In this study, we employed classic electrochemical techniques including cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) to perform electrochemical characterization on atomic-level single-crystal TiO2 electrodes and extract capacitive and resistive properties of single-crystal TiO2 electrode/solution interface in KCl and KCl/K3PO4 at various pH levels. The lattice structure and crystal appearance were characterized using X-ray diffractometry (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and Raman spectroscopy to facilitate the in-dep...