Defect‐Anchored Pt–Ov–Ti Charge Bridges Enable Iodine‐Mediated Selective Photocatalytic Gold Recovery From Electronic Waste

ABSTRACT Gold is indispensable to modern technologies, yet its supply remains heavily dependent on environmentally intensive primary mining. Rapidly accumulating electronic waste (e‐waste) represents a valuable urban mine, but Au recovery is still constrained by corrosive lixiviants, co‐dissolution of competing metals, and high reagent demand. Herein, defect‐anchored Pt–Ov–Ti charge bridges are proposed to couple photogenerated‐carrier dynamics with iodine redox cycling, achieving 98.25% Au dissolution within 2 h while limiting the co‐dissolution of competing metals to below 0.62%. Multiple lines of evidence indicate that Pt–Ov–Ti sites promote interfacial charge transfer and carrier utilization, enabling hole‐driven I − oxidation and O 2 ‐assisted iodine redox cycling. In situ characterization and theoretical calculations further reveal that Pt–Ov–Ti induces local interfacial redistribution, introduces Pt 5d‐derived frontier states, and enhances iodine species adsorption and charge transfer, enabling reversible interfacial electronic‐state evolution during iodide activation. This pathway enabled the dissolution of 196.04 mg of Au from 1 kg of discarded central processing units (CPUs) with Au accounting for 99.2% of the leached metals, while retaining >95% activity after 10 cycles and supporting catalyst recycling and iodine reuse. This work highlights defect‐associated interfacial charge‐transfer engineering as a promising strategy for directing photogenerated carriers toward selective ligand‐mediated leaching and sustainable precious‐metal recovery.