{"title":"呋喃基 HTCC/In2S3 异质结实现快速电荷分离,促进纯水中 H2O2 的光催化生成","authors":"Xiaolong Tang, Changlin Yu*, Jiaming Zhang, Kaiwei Liu, Debin Zeng, Fang Li, Feng Li, Guijun Ma, Yanbin Jiang and Yongfa Zhu*, ","doi":"10.1021/acscatal.4c0434110.1021/acscatal.4c04341","DOIUrl":null,"url":null,"abstract":"<p >The limitations imposed by the high carrier recombination rate in the current photocatalytic H<sub>2</sub>O<sub>2</sub> production system substantially restrict the rate of H<sub>2</sub>O<sub>2</sub> generation. Herein, we successfully prepared an In<sub>2</sub>S<sub>3</sub>/HTCC dense heterojunction bridged by In–S–C bonds through in situ polymerization of glucose on In<sub>2</sub>S<sub>3</sub>. This interfacial In–S–C bond provides a fast transfer channel for electrons at the interface to achieve a highly efficient interfacial charge transfer efficiency, leading to the formation of an enhanced built-in electric field between In<sub>2</sub>S<sub>3</sub> and HTCC, thus dramatically accelerating the rate of charge separation and effectively prolonging the lifetime of the photogenerated carriers. Moreover, the coverage of HTCC enhances the absorption of visible light and sorption of O<sub>2</sub> by In<sub>2</sub>S<sub>3</sub>, while lowering its two-electron oxygen reduction reaction (ORR) energy barrier. Notably, our research demonstrates that In<sub>2</sub>S<sub>3</sub>/HTCC can generate H<sub>2</sub>O<sub>2</sub> not only through the well-known two-step one-electron ORR but also via an alternative pathway utilizing <sup>1</sup>O<sub>2</sub> as an intermediate, thereby enhancing H<sub>2</sub>O<sub>2</sub> production. Benefiting from these advantages, In<sub>2</sub>S<sub>3</sub>/HTCC-2 can produce H<sub>2</sub>O<sub>2</sub> at a rate of up to 1392 μmol g<sup>–1</sup> h<sup>–1</sup> in a pure aqueous system, which is 18.2 and 5.2 times higher than that of pure In<sub>2</sub>S<sub>3</sub> and HTCC, respectively. Our work not only provides a novel synthesis method of new organic/inorganic heterojunction photocatalysts based on HTCC but also offers new insights into the potential mechanism of interfacial bonding of heterostructures to regulate the photocatalytic H<sub>2</sub>O<sub>2</sub> production activity.</p>","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"14 21","pages":"16245–16255 16245–16255"},"PeriodicalIF":11.3000,"publicationDate":"2024-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Furan-Based HTCC/In2S3 Heterojunction Achieves Fast Charge Separation To Boost the Photocatalytic Generation of H2O2 in Pure Water\",\"authors\":\"Xiaolong Tang, Changlin Yu*, Jiaming Zhang, Kaiwei Liu, Debin Zeng, Fang Li, Feng Li, Guijun Ma, Yanbin Jiang and Yongfa Zhu*, \",\"doi\":\"10.1021/acscatal.4c0434110.1021/acscatal.4c04341\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >The limitations imposed by the high carrier recombination rate in the current photocatalytic H<sub>2</sub>O<sub>2</sub> production system substantially restrict the rate of H<sub>2</sub>O<sub>2</sub> generation. Herein, we successfully prepared an In<sub>2</sub>S<sub>3</sub>/HTCC dense heterojunction bridged by In–S–C bonds through in situ polymerization of glucose on In<sub>2</sub>S<sub>3</sub>. This interfacial In–S–C bond provides a fast transfer channel for electrons at the interface to achieve a highly efficient interfacial charge transfer efficiency, leading to the formation of an enhanced built-in electric field between In<sub>2</sub>S<sub>3</sub> and HTCC, thus dramatically accelerating the rate of charge separation and effectively prolonging the lifetime of the photogenerated carriers. Moreover, the coverage of HTCC enhances the absorption of visible light and sorption of O<sub>2</sub> by In<sub>2</sub>S<sub>3</sub>, while lowering its two-electron oxygen reduction reaction (ORR) energy barrier. Notably, our research demonstrates that In<sub>2</sub>S<sub>3</sub>/HTCC can generate H<sub>2</sub>O<sub>2</sub> not only through the well-known two-step one-electron ORR but also via an alternative pathway utilizing <sup>1</sup>O<sub>2</sub> as an intermediate, thereby enhancing H<sub>2</sub>O<sub>2</sub> production. Benefiting from these advantages, In<sub>2</sub>S<sub>3</sub>/HTCC-2 can produce H<sub>2</sub>O<sub>2</sub> at a rate of up to 1392 μmol g<sup>–1</sup> h<sup>–1</sup> in a pure aqueous system, which is 18.2 and 5.2 times higher than that of pure In<sub>2</sub>S<sub>3</sub> and HTCC, respectively. Our work not only provides a novel synthesis method of new organic/inorganic heterojunction photocatalysts based on HTCC but also offers new insights into the potential mechanism of interfacial bonding of heterostructures to regulate the photocatalytic H<sub>2</sub>O<sub>2</sub> production activity.</p>\",\"PeriodicalId\":9,\"journal\":{\"name\":\"ACS Catalysis \",\"volume\":\"14 21\",\"pages\":\"16245–16255 16245–16255\"},\"PeriodicalIF\":11.3000,\"publicationDate\":\"2024-10-19\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Catalysis \",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acscatal.4c04341\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Catalysis ","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acscatal.4c04341","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Furan-Based HTCC/In2S3 Heterojunction Achieves Fast Charge Separation To Boost the Photocatalytic Generation of H2O2 in Pure Water
The limitations imposed by the high carrier recombination rate in the current photocatalytic H2O2 production system substantially restrict the rate of H2O2 generation. Herein, we successfully prepared an In2S3/HTCC dense heterojunction bridged by In–S–C bonds through in situ polymerization of glucose on In2S3. This interfacial In–S–C bond provides a fast transfer channel for electrons at the interface to achieve a highly efficient interfacial charge transfer efficiency, leading to the formation of an enhanced built-in electric field between In2S3 and HTCC, thus dramatically accelerating the rate of charge separation and effectively prolonging the lifetime of the photogenerated carriers. Moreover, the coverage of HTCC enhances the absorption of visible light and sorption of O2 by In2S3, while lowering its two-electron oxygen reduction reaction (ORR) energy barrier. Notably, our research demonstrates that In2S3/HTCC can generate H2O2 not only through the well-known two-step one-electron ORR but also via an alternative pathway utilizing 1O2 as an intermediate, thereby enhancing H2O2 production. Benefiting from these advantages, In2S3/HTCC-2 can produce H2O2 at a rate of up to 1392 μmol g–1 h–1 in a pure aqueous system, which is 18.2 and 5.2 times higher than that of pure In2S3 and HTCC, respectively. Our work not only provides a novel synthesis method of new organic/inorganic heterojunction photocatalysts based on HTCC but also offers new insights into the potential mechanism of interfacial bonding of heterostructures to regulate the photocatalytic H2O2 production activity.
期刊介绍:
ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels.
The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.