Enhanced Fenton performance of wet-mechanochemically synthesized FeS2/Biochar: The multiple synergistic effect derived from mutual element doping

Abstract

FeS2-biochar composites have been considered as promising heterogeneous Fenton materials for pollutants removal. However, the chemical synthesis of element-doped FeS2-biochar composite with superior performance and the comprehensive investigation for its underlying multiple synergistic mechanism remain a difficult endeavor. Herein, a novel FeS2/Biochar nanocomposite with mutual element doping was firstly synthesized by facile wet-mechanochemical method using iron, sulfur and bamboo-biochar for efficient organic pollutant (sulfamonomethoxine, SMM) removal. Experiment and DFT calculation results revealed that multiple synergistic effect between FeS2 and biochar derived from newly formed Fe-C and C-S-C bonds induced the abundant reactive oxygen species (ROS) and excellent electron transfer capacity. Fe-C sites facilitated the H2O2 adsorption and populated O-O bond in H2O2 for its barrierless dissociation into •OH via forming bridging C-Fe-O-O-Fe bond. Oxygen vacancy, C-S-C and Fe-C bonds, persistent free radicals (PFRs) accelerated the generation and transformation of ROS, which resulted in dominating free radical (•OH, •O2–, •SO4-) and auxiliary non-radical (1O2) pathway. Meanwhile, Fe3+/Fe2+ redox-cycle was expedited by electron donor/shuttle (S22-, BC, •O2–, C-S-C and Fe-C bonds). All these specialties contributed to the superior performance of FeS2/Biochar Fenton system for SMM removal at wide pH range (3–11) with negligible Fe release. Completely SMM (50 mg/L) removal was achieved within 20 min for 8 successive reuses. This work emphasized the concept of building mutual element doping on molecular level in enhancing FeS2-Biochar synergy towards efficient environmental remediation.