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While flow-electrode capacitive deionization (FCDI) is a potential alternative to brackish and/or sea water desalination, there is limited understanding of both the fate of ions following migration across the ion exchange membranes and the mechanisms responsible for ion separation. In this study, we investigate the desalting performance of an FCDI system operated over a range of conditions. Results show that although ion transport as a result of electrodialysis is inevitable in FCDI (and is principally responsible for pH excursion in the flow electrode), the use of high carbon content ensures that a high proportion of the charge and counterions are retained in the electrical double layers of the flowing carbon particles, even at high charging voltages (e.g., 2.0 V) during the deionization process. Estimation of the portions of sodium and chloride ions adsorbed in the flow electrode after migration through the membranes …