Abstract

The discovery of novel electrode materials with durable ion removal functionality for a designed capacitive deionization architecture is critical to enable seawater desalination. NASICON-based material, although having high theoretical capacity and fast sodium conductivity and thus a promising electrode material for sodium-ion removal, its desalination performance is limited by the poor electrical conductivity and aqueous electrolyte susceptibility. Herein, nano-sized sodium vanadium fluorophosphate Na3V2(PO4)2F3 at reduced graphene oxide (NVPF@rGO) is synthesized to improve electroconductivity and shorten the ion diffusion path, while fluorine content in its composition is regulated to lower the ions' diffusion barrier as a result of larger volume of the crystal. Moreover, the electrolyte concentration-controlled strategy is thoroughly investigated to minimize the dissolubility of the cathode over time. A proposed dual-ion electrochemical deionization system (DEDI) consisting of NVPF@rGO cathode and AgCl@rGO anode shows superior desalination stability in a highly concentrated synthetic seawater environment with ~98% capacity retention in over 500 cycles. Moreover, the salt removal capacity of 60 mg/g and desalination rate of 3.7 mg/g/min were achieved at a current density of 200 mA/g.

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