Efficient Photocatalytic Hydrogen Peroxide Generation Coupled with Selective Benzylamine Oxidation over Defective ZrS Nanobelts

Overview

Journal Nat Commun

Specialty Biology

Date 2021 Apr 2

PMID 33795681

Citations 7

Authors

Zhangliu Tian

Cheng Han

Yao Zhao

Wenrui Dai

Xu Lian

Yanan Wang

Yue Zheng

Yi Shi

Xuan Pan

Zhichao Huang

Hexing Li

Wei Chen

Affiliations

Soon will be listed here.

Abstract

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.

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