Understanding electrochemical interfaces through comparing experimental and computational charge density-potential curves

N Mohandas and S Bawari and JJT Shibuya and S Ghosh and J Mondal and TN Narayanan and A Cuesta, CHEMICAL SCIENCE, 15, 6643-6660 (2024).

DOI: 10.1039/d4sc00746h

Electrode-electrolyte interfaces play a decisive role in electrochemical charge accumulation and transfer processes. Theoretical modelling of these interfaces is critical to decipher the microscopic details of such phenomena. Different force field-based molecular dynamics protocols are compared here in a view to connect calculated and experimental charge density-potential relationships. Platinum-aqueous electrolyte interfaces are taken as a model. The potential of using experimental charge density-potential curves to transform cell voltage into electrode potential in force-field molecular dynamics simulations, and the need for that purpose of developing simulation protocols that can accurately calculate the double-layer capacitance, are discussed. A deep understanding of electrode-electrolyte interfaces requires the development of modelling protocols spanning from the local microscale to system-level macroscopic sizes which can be validated by comparison with high-quality experimental results.

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