Abstract:A composite adsorption-photocatalyst, Fe/Ti-MIL-NH2, was synthesized via the hydrothermal method and utilized to degrade NDPhA. The Fe/Ti-MIL-NH2 with Fe-Ti molar ratio of 3:1 could degrade more than 84.4% of NDPhA under various conditions, and 95.1% under adding 10 mmol/L HCO3-. Compared to Fe-MIL-NH2, the excellent performance of Fe/Ti-MIL-NH2 (3:1) was attributed to the in situ formation of intimate heterojunctions, which increased the specific surface area (310.2m2/g), accelerated the separation of photogenerated cavity pairs, and inhibited their complexation. Both surface adsorption and distribution existed during the adsorption of NDPhA on Fe/Ti-MIL-NH2 as observed from kinetic and adsorption isotherm fitting. The combination of radicals (·O2-, ·OH) and non-radical (h+, Fe[IV]=O) in the Fe/Ti-MIL-NH2 photolytic system was responsible for NDPhA degradation. Diphenylamine and 2-Nitrodiphenylamine and/or 4-nitrodiphenylamine were identified as the main intermediates during NDPhA degradation, and the pathways were speculated based on these intermediates. In addition, Fe/Ti-MIL-NH2(3:1) could completely remove NDPhA at concentrations <0.1mg/L in source water of water treatment plant and maintain an NDPhA removal efficiency of 83% after 5times of use, indicating the high stability of this material.
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