Electrical double layer and capacitance of TiO2 electrolyte interfaces from first principles simulations Article Swipe
YOU?
·
· 2024
· Open Access
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· DOI: https://doi.org/10.48550/arxiv.2404.00167
The electrical double layer (EDL) at aqueous solution-metal oxide interfaces critically affects many fundamental processes in electrochemistry, geology and biology, yet understanding its microscopic structure is challenging for both theory and experiments. Here we employ ab initio-based machine learning potentials including long-range electrostatics in large-scale atomistic simulations of the EDL at the TiO2-electrolyte interface. Our simulations provide a molecular-scale picture of the EDL that demonstrates the limitations of standard mean-field models. We further develop a method to accurately calculate the electrostatic potential drop at the interface. The computed capacitance originating from the adsorbed charges and the potential drop agrees with experiments, supporting the reliability of our description of the EDL. The larger interfacial capacitance of basic relative to acidic solutions originates from the higher affinity of the cations for the oxide surface and gives rise to distinct charging mechanisms on negative and positive surfaces.
Related Topics
- Type
- preprint
- Language
- en
- Landing Page
- http://arxiv.org/abs/2404.00167
- https://arxiv.org/pdf/2404.00167
- OA Status
- green
- Cited By
- 2
- Related Works
- 10
- OpenAlex ID
- https://openalex.org/W4393754236
Raw OpenAlex JSON
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https://openalex.org/W4393754236Canonical identifier for this work in OpenAlex
- DOI
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https://doi.org/10.48550/arxiv.2404.00167Digital Object Identifier
- Title
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Electrical double layer and capacitance of TiO2 electrolyte interfaces from first principles simulationsWork title
- Type
-
preprintOpenAlex work type
- Language
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enPrimary language
- Publication year
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2024Year of publication
- Publication date
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2024-03-29Full publication date if available
- Authors
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Chunyi Zhang, Marcos F. Calegari Andrade, Zachary K. Goldsmith, Abhinav S. Raman, Yifan Li, Pablo M. Piaggi, Xifan Wu, Roberto Car, Annabella SelloniList of authors in order
- Landing page
-
https://arxiv.org/abs/2404.00167Publisher landing page
- PDF URL
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https://arxiv.org/pdf/2404.00167Direct link to full text PDF
- Open access
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YesWhether a free full text is available
- OA status
-
greenOpen access status per OpenAlex
- OA URL
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https://arxiv.org/pdf/2404.00167Direct OA link when available
- Concepts
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Capacitance, Electrolyte, Materials science, Layer (electronics), Double layer (biology), Engineering physics, Composite material, Chemistry, Physics, Electrode, Physical chemistryTop concepts (fields/topics) attached by OpenAlex
- Cited by
-
2Total citation count in OpenAlex
- Citations by year (recent)
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2025: 1, 2024: 1Per-year citation counts (last 5 years)
- Related works (count)
-
10Other works algorithmically related by OpenAlex
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| abstract_inverted_index.electrochemistry, | 16 |
| cited_by_percentile_year | |
| countries_distinct_count | 0 |
| institutions_distinct_count | 9 |
| citation_normalized_percentile |