RESUMO
The photocatalytic conversion of nitrogen into high-value ammonia products holds tremendous potential in the global nitrogen cycle. However, the activation of N2 and competition of hydrogen evolution limit the improvement of nitrogen fixation performance. In this study, we developed a fluorinated TiO2 (F-TiO2) using a hydrothermal-annealing method. The incorporation of F dopants not only enhances the adsorption and activation of N2 through electronic structure regulation, but also facilitates an in situ increase in active sites via the electron repulsion effect between F and Ti atoms. In addition, the presence of F on the surface effectively improved the nitrogen supply problem and optimized the nitrogen fixation selectivity for its hydrophobic modulation. The NH3 yield of the F-TiO2 photocatalyst reached 63.8 µmol h-1 g-1, which was 8.5 times higher than that of pure TiO2. And the selectivity experiment showed that the electronic ratio of NH3 to H2 production reached 0.890. This research offers valuable insights for the design of highly efficient and selective nitrogen-fixing photocatalysts.