Effects of environmental aging on the adsorption behavior of antibiotics from aqueous solutions in microplastic-graphene coexisting systems

Abstract

The extensive use of nanofillers, such as graphene oxide (GO) and reduced graphene oxide (rGO), as plastic additives has led to the coexistence of microplastics (MPs) and nanomaterials in aquatic environments. However, there is a lack of studies on the adsorption behavior of MPs when coexisting with GO. Moreover, MPs and GO are prone to undergoing aging processes in real environments under conditions such as sunlight exposure, which changes their physicochemical properties and affects their adsorption behavior. In this study, the aging processes of MPs and GO in a real environment were simulated by ultraviolet (UV) irradiation and thermal treatments, respectively. The adsorption behavior of ciprofloxacin (CIP) on three types of MPs (polypropylene (PP), polyamide (PA), and polystyrene (PS)) before and after aging was explored. The MPs are ordered in terms of CIP adsorption capacity as aged-PA > aged-PS > aged-PP > PA > PP > PS, and the adsorption capacity of aged MPs was approximately twofold higher than that of pristine MPs. This paper also studied the adsorption performance of antibiotics in a coexisting system of aged MPs and GO/rGO, and the tetracycline (TC) adsorption capacity was increased by ~336% in aged PP-GO and ~100% in an aged PP-rGO coexisting system. GO/rGO with high degree of oxidation and concentration in an aged- PP-GO/rGO coexisting system are more conducive to the TC adsorption, due to the contribution of oxygen-containing functional groups. Surface and partition adsorption co-occurred during the TC adsorption process. The TC adsorption behavior in the MPs-GO/rGO coexisting system was strongly dependent on the solution pH, which was more favorable under acidic (pH = 3) or alkaline (pH = 11) conditions. This study improves the understanding of the environmental behavior of MPs, graphene, and antibiotics and guides research on strategies for preventing the migration of antibiotics in MPs-GO/rGO coexisting systems.