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Tuning water dissociation at oxide-electrolyte interfaces with electric fields.

Chunyi Zhang1,2, Zheng Yu1, Roberto Car1

  • 1Department of Chemistry, Princeton University, Princeton, NJ 08544.

Proceedings of the National Academy of Sciences of the United States of America
|August 20, 2025
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Summary
This summary is machine-generated.

Electric fields significantly alter water splitting at interfaces, crucial for energy technologies. Machine learning simulations reveal how electric fields control interfacial water dissociation and chemical reactions.

Keywords:
electrochemistrymachine learningmolecular dynamics

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Area of Science:

  • Surface Chemistry
  • Computational Materials Science
  • Electrochemistry

Background:

  • Understanding interfacial water behavior is key for energy applications.
  • Electric fields play a critical role in interfacial chemical reactions.

Purpose of the Study:

  • To investigate the influence of electric fields on water dissociation at heterogeneous interfaces.
  • To elucidate the mechanism of electric-field-controlled interfacial chemical reactions.

Main Methods:

  • Ab initio-based machine learning simulations.
  • Development of a machine-learned collective variable for reaction analysis.
  • Analysis of thousands of water dissociation/recombination events.

Main Results:

  • Small electric field changes significantly alter water dissociation fraction at TiO2-electrolyte interfaces.
  • Free energy difference shows linear dependence on electric field change (1.97 eÅ slope).
  • Electric fields influence local configurations favoring water dissociation, not individual energy barriers.

Conclusions:

  • Electric fields have a pronounced impact on interfacial water dissociation.
  • A mechanism for electric-field-controlled chemical reactions at interfaces is revealed.
  • Findings advance understanding for next-generation energy technologies.