Efficient photocatalytic hydrogen peroxide generation coupled with selective benzylamine oxidation over defective ZrS3 nanobelts

Photocatalytic hydrogen peroxide (H2O2) generation represents a promising approach for artificial photosynthesis. However, the sluggish half-reaction of water oxidation significantly limits the efficiency of H2O2 generation. Here, a benzylamine oxidation with more favorable thermodynamics is employed as the half-reaction to couple with H2O2 generation in water by using defective zirconium trisulfide (ZrS3) nanobelts as a photocatalyst. The ZrS3 nanobelts with disulfide (S-2(2-)) and sulfide anion (S2-) vacancies exhibit an excellent photocatalytic performance for H2O2 generation and simultaneous oxidation of benzylamine to benzonitrile with a high selectivity of >99%. More importantly, the S-2(2-) and S2- vacancies can be separately introduced into ZrS3 nanobelts in a controlled manner. The S-2(2-) vacancies are further revealed to facilitate the separation of photogenerated charge carriers. The S2- vacancies can significantly improve the electron conduction, hole extraction, and kinetics of benzylamine oxidation. As a result, the use of defective ZrS3 nanobelts yields a high production rate of 78.1 1.5 and 32.0 +/- 1.2 mu mol h(-1) for H2O2 and benzonitrile, respectively, under a simulated sunlight irradiation. Photocatalytic H2O2 generation represents a promising approach for artificial photosynthesis. Here, ZrS3 nanobelts with controllable disulfide and sulfide anion vacancies exhibit an excellent photocatalytic H2O2 generation performance together with selective oxidation of benzylamine to benzonitrile.

Automated summary

The photocatalytic generation of hydrogen peroxide (H2O2) using benzylamine oxidation as a half-reaction coupled with ZrS3 nanobelts shows excellent efficiency and selectivity in the simultaneous oxidation of benzylamine to benzonitrile.