Efficient photocatalytic hydrogen peroxide generation coupled with selective benzylamine oxidation over defective ZrS nanobelts.

Photocatalytic hydrogen peroxide (HO) generation represents a promising approach for artificial photosynthesis. However, the sluggish half-reaction of water oxidation significantly limits the efficiency of HO generation. Here, a benzylamine oxidation with more favorable thermodynamics is employed as the half-reaction to couple with HO generation in water by using defective zirconium trisulfide (ZrS) nanobelts as a photocatalyst. The ZrS nanobelts with disulfide (S) and sulfide anion (S) vacancies exhibit an excellent photocatalytic performance for HO generation and simultaneous oxidation of benzylamine to benzonitrile with a high selectivity of >99%. More importantly, the S and S vacancies can be separately introduced into ZrS nanobelts in a controlled manner. The S vacancies are further revealed to facilitate the separation of photogenerated charge carriers. The S vacancies can significantly improve the electron conduction, hole extraction, and kinetics of benzylamine oxidation. As a result, the use of defective ZrS nanobelts yields a high production rate of 78.1 ± 1.5 and 32.0 ± 1.2 μmol h for HO and benzonitrile, respectively, under a simulated sunlight irradiation.