Advanced Self‐Bias Photocatalytic System for U(VI) and Tetracycline Hydrochloride Removal Coupled with Electricity Generation via Ti₃C₂@Cu1.96S/TiO₂‐Si Heterojunction

The pervasive prevalence of organic pollutants in water bodies presents major obstacles to traditional uranic recovery methods. Herein, a spontaneous photocatalytic reaction system (SPRS) integrating a Ti 3 C 2 @Cu 1.96 S heterojunction cathode and a TiO 2 nanoarray (TNR)/Si photovoltaic cell (Si PVC) photoanode, achieving simultaneous U(VI) reduction, pollutant degradation, and electricity generation, is designed. The functional groups coupled with Cu + /S 2− redox‐active sites on the Ti 3 C 2 email>@Cu 1.96 S heterojunction facilitate multisite adsorption and cascade reduction of U(VI), endowing the SPRS with exceptional cyclability and practical potential. Under simulated sunlight irradiation, the SPRS achieves remarkable removal efficiencies of 96.7% for UO 2 2+ and 97.7% for tetracycline hydrochloride (TCH). Notably, U(VI) elimination efficiency exceeds 90.2% across diverse organic matrices, demonstrating robust anti‐interference capability. The system maintains superior performance retention (>93.9% for U(VI) and >94.3% for TCH) after 15 consecutive cycles. Crucially, under natural solar illumination, the removal efficiencies surpass 95.8% for both contaminants, confirming practical applicability. This work provides groundbreaking insights into the resource‐oriented treatment paradigm for radioactive wastewater and organic‐polluted water bodies through integrated energy‐water nexus management.