Carbon Nanotube Membrane Stack for Flow-through Sequential Regenerative Electro-Fenton

Abstract

Electro-Fenton is a promising advanced oxidation process for water treatment consisting a series redox reactions. Here, we design and examine an electrochemical filter for sequential electro-Fenton reactions to optimize the treatment process. The carbon nanotube (CNT) membrane stack (thickness ∼ 200 μm) used here consisted of 1) a CNT network cathode for O2 reduction to H2O2, 2) a CNT-COOFe(2+) cathode to chemical reduction H2O2 to (•)OH and HO(-) and to regenerate Fe(2+) in situ, 3) a porous PVDF or PTFE insulating separator, and 4) a CNT filter anode for remaining intermediate oxidation intermediates. The sequential electro-Fenton was compared to individual electrochemical and Fenton process using oxalate, a persistent organic, as a target molecule. Synergism is observed during the sequential electro-Fenton process. For example, when [DO]in = 38 ± 1 mg L(-1), J = 1.6 mL min(-1), neutral pH, and Ecell = 2.89 V, the sequential electro-Fenton oxidation rate was 206.8 ± 6.3 mgC m(-2) h(-1), which is 4-fold greater than the sum of the individual electrochemistry (16.4 ± 3.2 mgC m(-2) h(-1)) and Fenton (33.3 ± 1.3 mgC m(-2) h(-1)) reaction fluxes, and the energy consumption was 45.8 kWh kgTOC(-1). The sequential electro-Fenton was also challenged with the refractory trifluoroacetic acid (TFA) and trichloroacetic acid (TCA), and they can be transferred at a removal rate of 11.3 ± 1.2 and 21.8 ± 1.9 mmol m(-2) h(-1), respectively, with different transformation mechanisms.