4.8 Article

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

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NATURE COMMUNICATIONS
卷 12, 期 1, 页码 -

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NATURE PORTFOLIO
DOI: 10.1038/s41467-021-22394-8

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资金

  1. Singapore National Research Foundation [NRF2017NRF-NSFC001-007]
  2. NUS Flagship Green Energy Programme, Fundamental Research Foundation of Shenzhen [JCYJ20190808152607389, JCYJ20170817100405375]
  3. China Postdoctoral Science Foundation [2020M672794]
  4. Shenzhen Peacock Plan [KQTD2016053112042971]

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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.
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.

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