Two-dimensional ammonia-linked COF structures with different substituents for the adsorption and separation of sulfur hexafluoride: A theoretical study
{"title":"Two-dimensional ammonia-linked COF structures with different substituents for the adsorption and separation of sulfur hexafluoride: A theoretical study","authors":"Kun Shen, Junjie Ning, Rui Zhao, Kunqi Gao, Xiangyu Yin, Linxi Hou","doi":"10.1002/qua.27453","DOIUrl":null,"url":null,"abstract":"<p>As one of the most potent greenhouse gases, SF<sub>6</sub> has a significant economic and environmental impact on the purification and recovery of exhaust gases from the semiconductor industry. The adsorption and separation performance of SF<sub>6</sub> on a two-dimensional covalent organic framework TAT-COFs-1-AB with different functional groups (<span></span>SO<sub>3</sub>H, <span></span>Et, <span></span>NH<sub>2</sub>, <span></span>OMe, <span></span>OH, <span></span>H) was investigated by using grand canonical Monte Carlo (GCMC) simulations and density functional theory (DFT) calculations. The results show that the adsorption at low pressure depends on the interactions between the SF<sub>6</sub> and COF frameworks, while at high pressure it is mainly affected by the porosity. The highest adsorption capacity of 8.44 mmol/g (298 K, 100 kPa) is exhibited by TAT-COF-1-AB-H, which has the highest porosity. Chemical functionalization was found to be effective in enhancing the SF<sub>6</sub>/N<sub>2</sub> selectivity. Among all the functionalized COFs, TAT-COF-1-AB-NH<sub>2</sub>, with the highest specific surface area and strong heat of adsorption, showed the highest selectivity. The simulation of self-diffusion also shows consistent results with the GCMC simulation. The findings highlight that the adsorption capacity is influenced by substituent and porosity, with SF<sub>6</sub> showing a consistent preference for adsorption at hollow sites, as evidenced by binding energy and charge transfer analyses.</p>","PeriodicalId":182,"journal":{"name":"International Journal of Quantum Chemistry","volume":null,"pages":null},"PeriodicalIF":2.3000,"publicationDate":"2024-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"International Journal of Quantum Chemistry","FirstCategoryId":"92","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/qua.27453","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
As one of the most potent greenhouse gases, SF6 has a significant economic and environmental impact on the purification and recovery of exhaust gases from the semiconductor industry. The adsorption and separation performance of SF6 on a two-dimensional covalent organic framework TAT-COFs-1-AB with different functional groups (SO3H, Et, NH2, OMe, OH, H) was investigated by using grand canonical Monte Carlo (GCMC) simulations and density functional theory (DFT) calculations. The results show that the adsorption at low pressure depends on the interactions between the SF6 and COF frameworks, while at high pressure it is mainly affected by the porosity. The highest adsorption capacity of 8.44 mmol/g (298 K, 100 kPa) is exhibited by TAT-COF-1-AB-H, which has the highest porosity. Chemical functionalization was found to be effective in enhancing the SF6/N2 selectivity. Among all the functionalized COFs, TAT-COF-1-AB-NH2, with the highest specific surface area and strong heat of adsorption, showed the highest selectivity. The simulation of self-diffusion also shows consistent results with the GCMC simulation. The findings highlight that the adsorption capacity is influenced by substituent and porosity, with SF6 showing a consistent preference for adsorption at hollow sites, as evidenced by binding energy and charge transfer analyses.
期刊介绍:
Since its first formulation quantum chemistry has provided the conceptual and terminological framework necessary to understand atoms, molecules and the condensed matter. Over the past decades synergistic advances in the methodological developments, software and hardware have transformed quantum chemistry in a truly interdisciplinary science that has expanded beyond its traditional core of molecular sciences to fields as diverse as chemistry and catalysis, biophysics, nanotechnology and material science.