Efficient removal of chloroform from groundwater using activated percarbonate by cellulose nanofiber-supported Fe/Cu nanocomposites

Abstract

Chloroform (CF) is a recalcitrant halogenated methane (HM) that has received widespread attention due to its frequent detection in groundwater and its potential carcinogenic risk. In this study, TEMPO-oxidized cellulose nanofiber-supported iron/copper bimetallic nanoparticles (TOCNF-Fe/Cu), a novel composite catalyst, was synthesized to activate sodium percarbonate (SPC) for the removal of CF from groundwater. The results showed that over 96.3% of CF could be removed in a neutral reaction medium (pH 6.5–9) within 180 min using 0.66 g L−1 of TOCNF (0.32)-Fe/Cu (1) and 1 mM of SPC, which outperforms typical advanced oxidation processes. The reaction mechanism of the TOCNF-Fe/Cu-SPC system for the CF removal was elucidated. As demonstrated through electron paramagnetic resonance and quenching experiments, the TOCNF-Fe/Cu-SPC system was found to include •OH and O2•−, where the latter played a dominant role in the CF removal. DFT calculations indicated that TOCNF improved the electron transport capability of Fe/Cu and reduced the transition state energy. The Fe species on the surface of TOCNF-Fe/Cu were identified as the primary active sites for SPC activation, whereas the Cu species were beneficial to the regeneration of the Fe species. Additionally, TOCNF-Fe/Cu was found to have good recyclability and stability. The feasibility of the TOCNF-Fe/Cu-SPC system was further confirmed by applying it for the efficient removal of composite HMs from actually contaminated groundwater. Overall, the TOCNF-Fe/Cu-SPC system is an attractive candidate for the treatment of HM-contaminated groundwater.