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The recent application of electrosprays to characterize the air-waterinterface, along with the reports on dramatically accelerated chemicalreactions in aqueous electrosprays, have sparked a broad interest. Herein, wereport on complementary laboratory and in silico experiments tracking theoligomerization of isoprene, an important biogenic gas, in electrosprays andisoprene-water emulsions to differentiate the contributions of interfacialeffects from those of high voltages leading to charge-separation andconcentration of reactants in the electrosprays. To this end, we employedelectrospray ionization mass spectrometry, proton nuclear magnetic resonance,and quantum mechanical simulations. We found that the oligomerization ofisoprene in aqueous electrosprays involved minimally hydrated and highlyreactive hydronium ions. Those conditions, however, are non-existent atpristine air-water interfaces and oil-water emulsions under normal temperatureand pressure. Thus, electrosprays should be complemented with surface-specificplatforms and theoretical methods to reliably investigate chemistries at thepristine air-water interface.

The Chemical Reactions in Electrosprays of Water Do Not Always Correspond to Those at the Pristine Air-Water Interface