Prussian blue analogues derived magnetic FeCo@GC material as high-performance metallic peroxymonosulfate activators to degrade tetrabromobisphenol A over a wide pH range.

Abstract

Metal-organic frame (MOF) materials can effectively degrade organic pollutants, whereas the MOF is rapidly hydrolysed in water and has poor stability and low reusability. However, in the current advanced oxidation process (AOP) system, the removal effect of pollutants under alkaline condition is not ideal. In this study, a magnetic composite material derived from MOF was synthesised and used as a new catalyst for rapid degradation of tetrabromobisphenol A (TBBPA). Compared to precarbonisation, FeCo@GC formed a conductive graphite carbon skeleton, retained the complete rhombododecahedron structure, had a larger specific surface area and provided more active sites for peroxymonosulfate (PMS) activation. The target pollutant TBBPA (20 mg/L) was completely degraded within 30 min, and the mineralisation rate reached 40.98% in the FeCo@GC (150 mg/L) and PMS (1 mM) systems, owing to the synergistic interaction between Fe, Co and graphite carbon. The reactive oxygen species (ROS) involved in the reaction were determined to be SO4•-, ·OH, 1O2 and O2•- by electron paramagnetic resonance and free radical scavenging experiments, and the 1O2 played a dominant role. Based on the results of LC-MS analysis results, the main degradation pathways of TBBPA involve three mechanisms: the debromination reaction, hydroxylation and cleavage of the benzene ring. In addition, compared with previous AOP systems, FeCo@GC/PMS overcomes the disadvantage of poor degradation effect of TBPPA under alkaline conditions, has a wide range pH (3-11) application and has the best effect on TBBPA degradation under alkaline conditions. FeCo@GC has an excellent cycle performance, with a removal rate of re-calcined material of 88.52% after five cycles. Therefore, FeCo@GC can be used as a promising and efficient catalyst for removing environmental organic pollutants.