Ion-neutral clustering alters gas-phase hydrogen-deuterium exchange rates

Haley M. Schramm, Tomoya Tamadate, Christopher J. Hogan, Brian H. Clowers

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The rates and mechanisms of chemical reactions that occur at a phase boundary often differ considerably from chemical behavior in bulk solution, but remain difficult to quantify. Ion-neutral interactions are one such class of chemical reactions whose behavior during the nascent stages of solvation differs from bulk solution while occupying critical roles in aerosol formation, atmospheric chemistry, and gas-phase ion separations. Through a gas-phase ion separation technique utilizing a counter-current flow of deuterated vapor, we quantify the degree of hydrogen-deuterium exchange (HDX) and ion-neutral clustering on a series of model chemical systems (i.e. amino acids). By simultaneously quantifying the degree of vapor association and HDX, the effects of cluster formation on reaction kinetics are realized. These results imply that cluster formation cannot be ignored when modeling complex nucleation processes and biopolymer structural dynamics.

Original languageEnglish (US)
Pages (from-to)4959-4968
Number of pages10
JournalPhysical Chemistry Chemical Physics
Issue number6
StatePublished - Jan 24 2023

Bibliographical note

Funding Information:
The contributions by C. Hogan and T. Tamadate were supported by US NSF 2002852. H. Schramm and B. Clowers acknowledge the support provided by US NSF 2003042. We would also like to thank Dr Stephen Valentine for helpful discussions regarding observations of multiple exchange rates within the drift tube ion mobility experiment.

Publisher Copyright:
© 2023 The Royal Society of Chemistry.

PubMed: MeSH publication types

  • Journal Article


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