Enhanced Fe(III)-mediated Fenton oxidation of atrazine in the presence of functionalized multi-walled carbon nanotubes

In this study we reported that the presence of functionalized multi-walled carbon nanotubes (FCNT-H) would greatly enhance the degradation of atrazine (ATZ), a model contaminant, in the Fe(III)-mediated Fenton-like system. Efficient ATZ degradation (>90%) was achieved within 30 min in the presence of 20 mg.L-1 FCNT-H, 2.0 mg.L-1 Fe(III), and 170 mg.L-1 H2O2, whereas negligible ATZ degradation occurred in FCNT-H free system. The structure and surface chemistry of FCNT-H and other CNTs were well characterized. The formed active species were determined based on ESR analysis, and the mass balance of Fe species during the reaction was monitored. In particular, a new method based on ferrozine complexation was proposed to track the formed Fe(II). The results indicated that ATZ was mainly degraded by the generated hydroxyl radical (HO center dot), and Fe(Ill)/Fe(II) cycling was still the rate-limiting step. Besides a small fraction of Fe(III) reduced by FCNT-H, a new pathway was revealed for fast reduction of most Fe(III), i.e., reaction of FCNT-H-Fe(III) complexes with H2O2. Comparison of different CNTs-mediated Fe(III)/H2O2 systems indicated that such enhanced effect of CNTs mainly resulted from the surface carboxyl group instead of hydroxyl and carbonyl group. Combined with X-ray photoelectron spectroscopy (XPS) analysis, the electron density migration from Fe(III) to FCNT-H possibly resulted in the fast reduction of FCNT-H-Fe(III) complexes by H2O2. This study enables better understanding the enhanced Fe(III)-mediated Fenton-like reaction in the presence of MWCNTs and thus, will shed new light on how to develop more efficient similar Fenton systems via Fe(III) complexation. (C) 2018 Elsevier Ltd. All rights reserved.