{"title":"Sulfur-doped g-C3N4/V2C MXene Schottky junctions for superior photocatalytic H2 evolution","authors":"Haitao Wang, Jipeng Fan, Jing Zou, Yujie Zheng, Dingsheng Wang, Jizhou Jiang","doi":"10.1039/d4ta05929h","DOIUrl":null,"url":null,"abstract":"Graphitic carbon nitride (g-C3N4) is considered to be a promising photocatalyst for hydrogen evolution reaction (HER) due to its facile synthesis, outstanding chemical/thermal stability and suitable band structure. However, the unsatisfactory performance of pristine g-C3N4 severely restricts its its further widespread application. In this work, theoretical predictions reveal that integrating sulfur dopants and coupling vanadium carbide (V2C) MXene can significantly optimize the hydrogen adsorbed Gibbs free energy (ΔGH*) of g-C3N4 to near zero. Inspired by the theoretical predictions, an advanced HER photocatalyst of sulfur-doped g-C3N4/V2C MXene (SCN/V2C) Schottky junction is fabricated successfully by vacuum ball milling and subsequent annealing treatment. Interface-charge transfer between SCN and V2C endows a strong electron interaction, which not only improves hydrophilicity and visible-light absorption, but also facilitates the separation and migration of photoexcited carriers. Density functional theory calculations and in situ characterization results corroborate that the carrier migration of SCN/V2C adheres to the typical Schottky heterojunction mechanism. Femtosecond transientabsorption (fs-TA) spectroscopy demonstrates the favorable carrier dynamic behavior of developed SCN/V2C photocatalysts. Thus, the SCN/V2C achieves a superior H2 production rate of 8003 μmol g-1 h-1. The Schottky heterojunction established in this research provides valuable insights into the further strategic design and construction of high-performance HER photocatalysts.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":10.7000,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Materials Chemistry A","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1039/d4ta05929h","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Graphitic carbon nitride (g-C3N4) is considered to be a promising photocatalyst for hydrogen evolution reaction (HER) due to its facile synthesis, outstanding chemical/thermal stability and suitable band structure. However, the unsatisfactory performance of pristine g-C3N4 severely restricts its its further widespread application. In this work, theoretical predictions reveal that integrating sulfur dopants and coupling vanadium carbide (V2C) MXene can significantly optimize the hydrogen adsorbed Gibbs free energy (ΔGH*) of g-C3N4 to near zero. Inspired by the theoretical predictions, an advanced HER photocatalyst of sulfur-doped g-C3N4/V2C MXene (SCN/V2C) Schottky junction is fabricated successfully by vacuum ball milling and subsequent annealing treatment. Interface-charge transfer between SCN and V2C endows a strong electron interaction, which not only improves hydrophilicity and visible-light absorption, but also facilitates the separation and migration of photoexcited carriers. Density functional theory calculations and in situ characterization results corroborate that the carrier migration of SCN/V2C adheres to the typical Schottky heterojunction mechanism. Femtosecond transientabsorption (fs-TA) spectroscopy demonstrates the favorable carrier dynamic behavior of developed SCN/V2C photocatalysts. Thus, the SCN/V2C achieves a superior H2 production rate of 8003 μmol g-1 h-1. The Schottky heterojunction established in this research provides valuable insights into the further strategic design and construction of high-performance HER photocatalysts.
期刊介绍:
The Journal of Materials Chemistry A, B & C covers a wide range of high-quality studies in the field of materials chemistry, with each section focusing on specific applications of the materials studied. Journal of Materials Chemistry A emphasizes applications in energy and sustainability, including topics such as artificial photosynthesis, batteries, and fuel cells. Journal of Materials Chemistry B focuses on applications in biology and medicine, while Journal of Materials Chemistry C covers applications in optical, magnetic, and electronic devices. Example topic areas within the scope of Journal of Materials Chemistry A include catalysis, green/sustainable materials, sensors, and water treatment, among others.