Electrical double layer and capacitance of TiO2 electrolyte interfaces from first principles simulations

Understand

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.