• • Cyano-functionalized C3N4/ZnIn2S4 (CCN/ZIS) achieved a maximum adsorption capacity of 123.65 mg·g−1 for U(VI), significantly enhancing selective enrichment from wastewater.
• • Under visible light, CCN/ZIS removed over 95% of U(VI) within 10 minutes, representing a 20-fold improvement over pristine materials, enabling rapid treatment.
• • The material maintained stable performance in the presence of high concentrations of CO3^2− and F−, demonstrating robustness against common interfering ions in real uranium mining wastewater.
• • Quenching experiments confirmed that e− and ·O2− are the primary reactive species driving U(VI) reduction, providing mechanistic insight for optimizing photocatalytic systems.
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