Efficient photocatalytic hydrogen peroxide generation coupled with selective benzylamine oxidation over defective ZrS(3) nanobelts

Photocatalytic hydrogen peroxide (H(2)O(2)) generation represents a promising approach for artificial photosynthesis. However, the sluggish half-reaction of water oxidation significantly limits the efficiency of H(2)O(2) generation. Here, a benzylamine oxidation with more favorable thermodynamics is employed as the half-reaction to couple with H(2)O(2) generation in water by using defective zirconium trisulfide (ZrS(3)) nanobelts as a photocatalyst. The ZrS(3) nanobelts with disulfide (S(2)(2−)) and sulfide anion (S(2−)) vacancies exhibit an excellent photocatalytic performance for H(2)O(2) generation and simultaneous oxidation of benzylamine to benzonitrile with a high selectivity of >99%. More importantly, the S(2)(2−) and S(2−) vacancies can be separately introduced into ZrS(3) nanobelts in a controlled manner. The S(2)(2−) vacancies are further revealed to facilitate the separation of photogenerated charge carriers. The S(2−) vacancies can significantly improve the electron conduction, hole extraction, and kinetics of benzylamine oxidation. As a result, the use of defective ZrS(3) nanobelts yields a high production rate of 78.1 ± 1.5 and 32.0 ± 1.2 μmol h(−1) for H(2)O(2) and benzonitrile, respectively, under a simulated sunlight irradiation.