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The origins of the pH-dependent kinetics of hydrogen evolution and oxidation reactions on Pt surfaces are unsolved dilemmas that have lasted for over half a century. In this study, surface-enhanced infrared absorption spectroscopy is applied to directly monitor the vibrational behaviors of adsorbed hydrogen atoms and interfacial water molecules on Pt surfaces in a wide pH window from 1.1 to 12.9. For the first time, we successfully measure the pH-dependent changes of hydrogen and water binding strength according to their vibrational wave