In Situ Formation of Prussian Blue Analogue Nanoparticles Decorated with Three-Dimensional Carbon Nanosheet Networks for Superior Hybrid Capacitive Deionization Performance

Capacitive deionization (CDI) is considered to be an alternative water purification technology because of its low cost and low driven energy. However, the desalination performance of traditional CDI still cannot meet the requirement of actual operations, which is the limited adsorption capacity of carbon electrodes. Here, we report a feasible and simple strategy for the synthesis of a three-dimensional hierarchical composite with homogeneous Prussian blue analogue nanoparticles, decorating hierarchical porous carbon nanosheet networks (NiHCF@3DC-2) as a redox-active intercalation electrode material for hybrid capacitive deionization (HCDI). The interconnected network structure, accompanied by its unique porous characteristic and uniform NiHCF nanoparticles, endows the prepared NiHCF@3DC-2 with enough straining space for alleviating the effect of volume change upon the regeneration process and guarantees fast transmission kinetics for both electrons and salt ions. As a consequence, an HCDI cell with NiHCF@3DC-2 and activated carbon showed superior desalination ability with a high ion removal capacity of 47.8 mg g^-1 (107.5 mg g^-1 NiHCF@3DC-2) and good cyclic regenerative performance. Moreover, the Na⁺ ions storage mechanism and the interfacial synergy of the NiHCF@3DC-2 were also explored by structure and electrochemistry analyses during the CDI process. Our work provides a promising redox-active intercalation electrode material to highly efficient hybrid capacitive deionization for brine.