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Frustrated Solvation Structures Can Enhance Electron Transfer Rates.

Richard C Remsing1, Ian G McKendry1, Daniel R Strongin1

  • 1Institute for Computational Molecular Science, ‡Department of Chemistry, and §Center for the Computational Design of Functional Layered Materials, Temple University , Philadelphia, Pennsylvania 19122, United States.

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Highly ordered water structures near polar surfaces can frustrate hydrogen bonds. This frustration enhances ion-surface electron transfer rates, impacting water oxidation catalysis in manganese dioxide materials.

Keywords:
Marcus theoryXY modelbirnessitecatalysisconfinementfluctuationsquenched disorder

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Area of Science:

  • Surface Chemistry
  • Catalysis
  • Physical Chemistry

Background:

  • Polar surfaces strongly interact with water, forming ordered interfacial hydration structures.
  • This ordering can lead to frustrated hydrogen bond networks, especially with solutes like cations.
  • Frustrated hydration structures are observed when cations are confined by manganese dioxide sheets.

Purpose of the Study:

  • To investigate the effects of frustrated hydration structures on ion-surface electron transfer.
  • To understand how cation confinement influences electron transfer dynamics at the water-catalyst interface.
  • To explore the link between cation hydration frustration and water oxidation rates.

Main Methods:

  • Computational study of cation hydration between manganese dioxide sheets.
  • Analysis of ion-surface electron transfer using Marcus theory as a baseline.
  • Development of a charge frustrated XY model to generalize the phenomenon.

Main Results:

  • Frustrated hydration structures significantly enhance energy gap fluctuations.
  • These fluctuations increase electron transfer rates beyond predictions from Marcus theory.
  • The phenomenon of enhanced fluctuations due to frustration is general and can be modeled using topological defects.

Conclusions:

  • Frustrated hydration structures play a critical role in modulating electron transfer at interfaces.
  • The findings explain experimental observations linking water oxidation rates to cation charge and catalyst oxidation state.
  • This work provides fundamental insights into interfacial water behavior and its impact on catalytic processes.