Treatment of PBDEs from Soil-Washing Effluent by Granular-Activated Carbon: Adsorption Behavior, Influencing Factors and Density Functional Theory Calculation

Abstract

Soil-washing is a potential technology for the disposal of soil contaminated by e-waste; however, the produced soil-washing effluent will contain polybrominated diphenyl ethers (PBDEs) and a large number of surfactants, which are harmful to the environment, so the treatment of PBDEs and the recycling of surfactants are the key to the application of soil-washing technology. In this study, coconut shell granular-activated carbon (GAC) was applied to remove PBDEs from Triton X-100 (TX-100) surfactant which simulates soil-washing effluent. The adsorption results show that, GAC can simultaneously achieve effective removal of 4,4′-dibromodiphenyl ether (BDE-15) and efficient recovery of TX-100. Under optimal conditions, the maximum adsorption capacity of BDE-15 could reach 623.19 μmol/g, and the recovery rate of TX-100 was always higher than 83%. The adsorption process of 4,4′-dibromodiphenyl ether (BDE-15) by GAC could best be described using the pseudo-second-order kinetic model and Freundlich isothermal adsorption model. The coexistence ions had almost no effect on the removal of BDE-15 and the recovery rate of TX-100, and the solution pH had little effect on the recovery rate of TX-100; BDE-15 had the best removal effect under the condition of weak acid to weak base, indicating that GAC has good environmental adaptability. After adsorption, GAC could be regenerated with methanol and the adsorption effect of BDE-15 could still reach more than 81%. Density functional theory (DFT) calculation and characterization results showed that, Van der Waals interaction and π–π interaction are dominant between BDE-15 and GAC, and hydrogen bond interactions also exist. The existence of oxygen-containing functional groups is conducive to the adsorption of BDE-15, and the carboxyl group (-COOH) has the strongest promoting effect. The study proved the feasibility of GAC to effectively remove PBDEs and recover surfactants from the soil-washing effluent, and revealed the interaction mechanism between PBDEs and GAC, which can provide reference for the application of soil-washing technology.