The stack configuration in flow-electrode capacitive deionization (FCDI) has been verified to be an attractive and feasible strategy for scaling up the desalination process. However, challenges still exist when attempting to simultaneously improve the desalination scale and the cell configuration. Here, we describe a novel stack FCDI configuration (termed a gradient FCDI system) based on a membrane-current collector assembly, in which the charge neutralization enables the in situ regeneration of the flow electrodes in the single cycle operation, thereby realizing a considerable increase in the desalinating performance. By evaluating standardized metrics such as the salt rejection, productivity (P), average salt removal rate (ASRR), energy-normalized removed salt (ENRS), and TEE, the results indicated that the gradient FCDI system could be a performance-stable and energy-efficient alternative for scale-up desalination. Under optimal operating conditions (carbon content = 10 wt %, feed salinity = 3000 mg L-1, cell voltage = 1.2 V, and productivity = 56.7 L m-2 h-1), the robust desalination performance (ASRR = 1.07 μmol cm-2 min-1) and energy consumption (ENRS = 7.8 μmol J-1) of the FCDI system with a desalination unit number of four were verified at long-term operation. In summary, the stacked gradient FCDI system and its operation mode described here may be an innovative and promising strategy capable of enlarging the scale of desalination while realizing performance improvement and device simplification.

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