Danqi Zhao, Yang Wen, Zhiqiang Li, Yan Cui, Yimin Zhao, Teng-Fei Lu, Ming He, Bo Song, Zhihua Zhang
{"title":"Theoretical study of adsorption of gas (CO, CO2, NH3) by metal (Au, Ag, Cu)-doped single-layer WS2","authors":"Danqi Zhao, Yang Wen, Zhiqiang Li, Yan Cui, Yimin Zhao, Teng-Fei Lu, Ming He, Bo Song, Zhihua Zhang","doi":"10.1007/s00894-024-06118-5","DOIUrl":null,"url":null,"abstract":"<div><h3>Context</h3><p>The adsorptions of gas (CO, CO<sub>2</sub>, NH<sub>3</sub>) by metal (Au, Ag, Cu)-doped single layer WS<sub>2</sub> are studied by density functional theory. The doping of metal atoms makes WS<sub>2</sub> behave as n-type semiconductors. The final adsorption sites for CO, CO<sub>2</sub>, and NH<sub>3</sub> are close to the atomic sites of the doped metal. The adsorptions of CO and NH<sub>3</sub> gases on Cu/WS<sub>2</sub>, Ag/WS<sub>2</sub>, and Au/WS<sub>2</sub> are dominated by chemisorption. The doped metal atoms enhance the hybridization of the substrate with the gas molecular orbitals, which contributes to the charge transfer and enhances the adsorption of the gas with the material surface. The adsorptions of CO and NH<sub>3</sub> on Cu/WS<sub>2</sub> and Ag/WS<sub>2</sub> allow favorable desorption in a short time after heating. The single-layer Cu/WS<sub>2</sub> is proved to have the potential to be used as a reliable recyclable sensor for CO. This work provides a theoretical basis for developing high-performance WS<sub>2</sub>-based gas sensors.</p><h3>Methods</h3><p>In this paper, the adsorption energy, electronic structure, charge transfer, and recovery time of CO, CO<sub>2</sub>, and NH<sub>3</sub> in the doped system have been investigated based on the CASTEP code of density functional theory. The exchange correlation function used is the Perdew-Burke-Ernzerhof (PBE) generalized gradient approximation (GGA). The TS (Tkatchenko-Scheffler) dispersion correction method was used to involve the effects of van der Waals interaction on the adsorption energies for all adsorption system. The ultrasoft pseudopotentials are chosen and the plane-wave cut-off energies are set to 500 eV. The k-point mesh generated by the Monkhorst package scheme is used to perform the numerical integration of the Brillouin zone and 5 × 5 × 1 k-point grid is used. The tolerances of total energy convergence, maximum ionic force, ionic displacement, and stress component are 1.0 × 10<sup>−5</sup> eV/atom, 0.03 eV/Å, 0.001 Å, and 0.05 GPa, respectively.</p></div>","PeriodicalId":651,"journal":{"name":"Journal of Molecular Modeling","volume":null,"pages":null},"PeriodicalIF":2.1000,"publicationDate":"2024-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Molecular Modeling","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1007/s00894-024-06118-5","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q4","JCRName":"BIOCHEMISTRY & MOLECULAR BIOLOGY","Score":null,"Total":0}
引用次数: 0
Abstract
Context
The adsorptions of gas (CO, CO2, NH3) by metal (Au, Ag, Cu)-doped single layer WS2 are studied by density functional theory. The doping of metal atoms makes WS2 behave as n-type semiconductors. The final adsorption sites for CO, CO2, and NH3 are close to the atomic sites of the doped metal. The adsorptions of CO and NH3 gases on Cu/WS2, Ag/WS2, and Au/WS2 are dominated by chemisorption. The doped metal atoms enhance the hybridization of the substrate with the gas molecular orbitals, which contributes to the charge transfer and enhances the adsorption of the gas with the material surface. The adsorptions of CO and NH3 on Cu/WS2 and Ag/WS2 allow favorable desorption in a short time after heating. The single-layer Cu/WS2 is proved to have the potential to be used as a reliable recyclable sensor for CO. This work provides a theoretical basis for developing high-performance WS2-based gas sensors.
Methods
In this paper, the adsorption energy, electronic structure, charge transfer, and recovery time of CO, CO2, and NH3 in the doped system have been investigated based on the CASTEP code of density functional theory. The exchange correlation function used is the Perdew-Burke-Ernzerhof (PBE) generalized gradient approximation (GGA). The TS (Tkatchenko-Scheffler) dispersion correction method was used to involve the effects of van der Waals interaction on the adsorption energies for all adsorption system. The ultrasoft pseudopotentials are chosen and the plane-wave cut-off energies are set to 500 eV. The k-point mesh generated by the Monkhorst package scheme is used to perform the numerical integration of the Brillouin zone and 5 × 5 × 1 k-point grid is used. The tolerances of total energy convergence, maximum ionic force, ionic displacement, and stress component are 1.0 × 10−5 eV/atom, 0.03 eV/Å, 0.001 Å, and 0.05 GPa, respectively.
期刊介绍:
The Journal of Molecular Modeling focuses on "hardcore" modeling, publishing high-quality research and reports. Founded in 1995 as a purely electronic journal, it has adapted its format to include a full-color print edition, and adjusted its aims and scope fit the fast-changing field of molecular modeling, with a particular focus on three-dimensional modeling.
Today, the journal covers all aspects of molecular modeling including life science modeling; materials modeling; new methods; and computational chemistry.
Topics include computer-aided molecular design; rational drug design, de novo ligand design, receptor modeling and docking; cheminformatics, data analysis, visualization and mining; computational medicinal chemistry; homology modeling; simulation of peptides, DNA and other biopolymers; quantitative structure-activity relationships (QSAR) and ADME-modeling; modeling of biological reaction mechanisms; and combined experimental and computational studies in which calculations play a major role.