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Graphene has been synthesized by the modified Hummers method and used as electrosorptive electrodes for capacitive deionization. Batch-mode experiments in NaCl solutions at low voltage (≤2 V) are conducted in a continuously recycling system to investigate the electrosorption performance of graphene. The results show that the graphene exhibits a high electrosorption capacity of 1.85 mg/g. The ion sorption follows a Freundlich isotherm, indicating monolayer adsorption. And the electrosorption of NaCl onto graphene electrodes is driven by a physisorption process by taking into account the thermodynamic parameters.