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· A novel ZIF-8 derived nitrogen-doped nanocarbon was developed for accelerating Fe cycle.
· The evolution of Fe species was discussed by monitoring the mass balance of Fe.
· Pre-oxidation was used to reveal possible catalytic reduction pathways.
· Two Fe(Ⅲ)/Fe(Ⅱ) cycling pathways were verified in ZCN/Fe(Ⅲ)/H2O2 process.
Zeolite imidazole framework-8 (ZIF-8) is a promising template to obtain porous nanocarbons. In this study, microporous nitrogen-doped nanocarbons from the carbonization of ZIF-8 (ZCN) was prepared as an efficient metal-free catalyst to improve several micropollutants degradation in Fe(Ⅲ)/H2O2 process. The sulfamethoxazole (SMX) ratio was increased from 20% to 100% with the addition of ZCN (50 mg/L) in Fe(Ⅲ)/H2O2 within 20 min, and the working pH was endowed. The direct reduction for Fe(Ⅲ) resulting from carbonyl on ZCN's surface was revealed. Hydroxyl radical (•OH) was determined to be the main reactive species, and the evolution of different Fe species during the reaction was discussed by monitoring the mass balance of Fe species. We found that part of the iron was bound to the surface of ZCN during the reaction. Additionally, the dissociative Fe was captured by ZCN to form Fe-N bonds. Surface-bound Fe with a lower energy barrier was more likely to react with H2O2 to generate Fe(Ⅱ). Our work revealed that in addition to the direct reduction by ZCN, another catalytic reduction pathway for the sustainable conversion of Fe(Ⅲ) to Fe(Ⅱ) in the ZCN/Fe(Ⅲ)/H2O2 process was operative.
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