Flexible construction of three-dimensional continuous conductive structure by hollow carbon sphere and CNT for promoted ions transport in flow-electrode capacitive deionization

Flow-electrode capacitive deionization (FCDI) emerges as a promising desalination technique, characterized by its unlimited desalination capacity, seamless operation, and easy scalability. However, challenges such as discontinuous electronic network, inadequate dispersion of suspended carbon particles, and hindered electron/ion transport pathways have impeded the full potential of FCDI. This study addresses the above issues by synergistically leveraging the advantage of hollow carbon sphere (HCS) and CNT to construct a flexible, continuous three-dimensional conductive network (HCS@CNT) as the flow-electrode for FCDI. The incorporation of HCS substantially improves the fluidity and effective collision of the flow-electrode slurry. Simultaneously, the bridging effect of CNT facilitates smooth ion transport routes and rapid electron/ion transfer. Moreover, the spherical structure of HCS as a node can effectively alleviate the agglomeration of CNT due to its inherent good fluidity. As a result, the meticulously designed HCS@CNT flow-electrode demonstrates outstanding rheological behavior with excellent hydrophilicity, a large specific capacitance, and low ion diffusion resistance. During desalination tests, the HCS@CNT flow-electrode exhibited a high average salt removal rate (0.56 µmol min−1 cm−2), appropriate energy-normalized removal salt (15 µmol J−1), and notable charge efficiency (89 %) in a 1 g L-1 NaCl solution. Impressively, it maintained good stability and continuity over a continuous 10-hour desalination process, showcasing substantial potential for treating highly concentrated saline water. In addition, density functional theory (DFT) calculations provided additional insights, confirming that the construction of HCS@CNT facilitated interfacial charge transfer and electron transport from HCS to CNT. This innovative approach sheds light on enhancing electron/ion transfer by harnessing the unique structural characteristics of the flow-electrode.