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

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:

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

^[1]

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

Publication Date:: Thu Oct 17 00:00:00 EDT 2019

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.

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                    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

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                    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.

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@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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Title: Droplet Imbibition Enables Nonequilibrium Interfacial Reactions in Charged Microdroplets

Abstract

Citation Formats

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journal, June 1984

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journal, March 1995

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Role of liquid droplet surface diffusion in the vapor‐liquid‐solid whisker growth mechanism
journal, August 1994

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