Flow-electrode capacitive deionization (FCDI) represents an innovative, chemically-free, and environmentally-friendly approach for desalination. However, the long-standing challenge of constrained electronic and ionic transport within its flow-electrode has impacted overall desalination performance. In this study, we explore novel concepts and advancements in capacitive deionization by utilizing hierarchical porous carbon (HPC) flow electrodes. By employing widely available sodium carboxymethyl cellulose as a carbon precursor and NaCl as an activator, we have successfully synthesized a carbon-based particle electrode featuring a hierarchical porous structure. The HPC electrode was further optimized through precise adjustments to its pore structure. The optimized electrode exhibited excellent dispersion, viscosity, and remarkable specific capacitance of 283.96 F g−1. Under optimal conditions of a 10% mass loading and an applied voltage of 1.2 V, the electrode demonstrated an average salt removal rate of 82.11 μg cm−2 min−1, a charge efficiency of 101.44%, and an energy consumption of 9.32 × 10−3 kWh mol−1. Furthermore, we investigated the optimal operating parameters for the FCDI device equipped with the HPC flow electrode. Impressively, the HPC flow electrode achieved a salt removal efficiency exceeding 80% over five cycles, maintaining an average salt removal rate of 54.00 μg cm−2 min−1 during 12 h of continuous operation. Detailed textural analysis and electrochemical characterizations revealed that the superior desalination performance is attributed to the hierarchical porous structure of the electrode. This unique structure significantly enhances both electronic and ionic transport within the FCDI system. Our study underscores the critical role of hierarchical porous carbon flow electrodes in capacitive deionization, paving the way for novel strategies to optimize ion and electron transport.
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