Understanding the membrane fouling control process at molecular level in the heated persulfate activation- membrane...

Sulfate radical (SO₄^●-) based advanced oxidation is considered as a promising pretreatment strategy to degrade organic pollutants and thereby mitigate the membrane fouling in the membrane process. In this study, heat-activated persulfate (PS) activation was integrated with the membrane distillation (MD) process for the alleviation of membrane fouling in treatment of wastewater treatment plant (WWTP) secondary effluent and surface water. In-depth understanding of the molecular fate during membrane fouling control process was performed by using a non-targeted screening method of two-dimensional gas chromatography-time-of-flight mass spectrometry (GC × GC-TOF-MS) coupling with multiple characterizations. It was found that the heat-activated PS activation pretreatment could effectively degrade the dissolved organic matter (DOM) and change its molecular conformation, wherein the relative abundance of oxygen-containing substances was remarkably increased through oxygenation reactions. Moreover, the refractory organics with higher molecular weight (MW) and unsaturation degree were more inclined to be destroyed, following by partial mineralization during pretreatment process. It was also identified that oxygen-deficient compounds and the molecular formulas featuring higher double bond equivalent (DBE) values and lower MW tended to be deposited on the membrane surface to cause the membrane fouling. In particular, the aliphatic substances were the predominant components irrespective of membrane foulant samples from secondary effluent or surface water. Meanwhile, the complexation between organic compounds and high valence cations as well as the precipitation of inorganics were restrained owing to the reduction of DOM concentration and the transformation of molecular structure, consequently leading to reduced membrane fouling. This study is believed to further provide new insight into the membrane fouling control mechanism at molecular level.