| Autor: |
Kanhaiya K; Department of Chemical and Biological Engineering, University of Colorado at Boulder, Boulder, Colorado 80309, United States., Nathanson M; Department of Chemical and Biological Engineering, University of Colorado at Boulder, Boulder, Colorado 80309, United States., In 't Veld PJ; BASF SE, Molecular Modeling & Drug Discovery, Carl Bosch Str. 38, 67056 Ludwigshafen, Germany., Zhu C; Department of Chemical and Biological Engineering, University of Colorado at Boulder, Boulder, Colorado 80309, United States., Nikiforov I; Department of Aerospace Engineering and Mechanics, University of Minnesota, Minneapolis, Minnesota 55455, United States., Tadmor EB; Department of Aerospace Engineering and Mechanics, University of Minnesota, Minneapolis, Minnesota 55455, United States., Choi YK; Department of Biological Sciences, Lehigh University, Bethlehem, Pennsylvania 18015, United States., Im W; Department of Biological Sciences, Lehigh University, Bethlehem, Pennsylvania 18015, United States., Mishra RK; BASF SE, Molecular Modeling & Drug Discovery, Carl Bosch Str. 38, 67056 Ludwigshafen, Germany., Heinz H; Department of Chemical and Biological Engineering, University of Colorado at Boulder, Boulder, Colorado 80309, United States. |
| Jazyk: |
angličtina |
| Zdroj: |
Journal of chemical theory and computation [J Chem Theory Comput] 2023 Nov 28; Vol. 19 (22), pp. 8293-8322. Date of Electronic Publication: 2023 Nov 14. |
| DOI: |
10.1021/acs.jctc.3c00750 |
| Abstrakt: |
The simulation of metals, oxides, and hydroxides can accelerate the design of therapeutics, alloys, catalysts, cement-based materials, ceramics, bioinspired composites, and glasses. Here we introduce the INTERFACE force field (IFF) and surface models for α-Al 2 O 3 , α-Cr 2 O 3 , α-Fe 2 O 3 , NiO, CaO, MgO, β-Ca(OH) 2 , β-Mg(OH) 2 , and β-Ni(OH) 2 . The force field parameters are nonbonded, including atomic charges for Coulomb interactions, Lennard-Jones (LJ) potentials for van der Waals interactions with 12-6 and 9-6 options, and harmonic bond stretching for hydroxide ions. The models outperform DFT calculations and earlier atomistic models (Pedone, ReaxFF, UFF, CLAYFF) up to 2 orders of magnitude in reliability, compatibility, and interpretability due to a quantitative representation of chemical bonding consistent with other compounds across the periodic table and curated experimental data for validation. The IFF models exhibit average deviations of 0.2% in lattice parameters, <10% in surface energies (to the extent known), and 6% in bulk moduli relative to experiments. The parameters and models can be used with existing parameters for solvents, inorganic compounds, organic compounds, biomolecules, and polymers in IFF, CHARMM, CVFF, AMBER, OPLS-AA, PCFF, and COMPASS, to simulate bulk oxides, hydroxides, electrolyte interfaces, and multiphase, biological, and organic hybrid materials at length scales from atoms to micrometers. The nonbonded character of the models also enables the analysis of mixed oxides, glasses, and certain chemical reactions, and well-performing nonbonded models for silica phases, SiO 2 , are introduced. Automated model building is available in the CHARMM-GUI Nanomaterial Modeler. We illustrate applications of the models to predict the structure of mixed oxides, and energy barriers of ion migration, as well as binding energies of water and organic molecules in outstanding agreement with experimental data and calculations at the CCSD(T) level. Examples of model building for hydrated, pH-sensitive oxide surfaces to simulate solid-electrolyte interfaces are discussed. |
| Databáze: |
MEDLINE |
| Externí odkaz: |
|
