CuFe2O4/diatomite actuates peroxymonosulfate activation process: Mechanism for active species transformation and pesticide degradation

Peroxymonosulfate (PMS) activation is a promising technology for water purification, but the removal performance of multiple pollutant matrices and the mechanism for reactive species transformation in the heterogeneous catalytic system remain ambiguous. Herein, a novel CuFe2O4/diatomite was fabricated for PMS activation to achieve efficient removal of typical pesticides. Uniform distribution of CuFe2O4 on diatomite efficiently alleviated the agglomeration of CuFe2O4 and increased specific surface area (57.20 m2 g-1, 3.8-fold larger than CuFe2O4). CuFe2O4/5% diatomite (5-CFD)/PMS system showed nearly 100% removal efficiency for mixed pesticide solution within 10 min (0.10 g L-1 5-CFD and 0.40 g L-1 PMS) and excellent anti-interference performance towards various coexisting substances (>= 90% removal efficiency). The electrochemical measurements confirmed that the lower charge transfer resistance of 5-CFD significantly enhanced the electron-transfer capacity between 5-CFD and PMS, accelerating the reactions among ---Fe(III)/---Fe(II), ---Cu(II)/---Cu(I), and PMS, further generating center dot OH (261.3 mu M), 1O2 (138.8 mu M), SO4 center dot- (11.8 mu M), and O2 center dot-. The O in reactive oxygen species didn't originate from dissolved oxygen (DO) but PMS, independent of the low solubility of DO and slow diffusion rate of O2 in water. Furthermore, the production of 1O2 went through the process: PMS -> O2 center dot- -> 1O2, and SO4 center dot- could rapidly convert into center dot OH. The degradation pathways and the evolution of intermediates were proposed by HPLC-QTOF-MS/MS and DFT calculations. QSAR analysis illustrated that the toxicity became lower with the reaction process. This study provides novel insights into the mechanism for pesticide degradation and active species transformation and the anti-interference capability of systems.