Lijun He , Xing Long , Liyan Wang , Cheng Mi , Chaopeng Zhang , Kang Ma , Liang She , Mi Yu
{"title":"Highly efficient photocatalytic performance of Z-scheme BTe/HfS2 heterostructure for H2O splitting","authors":"Lijun He , Xing Long , Liyan Wang , Cheng Mi , Chaopeng Zhang , Kang Ma , Liang She , Mi Yu","doi":"10.1016/j.jcat.2024.115606","DOIUrl":null,"url":null,"abstract":"<div><p>Constructing van der Waals (vdW) heterostructures is one of the effective strategies for developing highly efficient photocatalysts. In this study, we have designed a novel BTe/HfS<sub>2</sub> heterostructure and systematically investigated its electronic properties and photocatalytic performance using first-principles calculations. The dynamic stability and thermodynamic stability of the heterostructure are verified through phonon spectrum simulations and ab initio molecular dynamics (AIMD) simulations, respectively, enhancing the likelihood of experimental synthesis. The bandgap of the BTe/HfS<sub>2</sub> heterostructure is 0.12 eV, and the band edge positions satisfy the overall water splitting requirements for photocatalysts. The charge density difference, work function, Bader charge, and band alignment all confirm that the BTe/HfS<sub>2</sub> heterostructure is a typical direct Z-scheme heterostructure, effectively facilitating the separation of photogenerated charge carriers and exhibiting strong redox capability. The solar-to-hydrogen (STH) efficiency of the BTe/HfS<sub>2</sub> heterostructure reaches as high as 17.32 %. Moreover, the heterostructure exhibits strong light absorption capability, reaching a magnitude of 10<sup>5</sup>. The carrier mobility of the BTe/HfS<sub>2</sub> heterostructure surpasses that of two individual monolayer materials, with the hole mobility in the <em>x</em>-direction reaching an impressive 28357.15 cm<sup>2</sup>s<sup>-1</sup>V<sup>-1</sup>. Simultaneously, the Gibbs free energy indicates that the BTe/HfS<sub>2</sub> heterostructure can undergo the hydrogen evolution reaction (HER) with only 0.19 eV of external potential at pH = 0. Moreover, at pH = 7, it can spontaneously convert H<sub>2</sub>O into O<sub>2</sub>. Therefore, the newly designed BTe/HfS<sub>2</sub> heterostructure offers a new direction for practical applications of photocatalysts.</p></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":null,"pages":null},"PeriodicalIF":6.5000,"publicationDate":"2024-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0021951724003191","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Constructing van der Waals (vdW) heterostructures is one of the effective strategies for developing highly efficient photocatalysts. In this study, we have designed a novel BTe/HfS2 heterostructure and systematically investigated its electronic properties and photocatalytic performance using first-principles calculations. The dynamic stability and thermodynamic stability of the heterostructure are verified through phonon spectrum simulations and ab initio molecular dynamics (AIMD) simulations, respectively, enhancing the likelihood of experimental synthesis. The bandgap of the BTe/HfS2 heterostructure is 0.12 eV, and the band edge positions satisfy the overall water splitting requirements for photocatalysts. The charge density difference, work function, Bader charge, and band alignment all confirm that the BTe/HfS2 heterostructure is a typical direct Z-scheme heterostructure, effectively facilitating the separation of photogenerated charge carriers and exhibiting strong redox capability. The solar-to-hydrogen (STH) efficiency of the BTe/HfS2 heterostructure reaches as high as 17.32 %. Moreover, the heterostructure exhibits strong light absorption capability, reaching a magnitude of 105. The carrier mobility of the BTe/HfS2 heterostructure surpasses that of two individual monolayer materials, with the hole mobility in the x-direction reaching an impressive 28357.15 cm2s-1V-1. Simultaneously, the Gibbs free energy indicates that the BTe/HfS2 heterostructure can undergo the hydrogen evolution reaction (HER) with only 0.19 eV of external potential at pH = 0. Moreover, at pH = 7, it can spontaneously convert H2O into O2. Therefore, the newly designed BTe/HfS2 heterostructure offers a new direction for practical applications of photocatalysts.
期刊介绍:
The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes.
The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods.
The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.