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A reactive neural network framework for water-loaded acidic zeolites.
Erlebach, Andreas; Sípka, Martin; Saha, Indranil; Nachtigall, Petr; Heard, Christopher J; Grajciar, Lukás.
Afiliação
  • Erlebach A; Department of Physical and Macromolecular Chemistry, Faculty of Sciences, Charles University, Hlavova 8, 128 43, Prague 2, Czech Republic. andreas.erlebach@natur.cuni.cz.
  • Sípka M; Department of Physical and Macromolecular Chemistry, Faculty of Sciences, Charles University, Hlavova 8, 128 43, Prague 2, Czech Republic.
  • Saha I; Mathematical Institute, Faculty of Mathematics and Physics, Charles University, Sokolovská 83, 186 75, Prague, Czech Republic.
  • Nachtigall P; Department of Physical and Macromolecular Chemistry, Faculty of Sciences, Charles University, Hlavova 8, 128 43, Prague 2, Czech Republic.
  • Heard CJ; Department of Physical and Macromolecular Chemistry, Faculty of Sciences, Charles University, Hlavova 8, 128 43, Prague 2, Czech Republic.
  • Grajciar L; Department of Physical and Macromolecular Chemistry, Faculty of Sciences, Charles University, Hlavova 8, 128 43, Prague 2, Czech Republic.
Nat Commun ; 15(1): 4215, 2024 May 17.
Article em En | MEDLINE | ID: mdl-38760371
ABSTRACT
Under operating conditions, the dynamics of water and ions confined within protonic aluminosilicate zeolite micropores are responsible for many of their properties, including hydrothermal stability, acidity and catalytic activity. However, due to high computational cost, operando studies of acidic zeolites are currently rare and limited to specific cases and simplified models. In this work, we have developed a reactive neural network potential (NNP) attempting to cover the entire class of acidic zeolites, including the full range of experimentally relevant water concentrations and Si/Al ratios. This NNP has the potential to dramatically improve sampling, retaining the (meta)GGA DFT level accuracy, with the capacity for discovery of new chemistry, such as collective defect formation mechanisms at the zeolite surface. Furthermore, we exemplify how the NNP can be used as a basis for further extensions/improvements which include data-efficient adoption of higher-level (hybrid) references via Δ-learning and the acceleration of rare event sampling via automatic construction of collective variables. These developments represent a significant step towards accurate simulations of realistic catalysts under operando conditions.

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Revista: Nat Commun Assunto da revista: BIOLOGIA / CIENCIA Ano de publicação: 2024 Tipo de documento: Article País de afiliação: República Tcheca

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Revista: Nat Commun Assunto da revista: BIOLOGIA / CIENCIA Ano de publicação: 2024 Tipo de documento: Article País de afiliação: República Tcheca