Fatemeh Pourroustaei-Ardakani , Hossein Mohammadi-Manesh , S. Javad Hashemifar
{"title":"Adsorption behavior of hydrogen sulfide in the channels of Li-ABW zeolite: A study using density functional theory","authors":"Fatemeh Pourroustaei-Ardakani , Hossein Mohammadi-Manesh , S. Javad Hashemifar","doi":"10.1016/j.jmgm.2024.108765","DOIUrl":null,"url":null,"abstract":"<div><p>H<sub>2</sub>S is a highly toxic, flammable gas that poses risks to health, the environment, and industrial infrastructure. Zeolites, with their high porosity, offer a promising solution for its removal. This study employs density functional theory (DFT) to investigate the adsorption behavior of H<sub>2</sub>S within the Li-ABW zeolite framework, focusing on the synergistic effect of co-adsorbed water molecules. Six distinct systems were modeled: empty Li-ABW zeolite, half and full filled Li-ABW with H<sub>2</sub>O or H<sub>2</sub>S molecules, and equally filled zeolite with H<sub>2</sub>S and H<sub>2</sub>O molecules. Detailed analysis of geometric, energetic, and electronic properties reveals that the presence of water significantly enhances H<sub>2</sub>S adsorption in Li-ABW. Increased bond lengths between H<sub>2</sub>S and the zeolite framework suggest possible dissociative adsorption, while weakened H<sub>2</sub>S-zeolite interaction compared to H<sub>2</sub>O-zeolite interaction indicates facile H<sub>2</sub>S desorption. Furthermore, charge transfer analysis and HOMO/LUMO plots highlight stronger interactions and a more balanced electron distribution in the co-adsorbed system. Interestingly, the presence of water minimizes structural deformations of the zeolite framework while facilitating the formation of additional hydrogen bonds, potentially further promoting H<sub>2</sub>S desorption through water extraction. These findings demonstrate that Li-ABW zeolite, particularly in conjunction with water molecules, exhibits remarkable potential for efficient and selective H<sub>2</sub>S adsorption, offering promising avenues for practical applications in gas sweetening and industrial gas purification. In order to realize this potential, further investigation into the effects of solvents and cation exchange is necessary, which are outlined for future research.</p></div>","PeriodicalId":16361,"journal":{"name":"Journal of molecular graphics & modelling","volume":null,"pages":null},"PeriodicalIF":2.7000,"publicationDate":"2024-04-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of molecular graphics & modelling","FirstCategoryId":"99","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1093326324000652","RegionNum":4,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"BIOCHEMICAL RESEARCH METHODS","Score":null,"Total":0}
引用次数: 0
Abstract
H2S is a highly toxic, flammable gas that poses risks to health, the environment, and industrial infrastructure. Zeolites, with their high porosity, offer a promising solution for its removal. This study employs density functional theory (DFT) to investigate the adsorption behavior of H2S within the Li-ABW zeolite framework, focusing on the synergistic effect of co-adsorbed water molecules. Six distinct systems were modeled: empty Li-ABW zeolite, half and full filled Li-ABW with H2O or H2S molecules, and equally filled zeolite with H2S and H2O molecules. Detailed analysis of geometric, energetic, and electronic properties reveals that the presence of water significantly enhances H2S adsorption in Li-ABW. Increased bond lengths between H2S and the zeolite framework suggest possible dissociative adsorption, while weakened H2S-zeolite interaction compared to H2O-zeolite interaction indicates facile H2S desorption. Furthermore, charge transfer analysis and HOMO/LUMO plots highlight stronger interactions and a more balanced electron distribution in the co-adsorbed system. Interestingly, the presence of water minimizes structural deformations of the zeolite framework while facilitating the formation of additional hydrogen bonds, potentially further promoting H2S desorption through water extraction. These findings demonstrate that Li-ABW zeolite, particularly in conjunction with water molecules, exhibits remarkable potential for efficient and selective H2S adsorption, offering promising avenues for practical applications in gas sweetening and industrial gas purification. In order to realize this potential, further investigation into the effects of solvents and cation exchange is necessary, which are outlined for future research.
期刊介绍:
The Journal of Molecular Graphics and Modelling is devoted to the publication of papers on the uses of computers in theoretical investigations of molecular structure, function, interaction, and design. The scope of the journal includes all aspects of molecular modeling and computational chemistry, including, for instance, the study of molecular shape and properties, molecular simulations, protein and polymer engineering, drug design, materials design, structure-activity and structure-property relationships, database mining, and compound library design.
As a primary research journal, JMGM seeks to bring new knowledge to the attention of our readers. As such, submissions to the journal need to not only report results, but must draw conclusions and explore implications of the work presented. Authors are strongly encouraged to bear this in mind when preparing manuscripts. Routine applications of standard modelling approaches, providing only very limited new scientific insight, will not meet our criteria for publication. Reproducibility of reported calculations is an important issue. Wherever possible, we urge authors to enhance their papers with Supplementary Data, for example, in QSAR studies machine-readable versions of molecular datasets or in the development of new force-field parameters versions of the topology and force field parameter files. Routine applications of existing methods that do not lead to genuinely new insight will not be considered.