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Oxygen-modified graphitic carbon nitride with nitrogen-defect for metal-free visible light photocatalytic H2O2 evolution

Journal 2023 · IF 9.9 · 发表于 2023 年 7 月 13 日
作者: Yanqing Cong,Shiyi Zhang,Qiuang Zheng,Xinyue Li,Yi Zhang,Shi-Wen Lv
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摘要

Photocatalytic oxygen reduction is regarded as the cleanest approach for the production of hydrogen peroxide (H 2 O 2 ). Herein, oxygen-modified graphite carbon nitride (g-C 3 N 4 ) with nitrogen-defect (namely g-C 3 N 4 -ND4-OM3) was synthesized by a feasible method. Owing to the existence of nitrogen vacancy and oxygen-containing functional group, the absorption bands derived from n → π* and π → π* electronic transitions were enhanced, thereby enlarging the visible light response range of catalysts. Interestingly, nitrogen-defect can capture electron and effectively suppress the recombination of photoinduced electrons and holes. More importantly, the introduction of oxygen-containing functional groups can improve the hydrophilicity of g-C 3 N 4 , which was beneficial for the adsorption of dissolved oxygen. The electrostatic potential distributions of g-C 3 N 4 -based photocatalyst structural unit were also changed after introducing nitrogen vacancy and oxygen-containing functional group, and the electron-donating ability of g-C 3 N 4 was improved. As a result, the evolution rate of H 2 O 2 catalyzed by g-C 3 N 4 -ND4-OM3 was as high as 146.96 μmol/g/L under visible light irradiation. The photocatalytic H 2 O 2 generation was completed through the direct 2-e − oxygen reduction. In short, current work will share novel insights into photocatalytic H 2 O 2 generation over g-C 3 N 4 -based catalyst.

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