Efficient Assessment of 'Instantaneous pK' Values from Molecular Dynamics Simulations.
crystal dissociation
molecular simulation
pK prediction
precipitate-solvent interfaces
solute aggregates
Journal
Chemphyschem : a European journal of chemical physics and physical chemistry
ISSN: 1439-7641
Titre abrégé: Chemphyschem
Pays: Germany
ID NLM: 100954211
Informations de publication
Date de publication:
05 Nov 2023
05 Nov 2023
Historique:
revised:
30
10
2023
received:
12
07
2023
pubmed:
6
11
2023
medline:
6
11
2023
entrez:
6
11
2023
Statut:
aheadofprint
Résumé
We present a molecular simulation approach to studying the role of local and momentary molecular environment for potential acid-base reactions. For this, we combine thermodynamic considerations on the pK of ionic species with rapid sampling of energy changes related to (de)protonation. Using dispersed carbonate ions in water as a reference, our approach aims at the fast assessment of the momentary protonation energy, and thus the 'instantaneous pK', of calcium-carbonate ion aggregates. The latter include transient complexes that are elusive to long sampling runs. This motivated the elaboration of approximate, yet particularly fast assessable sampling strategies. Along this line, we were able to characterize instantaneous pK values at a statistical accuracy of 0.4 pK units within sampling runs of only 10 ps duration, whereas statistical errors reduce to 0.1 pK units in 75 ps sampling runs, respectively. This readily enabled the required time resolution for the characterization of [Ca
Identifiants
pubmed: 37927201
doi: 10.1002/cphc.202300489
doi:
Types de publication
Journal Article
Langues
eng
Sous-ensembles de citation
IM
Pagination
e202300489Subventions
Organisme : Procter & Gamble Inc.
Organisme : Deutsche Forschungsgemeinschaft
ID : ZA 420/14-1
Informations de copyright
© 2023 The Authors. ChemPhysChem published by Wiley-VCH GmbH.
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