Your browser doesn't support javascript.
loading
An Efficient Reactive Force Field without Explicit Coordination Dependence for Studying Caustic Aluminum Chemistry.
Pouvreau, Maxime; Guo, Qing; Wang, Hsiu-Wen; Schenter, Gregory K; Pearce, Carolyn I; Clark, Aurora E; Rosso, Kevin M.
Affiliation
  • Pouvreau M; Pacific Northwest National Laboratory, Richland, Washington 99352, United States.
  • Guo Q; Department of Chemistry, University of Utah, Salt Lake City, Utah 84112, United States.
  • Wang HW; Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States.
  • Schenter GK; Pacific Northwest National Laboratory, Richland, Washington 99352, United States.
  • Pearce CI; Pacific Northwest National Laboratory, Richland, Washington 99352, United States.
  • Clark AE; Department of Chemistry, University of Utah, Salt Lake City, Utah 84112, United States.
  • Rosso KM; Pacific Northwest National Laboratory, Richland, Washington 99352, United States.
J Phys Chem Lett ; 14(30): 6743-6748, 2023 Aug 03.
Article in En | MEDLINE | ID: mdl-37470756
ABSTRACT
Reactive force fields (RFFs) are an expedient approach to sample chemical reaction paths in complex systems, relative to density functional theory. However, there is continued need to improve efficiencies, specifically in systems that have slow transverse degrees of freedom, as in highly viscous and superconcentrated solutions. Here, we present an RFF that is differentiated from current models (e.g., ReaxFF) by omitting explicit dependence on the atom coordination and employing a small parameter set based on Lennard-Jones, Gaussian, and Stillinger-Weber potentials. The model was parametrized from AIMD simulation data and is used to model aluminate reactivity in sodium hydroxide solutions with extensive validation against experimental radial distribution functions, computed free energy profiles for oligomerization, and formation energies. The model enables simulation of early stage Al(OH)3 nucleation which has significant relevance to industrial processing of aluminum and has a computational cost that is reduced by 1 order of magnitude relative to ReaxFF.

Full text: 1 Collection: 01-internacional Database: MEDLINE Language: En Journal: J Phys Chem Lett Year: 2023 Document type: Article Affiliation country: United States

Full text: 1 Collection: 01-internacional Database: MEDLINE Language: En Journal: J Phys Chem Lett Year: 2023 Document type: Article Affiliation country: United States