Phosphorous-doped 1T-MoS₂ decorated nitrogen-doped g-C₃N₄ nanosheets for enhanced photocatalytic nitrogen fixation

Herein, we report that the phosphorous-doped 1 T-MoS₂ as co-catalyst decorated nitrogen-doped g-C₃N₄ nanosheets (P-1 T-MoS₂@N-g-C₃N₄) are prepared by the hydrothermal and annealing process. The obtained P-1 T-MoS₂@N-g-C₃N₄ composite presents an enhanced photocatalytic N₂ reduction rate of 689.76 μmol L^-1 g^-1h^-1 in deionized water without sacrificial agent under simulated sunlight irradiation, which is higher than that of pure g-C₃N₄ (265.62 μmol L^-1 g^-1h^-1), 1 T-MoS₂@g-C₃N₄ (415.57 μmol L^-1 g^-1h^-1), 1 T-MoS₂@N doped g-C₃N₄ (469.84 μmol L^-1 g^-1h^-1), and P doped 1 T-MoS₂@g-C₃N₄ (531.24 μmol L^-1 g^-1h^-1). In addition, compared with pure g-C₃N₄ NSs (2.64 mmol L^-1 g^-1h^-1), 1 T-MoS₂@g-C₃N₄ (4.98 mmol L^-1 g^-1h^-1), 1 T-MoS₂@N doped g-C₃N₄ (6.21 mmol L^-1 g^-1h^-1), and P doped 1 T-MoS₂@g-C₃N₄ (9.78 mmol L^-1 g^-1h^-1), P-1 T-MoS₂@N-g-C₃N₄ (11.12 mmol L^-1 g^-1h^-1) composite also shows a significant improvement for photocatalytic N₂ fixation efficiency in the sacrificial agent (methanol). The improved photocatalytic activity of P-1 T-MoS₂@N-g-C₃N₄ composite is ascribed to the following advantages: 1) Compared to pure g-C₃N₄, P-1 T-MoS₂@N-g-C₃N₄ composite shows higher light absorption capacity, which can improve the utilization rate of the catalyst to light; 2) The P doping intercalation strategy can promote the conversion of 1 T phase MoS₂, which in turn in favor of photogenerated electron transfer and reduce the recombination rate of carriers; 3) A large number of active sites on the edge of 1 T-MoS₂ and the existence of N doping in g-C₃N₄ contribute to photocatalytic N₂ fixation.