Effect of co-existing kaolinite and goethite on the aggregation of graphene oxide in the aquatic environment

• pH had a notable effect on GO stability with kaolinite-goethite associations (KGAs).
• Kaolinite decreased the critical coagulation concentration of GO at pH 5.5
• Heteroaggregation of GO with KGAs was extremely sensitive to ionic strength.
• Heteroaggregation extent of GO with KGAs increased firstly, then decreased with Ce.

Broad applications of graphene oxide (GO) will result in the release of GO into aquatic environments, where clay minerals and metal (hydr)oxides are commonly present. Thereby the interactions between GO and a binary system containing clay minerals and metal (hydr)oxides can occur. We investigated the aggregation of GO with kaolinite and kaolinite-goethite associations (KGAs) in aquatic systems under different pHs, ionic strengths, and GO concentrations. GO suspension was unstable at low pHs, and the aggregation of GO occurred in the presence of KGA-4% and KGA-10% until pH 5 and 6, respectively. Kaolinite decreased the critical coagulation concentration (CCC) of GO at pH 5.5 from around 50 to 20 mM NaCl due to the reduced energy barrier. Heteroaggregation of GO with KGAs was extremely sensitive to ionic strength at pH 5.5, and the CCC of GO in the presence of KGA-10% increased from less than 1 mM NaCl to 5 mM NaCl with the increase of pH from 5.5 to 9. The heteroaggregation extent of GO with KGAs was enhanced firstly, then reduced with the increase of GO concentrations at pH 5.0, which is likely because KGA plates were more efficiently wrapped by large-size GO sheets with increasing GO concentrations. These findings are useful for understanding and predicting the fate of GO in the relatively complicated aquatic and soil environments where binary minerals co-exist.

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