Tailoring the Acidity of Liquid Media with Ionizing Radiation: Rethinking the Acid-Base Correlation beyond pH

Fritsch B, Körner A, Couasnon T, Blukis R, Taherkhani M, Benning LG, Jank M, Spiecker E, Hutzler A (2023)

Publication Type: Journal article

Publication year: 2023

Journal

Journal of Physical Chemistry Letters American Chemical Society

Pages Range: 4644-4651

DOI: 10.1021/acs.jpclett.3c00593

Abstract

Advanced in situ techniques based on electrons and X-rays are increasingly used to gain insights into fundamental processes in liquids. However, probing liquid samples with ionizing radiation changes the solution chemistry under observation. In this work, we show that a radiation-induced decrease in pH does not necessarily correlate to an increase in acidity of aqueous solutions. Thus, pH does not capture the acidity under irradiation. Using kinetic modeling of radiation chemistry, we introduce alternative measures of acidity (radiolytic acidity π* and radiolytic ion product KW*), that account for radiation-induced alterations of both H+ and OH- concentration. Moreover, we demonstrate that adding pH-neutral solutes such as LiCl, LiBr, or LiNO3 can trigger a significant change in π*. This provides a huge parameter space to tailor the acidity for in situ experiments involving ionizing radiation, as present in synchrotron facilities or during liquid-phase electron microscopy.

Authors with CRIS profile

Mehran Taherkhani Lehrstuhl für Elektronische Bauelemente Michael Jank Lehrstuhl für Elektronische Bauelemente Erdmann Spiecker Andreas Hutzler

Additional Organisation(s)

Graduiertenkolleg 1896/2 In situ Mikroskopie mit Elektronen, Röntgenstrahlen und Rastersonden Lehrstuhl für Werkstoffwissenschaften (Mikro- und Nanostrukturforschung) Interdisziplinäres Zentrum, Center for Nanoanalysis and Electron Microscopy (CENEM) Nanoanalysis and Electron Microscopy (CENEM)

Involved external institutions

Forschungszentrum Jülich / Research Centre Jülich (FZJ) DE Germany (DE) Helmholtz-Zentrum Potsdam Deutsches GeoForschungsZentrum - GFZ DE Germany (DE) Helmholtz-Institut Erlangen-Nürnberg für Erneuerbare Energien (HI-ERN) DE Germany (DE)

How to cite

APA:

Fritsch, B., Körner, A., Couasnon, T., Blukis, R., Taherkhani, M., Benning, L.G.,... Hutzler, A. (2023). Tailoring the Acidity of Liquid Media with Ionizing Radiation: Rethinking the Acid-Base Correlation beyond pH. Journal of Physical Chemistry Letters, 4644-4651. https://doi.org/10.1021/acs.jpclett.3c00593

MLA:

Fritsch, Birk, et al. "Tailoring the Acidity of Liquid Media with Ionizing Radiation: Rethinking the Acid-Base Correlation beyond pH." Journal of Physical Chemistry Letters (2023): 4644-4651.

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