Regulation of oxygen reduction pathway on carbon nitride for enhanced H2O2 photosynthesis

IF 4.7 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General Pub Date : 2025-04-29 DOI:10.1016/j.apcata.2025.120311

Bo Sheng, Jiarui Li, Jing Zhang

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引用次数: 0

Abstract

Photocatalytic oxygen reduction reaction (ORR) to produce H₂O₂ on graphitic carbon nitride (CN) has been regarded as a green and sustainable route by using endless solar energy. However, this process is limited by side-reactions of single electron transfer process, thus decreasing the overall efficiency. Herein, we have proposed an effective method to optimize H₂O₂ photosynthesis by modulation of oxygen reduction pathway. That is modification of CN by introducing cyano groups and N defect in the presence of NaBH₄. The H₂O₂ production rate was 570 μmol/g/h by the optimal photocatalyst of BCN, showing 11-fold enhanced efficiency. Mechanism analysis proved that the convert of the single electron oxygen reduction in pristine CN into two-electron pathway in B_xCN occurred, which contributed to improved ORR efficiency and accelerated conversion of O₂^•− on H₂O₂ photosynthesis. This work revealed an effective method for optimizing H₂O₂ photosynthesis by regulating oxygen reduction reaction pathway.

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氮化碳氧还原途径对H2O2光合作用增强的调控

利用无穷无尽的太阳能，光催化氧还原反应（ORR）在石墨氮化碳（CN）上生成H2O2被认为是一条绿色可持续的途径。然而，这一过程受到单电子转移过程副反应的限制，从而降低了整体效率。本文提出了一种通过调节氧还原途径来优化H2O2光合作用的有效方法。即在NaBH4的存在下，通过引入氰基和N缺陷对CN进行修饰。优化后的BCN光催化剂H2O2产率为570 μmol/g/h，效率提高了11倍。机理分析证明，在BxCN中，原始CN的单电子氧还原发生了向双电子的转化，这有助于提高ORR效率，加速H2O2光合作用中O2•−的转化。本研究揭示了一种通过调节氧还原反应途径来优化H2O2光合作用的有效方法。

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来源期刊

Applied Catalysis A: General 化学-环境科学

CiteScore

9.00

自引率

5.50%

发文量

415

审稿时长

24 days

期刊介绍： Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.