The aggregation behaviour and mechanism of commercial graphene oxide in surface aquatic environments

In this study, we comprehensively and critically discuss the aggregation mechanism of commercial graphene oxide (CGO) in surface aquatic environments. The aggregation kinetics and critical coagulation concentration of CGO were obtained through time-resolved dynamic light scattering and batch techniques over a wide range of water types. By employing transmission electron microscopy and elemental mapping, Fourier transform infrared spectroscopy, and X-ray photoelectron spectroscopy, we studied the effects of cations in natural waters on the microstructure transformation, element content and distribution, and oxygen-containing functional group vibrations of CGO. The aggregation of CGO in natural water is induced mainly by Ca²⁺ by complexing; Na⁺, with a higher concentration, plays a more important role than Mg²⁺ in inducing aggregation via electric double layer suppression. Ca²⁺ mainly interacts with C - COOH, while Mg²⁺ has a greater effect on C - OH. Na⁺ has less effect on the oxygen-containing functional group but decreases the C/O ratio in contrast with Mg²⁺/Ca²⁺/natural water, indicating the different inducing mechanisms. This study looks forward to providing pivotal knowledge to predict the environmental fate of CGO more accurately in natural surface water.