Evidence for covalently bonded chlorine–fullerene formed by ozonation and chlorination at room temperature

Abstract

This article reports for the first time that fullerene (nC60) can form chlorinated disinfection by-products in aqueous systems at ambient temperature. The ability of nC60 to form colloidal suspensions in aqueous media increases the chance that these particles will migrate in the environment and then in drinking water supply systems. Since nC60 is not completely removed by conventional water treatment, any residual nC60 is likely to be oxidized during disinfection process. While the ozonation of nC60 has been studied, little is known about the reaction between nC60 and chlorine. To address this issue, we subjected aqueous nC60 suspensions to chlorination and sequential ozonation/chlorination at ozone dosages of 4.5, 10, 15 and 24 mg O3/mg nC60. The morphology and physicochemical properties of oxidized nC60 aggregates were evaluated by scanning electron microscopy, transmission electron microscopy, UV–visible absorption spectroscopy and X-ray photoelectron spectroscopy (XPS). We found that while the particles in the as-prepared nC60 were predominantly spheres, the ozonation of nC60 resulted in the formation of irregularly shaped aggregates. The concentration of atomic carbon found by XPS in the nC60 samples decreased from 92 % for the as-prepared nC60 to 50 % for the aggregates ozonated at 24 mg O3/mg nC60 and then chlorinated at 68 mg Cl2/L and allowed to react for 100 min. The presence of Cl atoms covalently bonded to C atoms was confirmed by XPS peaks corresponding to a binding energy (Eb) of 200.1–202.4 eV. This demonstrates the need to better assess and monitor the formation of potentially toxic chlorinated disinfection by-products from carbon nanomaterials during water treatment.