Abstract

Synergistic nitrogen (N2) reduction with water (H2O) oxidation is meaningful but challenging owing to the inertness of the N2 molecule and the sluggish kinetics of H2O oxidation. Herein, a simutaneous-promotion strategy of redox capacities is presented for constructing a lead-free Cs3Sb2Br9-based S-scheme heterojunction, by decorating Mo-functionalized Cs3Sb2Br9 nanocrystals (Cs3MoxSbyBr9) on BiVO4 nanosheet through an in-situ plane-to-point growth manner. The Mo-functionalization for Cs3Sb2Br9 enables the regulation of the d-band center position, greatly improving surface reaction kinetics for N2 reduction. Furthermore, the construction of the S-scheme heterojunction enhances the driving force for H2O oxidation and spatial charge separation of photocatalysts. As anticipated, the resultant Cs3MoxSbyBr9/BiVO4 exhibits an excellent photocatalytic N2 reduction activity under ambient atmosphere, achieving ammonia (NH3) production at a rate of 300 ± 5 μmol g−1 h−1 under simulated sunlight illumination (100 mW cm−2), which is nearly 20-fold higher than that of pristine Cs3Sb2Br9.

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