arXiv (Cornell University)
Electrical double layer and capacitance of TiO2 electrolyte interfaces from first principles simulations
March 2024 • Chunyi Zhang, Marcos F. Calegari Andrade, Zachary K. Goldsmith, Abhinav S. Raman, Yifan Li, Pablo M. Piaggi, Xifan Wu, Roberto Car, Annabella Selloni
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 l…