Shear-activation of mechanochemical reactions through molecular deformation.
Journal
Scientific reports
ISSN: 2045-2322
Titre abrégé: Sci Rep
Pays: England
ID NLM: 101563288
Informations de publication
Date de publication:
05 Feb 2024
05 Feb 2024
Historique:
received:
25
10
2023
accepted:
30
01
2024
medline:
6
2
2024
pubmed:
6
2
2024
entrez:
5
2
2024
Statut:
epublish
Résumé
Mechanical stress can directly activate chemical reactions by reducing the reaction energy barrier. A possible mechanism of such mechanochemical activation is structural deformation of the reactant species. However, the effect of deformation on the reaction energetics is unclear, especially, for shear stress-driven reactions. Here, we investigated shear stress-driven oligomerization reactions of cyclohexene on silica using a combination of reactive molecular dynamics simulations and ball-on-flat tribometer experiments. Both simulations and experiments captured an exponential increase in reaction yield with shear stress. Elemental analysis of ball-on-flat reaction products revealed the presence of oxygen in the polymers, a trend corroborated by the simulations, highlighting the critical role of surface oxygen atoms in oligomerization reactions. Structural analysis of the reacting molecules in simulations indicated the reactants were deformed just before a reaction occurred. Quantitative evidence of shear-induced deformation was established by comparing bond lengths in cyclohexene molecules in equilibrium and prior to reactions. Nudged elastic band calculations showed that the deformation had a small effect on the transition state energy but notably increased the reactant state energy, ultimately leading to a reduction in the energy barrier. Finally, a quantitative relationship was developed between molecular deformation and energy barrier reduction by mechanical stress.
Identifiants
pubmed: 38316829
doi: 10.1038/s41598-024-53254-2
pii: 10.1038/s41598-024-53254-2
doi:
Types de publication
Journal Article
Langues
eng
Sous-ensembles de citation
IM
Pagination
2992Subventions
Organisme : National Science Foundation
ID : CMMI-2038499
Organisme : National Science Foundation
ID : CMMI-2038494
Organisme : National Science Foundation
ID : CMMI-2038494
Organisme : National Science Foundation
ID : CMMI-2038499
Informations de copyright
© 2024. The Author(s).
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