Junjie Song, Xiang Li, Xiaocheng Xu, Junbo Lu, Hanshi Hu, Jun Li
{"title":"开发锕系元素（An3+）溶液的多尺度力场。","authors":"Junjie Song, Xiang Li, Xiaocheng Xu, Junbo Lu, Hanshi Hu, Jun Li","doi":"10.1021/acs.jctc.4c01048","DOIUrl":null,"url":null,"abstract":"<p><p>A multiscale force field (FF) is developed for an aqueous solution of trivalent actinide cations An<sup>3+</sup> (An = U, Np, Pu, Am, Cm, Bk, and Cf) by using a 12-6-4 Lennard-Jones type potential considering ion-induced dipole interaction. Potential parameters are rigorously and automatically optimized by the meta-multilinear interpolation parametrization (meta-MIP) algorithm via matching the experimental properties, including ion-oxygen distance (IOD) and coordination number (CN) in the first solvation shell and hydration free energy (HFE). The water solvent models incorporate an especially developed polar coarse-grained (CG) water scheme named PW32 and three widely used all-atom (AA) level SPC/E, TIP3P, and TIP4P water schemes. Each PW32 is modeled as two bonded beads to represent three neighboring water molecules, the simulation efficiency of which is 1 to 2 orders of magnitude higher than that of AA waters. The newly developed FF shows high accuracy and transferability in reproducing the IOD, CN, and HFE of An<sup>3+</sup>. The molecular structure and water exchange dynamics of the first An<sup>3+</sup> hydration shell and the ionic (van der Waals) radii are reinvestigated in this work. Moreover, the new FF can readily be transferred to other popular FFs, as it has practicably predicted the permeability of An<sup>3+</sup> in a graphene oxide filter within the framework of optimized potentials for liquid simulations (OPLS)-AA FF. It holds promise for applications in exploring actinide aqueous solutions with multiscale computational overhead.</p>","PeriodicalId":45,"journal":{"name":"Journal of Chemical Theory and Computation","volume":" ","pages":"9799-9813"},"PeriodicalIF":5.7000,"publicationDate":"2024-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Development of Multiscale Force Field for Actinide (An<sup>3+</sup>) Solutions.\",\"authors\":\"Junjie Song, Xiang Li, Xiaocheng Xu, Junbo Lu, Hanshi Hu, Jun Li\",\"doi\":\"10.1021/acs.jctc.4c01048\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>A multiscale force field (FF) is developed for an aqueous solution of trivalent actinide cations An<sup>3+</sup> (An = U, Np, Pu, Am, Cm, Bk, and Cf) by using a 12-6-4 Lennard-Jones type potential considering ion-induced dipole interaction. Potential parameters are rigorously and automatically optimized by the meta-multilinear interpolation parametrization (meta-MIP) algorithm via matching the experimental properties, including ion-oxygen distance (IOD) and coordination number (CN) in the first solvation shell and hydration free energy (HFE). The water solvent models incorporate an especially developed polar coarse-grained (CG) water scheme named PW32 and three widely used all-atom (AA) level SPC/E, TIP3P, and TIP4P water schemes. Each PW32 is modeled as two bonded beads to represent three neighboring water molecules, the simulation efficiency of which is 1 to 2 orders of magnitude higher than that of AA waters. The newly developed FF shows high accuracy and transferability in reproducing the IOD, CN, and HFE of An<sup>3+</sup>. The molecular structure and water exchange dynamics of the first An<sup>3+</sup> hydration shell and the ionic (van der Waals) radii are reinvestigated in this work. Moreover, the new FF can readily be transferred to other popular FFs, as it has practicably predicted the permeability of An<sup>3+</sup> in a graphene oxide filter within the framework of optimized potentials for liquid simulations (OPLS)-AA FF. It holds promise for applications in exploring actinide aqueous solutions with multiscale computational overhead.</p>\",\"PeriodicalId\":45,\"journal\":{\"name\":\"Journal of Chemical Theory and Computation\",\"volume\":\" \",\"pages\":\"9799-9813\"},\"PeriodicalIF\":5.7000,\"publicationDate\":\"2024-11-26\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Chemical Theory and Computation\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.jctc.4c01048\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2024/11/13 0:00:00\",\"PubModel\":\"Epub\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Chemical Theory and Computation","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acs.jctc.4c01048","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2024/11/13 0:00:00","PubModel":"Epub","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Development of Multiscale Force Field for Actinide (An3+) Solutions.
A multiscale force field (FF) is developed for an aqueous solution of trivalent actinide cations An3+ (An = U, Np, Pu, Am, Cm, Bk, and Cf) by using a 12-6-4 Lennard-Jones type potential considering ion-induced dipole interaction. Potential parameters are rigorously and automatically optimized by the meta-multilinear interpolation parametrization (meta-MIP) algorithm via matching the experimental properties, including ion-oxygen distance (IOD) and coordination number (CN) in the first solvation shell and hydration free energy (HFE). The water solvent models incorporate an especially developed polar coarse-grained (CG) water scheme named PW32 and three widely used all-atom (AA) level SPC/E, TIP3P, and TIP4P water schemes. Each PW32 is modeled as two bonded beads to represent three neighboring water molecules, the simulation efficiency of which is 1 to 2 orders of magnitude higher than that of AA waters. The newly developed FF shows high accuracy and transferability in reproducing the IOD, CN, and HFE of An3+. The molecular structure and water exchange dynamics of the first An3+ hydration shell and the ionic (van der Waals) radii are reinvestigated in this work. Moreover, the new FF can readily be transferred to other popular FFs, as it has practicably predicted the permeability of An3+ in a graphene oxide filter within the framework of optimized potentials for liquid simulations (OPLS)-AA FF. It holds promise for applications in exploring actinide aqueous solutions with multiscale computational overhead.
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The Journal of Chemical Theory and Computation invites new and original contributions with the understanding that, if accepted, they will not be published elsewhere. Papers reporting new theories, methodology, and/or important applications in quantum electronic structure, molecular dynamics, and statistical mechanics are appropriate for submission to this Journal. Specific topics include advances in or applications of ab initio quantum mechanics, density functional theory, design and properties of new materials, surface science, Monte Carlo simulations, solvation models, QM/MM calculations, biomolecular structure prediction, and molecular dynamics in the broadest sense including gas-phase dynamics, ab initio dynamics, biomolecular dynamics, and protein folding. The Journal does not consider papers that are straightforward applications of known methods including DFT and molecular dynamics. The Journal favors submissions that include advances in theory or methodology with applications to compelling problems.
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