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Comparatively, electrostatic interactions from ions in solutions are mostly shielded by solvent or counter\u2010ion shells, creating negligible catalytic effects. Herein, we discovered that the interfacial Li<jats:sup>+<\/jats:sup> cations accumulated on electrodes catalyze the selective water\u2010involved O<jats:sub>2<\/jats:sub> electro\u2010reduction into peroxide anion (OOH<jats:sup>\u2212<\/jats:sup>), forming an active side\u2010on Li<jats:sup>+<\/jats:sup>\u2013OOH<jats:sup>\u2212<\/jats:sup> complex via short\u2010range electrostatic interaction. This complex reduces the O<jats:sub>2<\/jats:sub> reduction energy barrier and increases the nucleophilicity, expediting the aerobic oxygenation of ketones. Aside from trapping active intermediates, Li<jats:sup>+<\/jats:sup> cations also attract the excessive water dipoles to prevent them from quenching the active Li<jats:sup>+<\/jats:sup>\u2013OOH<jats:sup>\u2212<\/jats:sup> complex. By using probe\u2010assisted quantitative methods, we demonstrated the unique under\u2010coordinative characteristics of interfacial Li<jats:sup>+<\/jats:sup> for interacting with reaction intermediates, and the effective concentration of under\u2010coordinative Li<jats:sup>+<\/jats:sup> on the interface is an order of magnitude higher than in the bulk solution. 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