catalysis is crucial. Graphitic carbon nitride (gC 3 N 4 ) is a top contender, but fast carrier recombination limits its efficiency. We report the first ambient-condition synthesis of gC 3 N 4 -CDTBP hybrids which exhibited superior visible light photocatalytic activity, with the hydrogen production rate of ∼682.4 μmol/h.g and enhanced photocurrent, outperforming pristine gC 3 N 4 significantly.