Droplet Imbibition Enables Nonequilibrium Interfacial Reactions in Charged Microdroplets

Sahraeian, Taghi; Kulyk, Dmytro S.; Badu-Tawiah, Abraham K.

doi:10.1021/acs.langmuir.9b02439

Title: Droplet Imbibition Enables Nonequilibrium Interfacial Reactions in Charged Microdroplets

Journal Article · Thu Oct 17 00:00:00 UTC 2019 · Langmuir

DOI: https://doi.org/10.1021/acs.langmuir.9b02439 · OSTI ID:1802825

Sahraeian, Taghi ^[1]; Kulyk, Dmytro S. ^[2];

^[2]

The Ohio State Univ., Columbus, OH (United States); OSTI
The Ohio State Univ., Columbus, OH (United States)

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.

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Research Organization:: The Ohio State Univ., Columbus, OH (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0016044

OSTI ID:: 1802825

Journal Information:: Langmuir, Journal Name: Langmuir Journal Issue: 45 Vol. 35; ISSN 0743-7463

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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