Transition metals anchored on two-dimensional p-BN support with center-coordination scaling relationship descriptor for spontaneous visible-light-driven photocatalytic nitrogen reduction

Solar energy has the potential to revolutionize the production of ammonia, as it could provide a reliable and uninterrupted source of energy for the chemical reaction involved. However, improving the catalytic performance of catalysts often leads to a reduction in their band gaps, which results in insufficient photogenerated electron potential to realize the nitrogen reduction reaction (NRR), and thus the development of NRR efficient photocatalysts remains a great challenge. Herein, based on the density functional theory (DFT), a series of single-atom photocatalysts with transition metals (TMs) doped on porous boron nitride (p-BN) nanosheet are proposed for NRR. Among them, Re-B3@p-BN could effectively catalyze gas-phase N₂ through the corresponding pathways with limiting potentials of 0.31 V. Meanwhile, it exhibits excellent light absorption efficiency under illumination and could spontaneously catalyse nitrogen fixation reactions due to the suitable forbidden band and high photogenerated electron potential. Moreover, a linear relationship descriptor based on the intrinsic properties has been established, using a machine learning approach by considering the combined effects of the central metal atom and the coordination atoms. This descriptor could help accelerate the development of rational and improved 2D NRR photocatalysts with high catalytic activity and high selectivity.