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Molecular-level insight into interfacial water at buried electrode interfacesis essential in elucidating many phenomena of electrochemistry, butspectroscopic probing of the buried interfaces remains challenging. Here, usingsurface-specific vibrational spectroscopy, we probe and identify theinterfacial water orientation and interfacial electric field at the calciumfluoride (CaF2)-supported electrified graphene/water interface under appliedpotentials. Our data shows that the water orientation changes drastically atnegative potentials (<-0.03 V vs. Pd/H2), from O-H group pointing down towardsbulk solution to pointing up away from the bulk solution, which arises fromcharging/discharging not of the graphene but of the CaF2 substrate. Thepotential-dependent spectra are nearly identical to the pH-dependent spectra,evidencing that the applied potentials change the local pH (more than five pHunits) near the graphene electrode even at a current density below 1 microampper square centimeter. Our work provides molecular-level insights into thedissociation and reorganization of interfacial water on anelectrode/electrolyte interface.

Surface-specific vibrational spectroscopy of interfacial water reveals large pH change near graphene electrode at low current densities