Direct Experimental Evidence for Markedly Enhanced Surface Proton Activity Inherent to Water Ice

The Journal of Physical Chemistry Letters
Fumiaki KatoYoshiyasu Matsumoto

Abstract

Autoionization and subsequent proton transfer processes determine the proton activity inherent to water molecular systems. In this study, we provide direct experimental evidence that the proton activity is markedly enhanced at the surface of crystalline ice, on the basis of simultaneous observation of H/D exchange of water molecules at the surface and in the interior of well-defined double-layer ice films composed of H2O and D2O. Thermal desorption mass spectrometry showed clear signatures derived from the surface H/D exchange equilibrium, whereas infrared absorption spectroscopy indicated no appreciable H/D exchange progress in the interior. Detailed kinetic analyses revealed that the rate of H/D exchange at the surface is at least three orders of magnitude higher than in the interior. This drastic enhancement of the proton activity suggests an extremely high concentration of surface hydrated protons in comparison with those in the bulk. Our results also highlight the impact of the local hydrogen-bond structure on the autoionization event of water molecules.

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Citations

Jun 25, 2020·Physical Chemistry Chemical Physics : PCCP·Toshiki Sugimoto, Yoshiyasu Matsumoto
Sep 24, 2020·The Journal of Chemical Physics·Maurice de Koning
Jul 27, 2021·The Journal of Physical Chemistry. B·Du Hyeong Lee, Heon Kang

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