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Enhanced Heterogeneous Fenton-like Process for Sulfamethazine Removal via Dual-Reaction-Center Fe-Mo/rGO Catalyst

Journal 2022 · IF 5.719 · 12(23): 4138 · 发表于 2022 年 11 月 23 日
作者: Weihua Qin,Yueming Ma,Ting He,Jingbin Hu,Pan Gao,Shaoxia Yang
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摘要

A heterogeneous Fenton-like catalyst with single redox site has a rate-limiting step in oxidant activation, which limited its application in wastewater purification. To overcome this, a bimetallic doping strategy was designed to prepare a heterogeneous Fenton-like catalyst (Fe-Mo/rGO) with a double-reaction center. Combined with electrochemical impedance spectroscopy and density functional theory calculation, it was confirmed that the formation of an electron-rich Mo center and an electron-deficient Fe center through the constructed Fe-O-Mo and Mo-S-C bonding bridges induced a higher electron transfer capability in the Fe-Mo/rGO catalyst. The designed Fe-Mo/rGO catalyst exhibited excellent sulfamethazine (SMT) degradation efficiency in a broad pH range (4.8–8.4). The catalytic performance was hardly affected by inorganic anions (Cl−, SO42−and HCO3−) in the complicated and variable water environment. Compared to Fe/rGO and Mo/rGO catalysts, the SMT degradation efficiency increased by about 14.6 and 1.6 times in heterogeneous Fenton-like reaction over Fe-Mo/rGO catalyst. The electron spin resonance and radical scavenger experiments proved that ·O2−/HO2· and1O2dominate the SMT removal in the Fe-Mo/rGO/H2O2system. Fe and Mo, as active centers co-supported on rGO, significantly enhanced the electron transfer between catalyst, oxidant, and pollutants, which accelerated the reactive oxygen species generation and effectively improved the SMT degradation. Our findings offer a novel perspective to enhance the performance of heterogeneous Fenton-like catalysts by accelerating the electron transfer rate in the degradation of organic pollutants.Keywords:heterogeneous Fenton-like reaction;Fe-Mo dual-reaction-center catalyst;reactive oxygen species;sulfamethazine