{"title":"用于光催化固氮的 MIL-101(Fe)/g-C3N4 S-Scheme 异质结的纳米结构:机理与性能","authors":"","doi":"10.1016/j.surfin.2024.105083","DOIUrl":null,"url":null,"abstract":"<div><p>Recently, there has been a growing interest in the fundamental understanding of the mechanism of how MIL-101(Fe)/g-C<sub>3</sub>N<sub>4</sub> heterojunctions facilitate the occurrence of photocatalytic nitrogen fixation reactions, especially the electron transfer mechanism has attained increasing attention in photocatalysis. Herein, we implemented a \"triple win scenario\" strategy to fabricate the S-scheme MIL-101(Fe)/g-C<sub>3</sub>N<sub>4</sub> heterojunction through a straightforward solvothermal process. The MC-6 heterojunction minimizes the recombination of photogenerated carriers, enhances light utilization efficiency, and activates the N≡N bond, thus boosting photocatalytic nitrogen fixation efficiency. The transition metal iron activates the N≡N bond, while S-scheme heterojunctions reduce the photogenerated carrier recombination. In addition, the decrease in band gap (E<sub>g</sub>) leads to an increase in visible light utilization efficiency. ISIXPS proved the mechanism of interelectron transfer of MIL-101(Fe)/g-C<sub>3</sub>N<sub>4</sub> heterojunction under illumination. Upon the creation of the heterojunction, electrons migrate from g-C<sub>3</sub>N<sub>4</sub> to MIL-101(Fe), establishing an inherent electric field due to the disparate Fermi levels between the two materials. The electrons (e<sup>-</sup>) on the g-C<sub>3</sub>N<sub>4</sub> CB with a more negative reduction potential and the holes (<em>h</em><sup>+</sup>) on the MIL-101(Fe) VB are retained, which increased the redox capacity to a great extent required for the reduction of N<sub>2</sub> to NH<sub>3</sub>. The ammonia production efficiency of MC-6 photocatalyst was 160 µmol g<sub>cat</sub><sup>-1</sup> h<sup>-1</sup>, representing an 8-fold and 2.8-fold improvement over pristine g-C<sub>3</sub>N<sub>4</sub> (20 µmol g<sub>cat</sub><sup>-1</sup> h<sup>-1</sup>) and MIL-101(Fe) (57 µmol g<sub>cat</sub><sup>-1</sup> h<sup>-1</sup>), respectively.</p></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":null,"pages":null},"PeriodicalIF":5.7000,"publicationDate":"2024-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Nanoarchitectonics of MIL-101(Fe)/g-C3N4 S-Scheme heterojunction for photocatalytic nitrogen fixation: Mechanisms and performance\",\"authors\":\"\",\"doi\":\"10.1016/j.surfin.2024.105083\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Recently, there has been a growing interest in the fundamental understanding of the mechanism of how MIL-101(Fe)/g-C<sub>3</sub>N<sub>4</sub> heterojunctions facilitate the occurrence of photocatalytic nitrogen fixation reactions, especially the electron transfer mechanism has attained increasing attention in photocatalysis. Herein, we implemented a \\\"triple win scenario\\\" strategy to fabricate the S-scheme MIL-101(Fe)/g-C<sub>3</sub>N<sub>4</sub> heterojunction through a straightforward solvothermal process. The MC-6 heterojunction minimizes the recombination of photogenerated carriers, enhances light utilization efficiency, and activates the N≡N bond, thus boosting photocatalytic nitrogen fixation efficiency. The transition metal iron activates the N≡N bond, while S-scheme heterojunctions reduce the photogenerated carrier recombination. In addition, the decrease in band gap (E<sub>g</sub>) leads to an increase in visible light utilization efficiency. ISIXPS proved the mechanism of interelectron transfer of MIL-101(Fe)/g-C<sub>3</sub>N<sub>4</sub> heterojunction under illumination. Upon the creation of the heterojunction, electrons migrate from g-C<sub>3</sub>N<sub>4</sub> to MIL-101(Fe), establishing an inherent electric field due to the disparate Fermi levels between the two materials. The electrons (e<sup>-</sup>) on the g-C<sub>3</sub>N<sub>4</sub> CB with a more negative reduction potential and the holes (<em>h</em><sup>+</sup>) on the MIL-101(Fe) VB are retained, which increased the redox capacity to a great extent required for the reduction of N<sub>2</sub> to NH<sub>3</sub>. The ammonia production efficiency of MC-6 photocatalyst was 160 µmol g<sub>cat</sub><sup>-1</sup> h<sup>-1</sup>, representing an 8-fold and 2.8-fold improvement over pristine g-C<sub>3</sub>N<sub>4</sub> (20 µmol g<sub>cat</sub><sup>-1</sup> h<sup>-1</sup>) and MIL-101(Fe) (57 µmol g<sub>cat</sub><sup>-1</sup> h<sup>-1</sup>), respectively.</p></div>\",\"PeriodicalId\":22081,\"journal\":{\"name\":\"Surfaces and Interfaces\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.7000,\"publicationDate\":\"2024-09-08\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Surfaces and Interfaces\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2468023024012392\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Surfaces and Interfaces","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2468023024012392","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Nanoarchitectonics of MIL-101(Fe)/g-C3N4 S-Scheme heterojunction for photocatalytic nitrogen fixation: Mechanisms and performance
Recently, there has been a growing interest in the fundamental understanding of the mechanism of how MIL-101(Fe)/g-C3N4 heterojunctions facilitate the occurrence of photocatalytic nitrogen fixation reactions, especially the electron transfer mechanism has attained increasing attention in photocatalysis. Herein, we implemented a "triple win scenario" strategy to fabricate the S-scheme MIL-101(Fe)/g-C3N4 heterojunction through a straightforward solvothermal process. The MC-6 heterojunction minimizes the recombination of photogenerated carriers, enhances light utilization efficiency, and activates the N≡N bond, thus boosting photocatalytic nitrogen fixation efficiency. The transition metal iron activates the N≡N bond, while S-scheme heterojunctions reduce the photogenerated carrier recombination. In addition, the decrease in band gap (Eg) leads to an increase in visible light utilization efficiency. ISIXPS proved the mechanism of interelectron transfer of MIL-101(Fe)/g-C3N4 heterojunction under illumination. Upon the creation of the heterojunction, electrons migrate from g-C3N4 to MIL-101(Fe), establishing an inherent electric field due to the disparate Fermi levels between the two materials. The electrons (e-) on the g-C3N4 CB with a more negative reduction potential and the holes (h+) on the MIL-101(Fe) VB are retained, which increased the redox capacity to a great extent required for the reduction of N2 to NH3. The ammonia production efficiency of MC-6 photocatalyst was 160 µmol gcat-1 h-1, representing an 8-fold and 2.8-fold improvement over pristine g-C3N4 (20 µmol gcat-1 h-1) and MIL-101(Fe) (57 µmol gcat-1 h-1), respectively.
期刊介绍:
The aim of the journal is to provide a respectful outlet for ''sound science'' papers in all research areas on surfaces and interfaces. We define sound science papers as papers that describe new and well-executed research, but that do not necessarily provide brand new insights or are merely a description of research results.
Surfaces and Interfaces publishes research papers in all fields of surface science which may not always find the right home on first submission to our Elsevier sister journals (Applied Surface, Surface and Coatings Technology, Thin Solid Films)