Mechanisms of interfacial catalysis and mass transfer in a flow-through electro-peroxone process

作者：Yao, Jingjing; Li, Dong-Sheng; Li, Haipu^*; Yang, Ying^*; Yang, Hui Ying^*

来源：Journal of Hazardous Materials, 2023, 458: 131604.

DOI：10.1016/j.jhazmat.2023.131604

• Density functional theory
• Computational fluid dynamics
• Amitriptyline
• Flow-through electro-peroxone

To investigate the catalytic mechanism and mass transfer efficiency in the removal of amitriptyline using an electro-peroxide process, a CuFe2O4-modified carbon cloth cathode was prepared and utilized in a reaction unit. The results demonstrated a remarkable efficacy of the system, achieving 91.0% amitriptyline removal, 68.3% mineralization, 41.2% mineralization current efficiency, and 0.24 kWh/m(3) energy consumption within just five minutes of treatment. The study revealed that the exposed Fe atoms of the ferrite nanoparticles, with a size of 22.7 nm and 89.7% crystallinity, functioned as mediators to bind the adsorbed O atoms. The 3d(xy), 3d(xz), and 3d(z)(2) orbitals of Fe atoms interacted with the 2p(z) orbital of O atoms of H2O2 and O-3 to form sigma and pi bonds, facilitating the adsorption-activation of H2O2 and O-3 into hydroxyl radicals. These hydroxyl radicals (similar to 1.15 x 10(-13) mol/L) were distributed at the cathode-solution interface and rapidly consumed along the direction of liquid flow. The flow-through cathode design improved the mass transfer of aqueous O-3 and in-situ generated H2O2, leading to an increased yield of hydroxyl radicals, as well as the contact time and space between hydroxyl radicals and amitriptyline. Ultimately, this resulted in a higher degradation efficiency of the system.

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