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    Separating Convective from Diffusive Mass Transport Mechanisms in Ionic Liquids by Redox Pro-fluorescence Microscopy

    93736.pdf (705.6Kb)
    Access Status
    Open access
    Authors
    Belotti, Mattia
    El-Tahawy, M.M.T.
    Garavelli, M.
    Coote, M.L.
    Iyer, K.S.
    Ciampi, Simone
    Date
    2023
    Type
    Journal Article
    
    Metadata
    Show full item record
    Citation
    Belotti, M. and El-Tahawy, M.M.T. and Garavelli, M. and Coote, M.L. and Iyer, K.S. and Ciampi, S. 2023. Separating Convective from Diffusive Mass Transport Mechanisms in Ionic Liquids by Redox Pro-fluorescence Microscopy. Analytical Chemistry. 95 (26): pp. 9779-9786.
    Source Title
    Analytical Chemistry
    DOI
    10.1021/acs.analchem.3c00168
    ISSN
    0003-2700
    Faculty
    Faculty of Science and Engineering
    School
    School of Molecular and Life Sciences (MLS)
    Funding and Sponsorship
    http://purl.org/au-research/grants/arc/DP220100553
    http://purl.org/au-research/grants/arc/FT190100148
    Remarks

    This document is the Accepted Manuscript version of a Published Work that appeared in final form in Analytical Chemistry, copyright © American Chemical Society, after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.analchem.3c00168.

    URI
    http://hdl.handle.net/20.500.11937/93932
    Collection
    • Curtin Research Publications
    Abstract

    The study of electrochemical reactivity requires analytical techniques capable of probing the diffusion of reactants and products to and from electrified interfaces. Information on diffusion coefficients is often obtained indirectly by modeling current transients and cyclic voltammetry data, but such measurements lack spatial resolution and are accurate only if mass transport by convection is negligible. Detecting and accounting for adventitious convection in viscous and wet solvents, such as ionic liquids, is technically challenging. We have developed a direct, spatiotemporally resolved optical tracking of diffusion fronts which can detect and resolve convective disturbances to linear diffusion. By tracking the movement of an electrode-generated fluorophore, we demonstrate that parasitic gas evolving reactions lead to 10-fold overestimates of macroscopic diffusion coefficients. A hypothesis is put forward linking large barriers to inner-sphere redox reactions, such as hydrogen gas evolution, to the formation of cation-rich overscreening and crowding double layer structures in imidazolium-based ionic liquids.

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