Nonequilibrium wet–dry cycling acts as a catalyst for chemical reactions

  • Recent experimental studies suggest that wet–dry cycles and coexisting phases can each strongly alter chemical processes. The mechanisms of why and to what degree chemical processes are altered when subjected to evaporation and condensation are unclear. To close this gap, we developed a theoretical framework for nondilute chemical reactions subject to nonequilibrium conditions of evaporation and condensation. We find that such conditions can change the half-time of the product’s yield by more than an order of magnitude, depending on the substrate–solvent interaction. We show that the cycle frequency strongly affects the chemical turnover when the system is maintained out of equilibrium by wet–dry cycles. There exists a resonance behavior in the cycle frequency where the turnover is maximal. This resonance behavior enables wet–dry cycles to select specific chemical reactions, suggesting a potential mechanism for chemical evolution in prebiotic soups at early Earth.

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Metadaten
Author:Ivar Svalheim HaugerudORCiD, Pranay Jaiswal, Christoph A. WeberORCiDGND
URN:urn:nbn:de:bvb:384-opus4-1120985
Frontdoor URLhttps://opus.bibliothek.uni-augsburg.de/opus4/112098
ISSN:1520-6106OPAC
ISSN:1520-5207OPAC
Parent Title (English):The Journal of Physical Chemistry B
Publisher:American Chemical Society (ACS)
Type:Article
Language:English
Year of first Publication:2024
Publishing Institution:Universität Augsburg
Release Date:2024/03/19
Tag:Materials Chemistry; Surfaces, Coatings and Films; Physical and Theoretical Chemistry
Volume:128
Issue:7
First Page:1724
Last Page:1736
DOI:https://doi.org/10.1021/acs.jpcb.3c05824
Institutes:Mathematisch-Naturwissenschaftlich-Technische Fakultät
Mathematisch-Naturwissenschaftlich-Technische Fakultät / Institut für Physik
Mathematisch-Naturwissenschaftlich-Technische Fakultät / Institut für Physik / Lehrstuhl für Theoretische Physik II
Dewey Decimal Classification:5 Naturwissenschaften und Mathematik / 53 Physik / 530 Physik
Licence (German):CC-BY-NC-ND 4.0: Creative Commons: Namensnennung - Nicht kommerziell - Keine Bearbeitung (mit Print on Demand)