Ferrous metal-organic frameworks with strong electron-donating properties for persulfate activation to effectively degrade aqueous sulfamethoxazole.

ABSTRACT

Three novel persulfate activators, Fe(II)-based metal-organic frameworks (MOFs) were synthesized for the degradation of sulfamethoxazole (SMX). The degradation experiment results showed that all the Fe(II)MOFs could effectively activate persulfate and degrade more than 97% SMX within 180 min, with higher than 77% persulfate decomposition efficiencies. It was found by Mössbauer spectra that the variation of organic ligands for synthesis have an influence on the content of Fe(II) of these MOFs, thus resulted in the order of activation capacities Fe(Nic) > Fe(PyBDC) > Fe(PIP). It was demonstrated that the activation of persulfate was mainly ascribed to the heterogeneous process that accomplished by surface-bounded Fe(II) acted as the main active site to provided electrons for persulfate or dissolved oxygen. EPR and molecular probe studies confirmed the coexistence of SO4·-, ·OH, and O2·-, and differentiated their contributions in SMX degradation. Possible degradation pathways of SMX were proposed based on the detection results of intermediates by UPLC-MS/MS. This work provides a new prospect into the synthesis of high-performance MOFs with strong electron-donating properties as efficient persulfate activators, which may encourage the employ of MOFs in the wastewater treatment process.