Enhanced Photocatalytic Degradation of Thiocyanate Using an FCN/TiO2 Heterojunction: Performance, Mechanism, and Real Wastewater Application
摘要
The increasing environmental threat posed by stable and toxic thiocyanate (SCN−) in hydrometallurgical wastewater highlights the need for efficient and environmentally friendly removal technologies. Here, a folded carbon nitride (FCN)/TiO2 (TFCN) composite photocatalyst was synthesized via a sol–gel method and systematically optimized (TiO2: FCN = 1:4, 180 °C calcination for 18 h). The TFCN composite exhibits an outstanding specific surface area (71.77 m2/g) and exceptional photocatalytic performance. Under the best tested conditions (initial SCN− concentration = 200 mg/L, TFCN dosage = 0.5 g, pH = 12, LED wavelength = 405 nm, LED power = 15 W), 98% SCN− degradation efficiency was achieved. Free radical scavenging experiments and electron paramagnetic resonance (EPR) studies indicated that superoxide radicals (·O2−) and holes (h+) are the dominant reactive species responsible for the degradation. The enhanced activity is tentatively associated with a proposed Type-II-like interfacial charge-transfer pathway between FCN and TiO2, which may facilitate photogenerated charge separation. Intermediate-product analysis showed that SCN− was converted mainly into liquid-phase inorganic products, including SO42−, CO32−, and NH4+. Meanwhile, total cyanide exhibited a transient rise–fall profile during the reaction, suggesting the formation and subsequent conversion of cyanide-related intermediates under continued irradiation. This result indicates efficient SCN− conversion while limiting the accumulation of cyanide-related species in the measured liquid phase. This work presents TFCN as a promising photocatalyst for SCN− abatement and provides cautious mechanistic insight into photo-driven SCN− conversion in both simulated and real wastewater systems.