Droplet Imbibition Enables Nonequilibrium Interfacial Reactions in Charged Microdroplets
Abstract
A droplet imbibition experiment is proposed to study interfacial effects, which appears to be the main factor influencing reaction acceleration in charged microdroplets produced by electrospray ionization (ESI). One reagent is deposited onto the surface of rapidly moving microdroplets containing the second reagent to be reacted. In this manner, reactions are hindered from reaching equilibrium and monitored in real time by mass spectrometry. We demonstrated this phenomenon using Katritzky chemistry, which is known to proceed either by the solvent-stabilized 2H-pyran intermediate or via the surface-active pseudobase intermediate. Additionally, comparisons with reactions performed using ESI show obvious surface effects in favor of the droplet imbibition experiment. By keeping reactant mole ratio constant, it was demonstrated that similar interfacial effects observed in the droplet imbibition experiment can be reached by allowing ESI microdroplets containing premixed reagents to traverse a distance >16 mm. At such spray distance, molecular diffusion and droplet lifetime become comparable allowing reactants to be enriched at droplet surface. Reactions were also conducted in rapid mixing, theta capillary-based droplets, which showed markedly reduced yields compared with the interfacial droplet imbibition experiment.
- Authors:
-
- The Ohio State Univ., Columbus, OH (United States)
- Publication Date:
- Research Org.:
- The Ohio State Univ., Columbus, OH (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1802825
- Grant/Contract Number:
- SC0016044
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Langmuir
- Additional Journal Information:
- Journal Volume: 35; Journal Issue: 45; Journal ID: ISSN 0743-7463
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Chemical reactions; Adducts; Liquids; Cations; Ions
Citation Formats
Sahraeian, Taghi, Kulyk, Dmytro S., and Badu-Tawiah, Abraham K. Droplet Imbibition Enables Nonequilibrium Interfacial Reactions in Charged Microdroplets. United States: N. p., 2019.
Web. doi:10.1021/acs.langmuir.9b02439.
Sahraeian, Taghi, Kulyk, Dmytro S., & Badu-Tawiah, Abraham K. Droplet Imbibition Enables Nonequilibrium Interfacial Reactions in Charged Microdroplets. United States. https://doi.org/10.1021/acs.langmuir.9b02439
Sahraeian, Taghi, Kulyk, Dmytro S., and Badu-Tawiah, Abraham K. Thu .
"Droplet Imbibition Enables Nonequilibrium Interfacial Reactions in Charged Microdroplets". United States. https://doi.org/10.1021/acs.langmuir.9b02439. https://www.osti.gov/servlets/purl/1802825.
@article{osti_1802825,
title = {Droplet Imbibition Enables Nonequilibrium Interfacial Reactions in Charged Microdroplets},
author = {Sahraeian, Taghi and Kulyk, Dmytro S. and Badu-Tawiah, Abraham K.},
abstractNote = {A droplet imbibition experiment is proposed to study interfacial effects, which appears to be the main factor influencing reaction acceleration in charged microdroplets produced by electrospray ionization (ESI). One reagent is deposited onto the surface of rapidly moving microdroplets containing the second reagent to be reacted. In this manner, reactions are hindered from reaching equilibrium and monitored in real time by mass spectrometry. We demonstrated this phenomenon using Katritzky chemistry, which is known to proceed either by the solvent-stabilized 2H-pyran intermediate or via the surface-active pseudobase intermediate. Additionally, comparisons with reactions performed using ESI show obvious surface effects in favor of the droplet imbibition experiment. By keeping reactant mole ratio constant, it was demonstrated that similar interfacial effects observed in the droplet imbibition experiment can be reached by allowing ESI microdroplets containing premixed reagents to traverse a distance >16 mm. At such spray distance, molecular diffusion and droplet lifetime become comparable allowing reactants to be enriched at droplet surface. Reactions were also conducted in rapid mixing, theta capillary-based droplets, which showed markedly reduced yields compared with the interfacial droplet imbibition experiment.},
doi = {10.1021/acs.langmuir.9b02439},
journal = {Langmuir},
number = 45,
volume = 35,
place = {United States},
year = {Thu Oct 17 00:00:00 EDT 2019},
month = {Thu Oct 17 00:00:00 EDT 2019}
}
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