{"title":"粘弹性、无定形和微孔介质中的封闭流体动力学:通过分子模拟和广义朗文方程研究一种角质。","authors":"Kristina Ariskina, Guillaume Galliéro, Amaël Obliger","doi":"10.1063/5.0225299","DOIUrl":null,"url":null,"abstract":"<p><p>We combine the use of molecular dynamics simulations and the generalized Langevin equation to study the diffusion of a fluid adsorbed within kerogen, the main organic phase of shales. As a class of microporous and amorphous materials that can exhibit significant adsorption-induced swelling, the dynamics of the kerogen's microstructure is expected to play an important role in the confined fluid dynamics. This role is investigated by conducting all-atom simulations with or without solid dynamics. Whenever the dynamics coupling between the fluid and solid is accounted for, we show that the fluid dynamics displays some qualitative differences compared to bulk fluids, which can be modulated by the amount of adsorbed fluid owing to adsorption-induced swelling. We highlight that working with the memory kernel, the central time correlation function of the generalized Langevin equation, allows the fingerprint of the dynamics of the solid to appear on that of the fluid. Interestingly, we observe that the memory kernels of fluid diffusion in kerogen qualitatively behave as those of tagged particles in supercooled liquids. We emphasize the importance of reproducing the velocity-force correlation function to validate the memory kernel numerically obtained as confinement enhances the numerical instabilities. This route is interesting as it opens the way for modeling the impact of fluid concentration on the diffusion coefficient in such ultra-confining cases.</p>","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.1000,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Confined fluid dynamics in a viscoelastic, amorphous, and microporous medium: Study of a kerogen by molecular simulations and the generalized Langevin equation.\",\"authors\":\"Kristina Ariskina, Guillaume Galliéro, Amaël Obliger\",\"doi\":\"10.1063/5.0225299\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>We combine the use of molecular dynamics simulations and the generalized Langevin equation to study the diffusion of a fluid adsorbed within kerogen, the main organic phase of shales. As a class of microporous and amorphous materials that can exhibit significant adsorption-induced swelling, the dynamics of the kerogen's microstructure is expected to play an important role in the confined fluid dynamics. This role is investigated by conducting all-atom simulations with or without solid dynamics. Whenever the dynamics coupling between the fluid and solid is accounted for, we show that the fluid dynamics displays some qualitative differences compared to bulk fluids, which can be modulated by the amount of adsorbed fluid owing to adsorption-induced swelling. We highlight that working with the memory kernel, the central time correlation function of the generalized Langevin equation, allows the fingerprint of the dynamics of the solid to appear on that of the fluid. Interestingly, we observe that the memory kernels of fluid diffusion in kerogen qualitatively behave as those of tagged particles in supercooled liquids. We emphasize the importance of reproducing the velocity-force correlation function to validate the memory kernel numerically obtained as confinement enhances the numerical instabilities. This route is interesting as it opens the way for modeling the impact of fluid concentration on the diffusion coefficient in such ultra-confining cases.</p>\",\"PeriodicalId\":15313,\"journal\":{\"name\":\"Journal of Chemical Physics\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":3.1000,\"publicationDate\":\"2024-09-28\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Chemical Physics\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1063/5.0225299\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Chemical Physics","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1063/5.0225299","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Confined fluid dynamics in a viscoelastic, amorphous, and microporous medium: Study of a kerogen by molecular simulations and the generalized Langevin equation.
We combine the use of molecular dynamics simulations and the generalized Langevin equation to study the diffusion of a fluid adsorbed within kerogen, the main organic phase of shales. As a class of microporous and amorphous materials that can exhibit significant adsorption-induced swelling, the dynamics of the kerogen's microstructure is expected to play an important role in the confined fluid dynamics. This role is investigated by conducting all-atom simulations with or without solid dynamics. Whenever the dynamics coupling between the fluid and solid is accounted for, we show that the fluid dynamics displays some qualitative differences compared to bulk fluids, which can be modulated by the amount of adsorbed fluid owing to adsorption-induced swelling. We highlight that working with the memory kernel, the central time correlation function of the generalized Langevin equation, allows the fingerprint of the dynamics of the solid to appear on that of the fluid. Interestingly, we observe that the memory kernels of fluid diffusion in kerogen qualitatively behave as those of tagged particles in supercooled liquids. We emphasize the importance of reproducing the velocity-force correlation function to validate the memory kernel numerically obtained as confinement enhances the numerical instabilities. This route is interesting as it opens the way for modeling the impact of fluid concentration on the diffusion coefficient in such ultra-confining cases.
期刊介绍:
The Journal of Chemical Physics publishes quantitative and rigorous science of long-lasting value in methods and applications of chemical physics. The Journal also publishes brief Communications of significant new findings, Perspectives on the latest advances in the field, and Special Topic issues. The Journal focuses on innovative research in experimental and theoretical areas of chemical physics, including spectroscopy, dynamics, kinetics, statistical mechanics, and quantum mechanics. In addition, topical areas such as polymers, soft matter, materials, surfaces/interfaces, and systems of biological relevance are of increasing importance.
Topical coverage includes:
Theoretical Methods and Algorithms
Advanced Experimental Techniques
Atoms, Molecules, and Clusters
Liquids, Glasses, and Crystals
Surfaces, Interfaces, and Materials
Polymers and Soft Matter
Biological Molecules and Networks.