Metal-free electrified membranes for contaminants oxidation: Synergy effect between membrane rejection and nanoconfinement

Abstract

Electro-Fenton processes are frequently impeded by depletion of metal catalysts, unbalance between H2O2 generation and activation, and low concentration of reactive species (e.g., •OH) in the bulk solution. A metal-free electro-Fenton membrane was fabricated with nitrogen-doped carbon nanotube (N-CNT) and reduced graphene oxide (RGO). N-CNT acted as a catalyst for both H2O2 generation and activation, while the incorporated RGO served as the second catalyst for H2O2 generation and improved the performance of membrane rejection. The electrified membrane was optimized in terms of nitrogen precursors selection and composition of N-CNT and RGO to achieve optimal coupling between H2O2 generation and activation. The membrane fabricated with 67% mass of N-CNT with urea as the precursor achieved over 95% removal of the target contaminants in a single pass through the membrane with a water flux of 63 L m–2 h–1. This membrane also exhibited efficient transformation of various concentrations of contaminants (i.e., 1-10 mg L–1) over a broad range of pH (i.e., 3-9). Due to its good durability and low energy consumption, the metal-free electro-Fenton membrane holds promise for practical water treatment application. The concentration-catalytic oxidation model elucidated that the elevated contaminant concentration near the membrane surface enhanced the transformation rate by 40%. The nanoconfinement enhanced the transformation rate constant inside the membrane by a factor of 105 because of elevated •OH concentration inside the nanopores. Based on the prediction of this model, the configuration of the membrane reactor has been optimized.