Degradation and Mineralization of Carbamazepine Using an Electro-Fenton Reaction Catalyzed by Magnetite Nanoparticles Fixed on an Electrocatalytic Carbon Fiber Textile Cathode

催化作用 化学工程 化学 阴极 双功能 纳米颗粒 电解 矿化(土壤科学) 材料科学 电极 有机化学 电解质 工程类 物理化学 氮气
作者
Kai Liu,Joseph Che-Chin Yu,Heng Dong,Jeffrey C.S. Wu,Michael R. Hoffmann
出处
期刊:Environmental Science & Technology [American Chemical Society]
卷期号:52 (21): 12667-12674 被引量:145
标识
DOI:10.1021/acs.est.8b03916
摘要

Pharmaceutical wastes are considered to be important pollutants even at low concentrations. In this regard, carbamazepine has received significant attention due to its negative effect on both ecosystem and human health. However, the need for acidic conditions severely hinders the use of conventional Fenton reagent reactions for the control and elimination of carbamazepine in wastewater effluents and drinking water influents. Herein, we report of the synthesis and use of flexible bifunctional nanoelectrocatalytic textile materials, Fe3O4-NP@CNF, for the effective degradation and complete mineralization of carbamazepine in water. The nonwoven porous structure of the composite binder-free Fe3O4-NP@CNF textile is used to generate H2O2 on the carbon nanofiber (CNF) substrate by O2 reduction. In addition, ·OH radical is generated on the surface of the bonded Fe3O4 nanoparticles (NPs) at low applied potentials (−0.345 V). The Fe3O4-NPs are covalently bonded to the CNF textile support with a high degree of dispersion throughout the fiber matrix. The dispersion of the nanosized catalysts results in a higher catalytic reactivity than existing electro-Fenton systems. For example, the newly synthesized Fe3O4-NPs system uses an Fe loading that is 2 orders of magnitude less than existing electro-Fenton systems, coupled with a current efficiency that is higher than electrolysis using a boron-doped diamond electrode. Our test results show that this process can remove carbamazepine with high pseudo-first-order rate constants (e.g., 6.85 h–1) and minimal energy consumption (0.239 kW·h/g carbamazepine). This combination leads to an efficient and sustainable electro-Fenton process.

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