{"title":"氮化碳氧还原途径对H2O2光合作用增强的调控","authors":"Bo Sheng, Jiarui Li, Jing Zhang","doi":"10.1016/j.apcata.2025.120311","DOIUrl":null,"url":null,"abstract":"<div><div>Photocatalytic oxygen reduction reaction (ORR) to produce H<sub>2</sub>O<sub>2</sub> 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 H<sub>2</sub>O<sub>2</sub> photosynthesis by modulation of oxygen reduction pathway. That is modification of CN by introducing cyano groups and N defect in the presence of NaBH<sub>4</sub>. The H<sub>2</sub>O<sub>2</sub> 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<sub>x</sub>CN occurred, which contributed to improved ORR efficiency and accelerated conversion of O<sub>2</sub><sup>•−</sup> on H<sub>2</sub>O<sub>2</sub> photosynthesis. This work revealed an effective method for optimizing H<sub>2</sub>O<sub>2</sub> photosynthesis by regulating oxygen reduction reaction pathway.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"701 ","pages":"Article 120311"},"PeriodicalIF":4.7000,"publicationDate":"2025-04-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Regulation of oxygen reduction pathway on carbon nitride for enhanced H2O2 photosynthesis\",\"authors\":\"Bo Sheng, Jiarui Li, Jing Zhang\",\"doi\":\"10.1016/j.apcata.2025.120311\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Photocatalytic oxygen reduction reaction (ORR) to produce H<sub>2</sub>O<sub>2</sub> 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 H<sub>2</sub>O<sub>2</sub> photosynthesis by modulation of oxygen reduction pathway. That is modification of CN by introducing cyano groups and N defect in the presence of NaBH<sub>4</sub>. The H<sub>2</sub>O<sub>2</sub> 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<sub>x</sub>CN occurred, which contributed to improved ORR efficiency and accelerated conversion of O<sub>2</sub><sup>•−</sup> on H<sub>2</sub>O<sub>2</sub> photosynthesis. This work revealed an effective method for optimizing H<sub>2</sub>O<sub>2</sub> photosynthesis by regulating oxygen reduction reaction pathway.</div></div>\",\"PeriodicalId\":243,\"journal\":{\"name\":\"Applied Catalysis A: General\",\"volume\":\"701 \",\"pages\":\"Article 120311\"},\"PeriodicalIF\":4.7000,\"publicationDate\":\"2025-04-29\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Catalysis A: General\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0926860X25002121\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Catalysis A: General","FirstCategoryId":"1","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0926860X25002121","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Regulation of oxygen reduction pathway on carbon nitride for enhanced H2O2 photosynthesis
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 BxCN 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.
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.