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

Zhangliu Tian, Cheng Han (), Yao Zhao, Wenrui Dai, Xu Lian, Yanan Wang, Yue Zheng, Yi Shi, Xuan Pan, Zhichao Huang, Hexing Li and Wei Chen ()
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Zhangliu Tian: Shenzhen University
Cheng Han: Shenzhen University
Yao Zhao: National University of Singapore
Wenrui Dai: National University of Singapore
Xu Lian: National University of Singapore
Yanan Wang: National University of Singapore
Yue Zheng: National University of Singapore
Yi Shi: National University of Singapore
Xuan Pan: Shenzhen University
Zhichao Huang: Shenzhen University
Hexing Li: Shanghai Normal University
Wei Chen: National University of Singapore

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: Abstract 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 (S22−) 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 S22− and S2− vacancies can be separately introduced into ZrS3 nanobelts in a controlled manner. The S22− 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 μmol h−1 for H2O2 and benzonitrile, respectively, under a simulated sunlight irradiation.

Date: 2021
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DOI: 10.1038/s41467-021-22394-8

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