Abstract

Battery deionization (BDI) technique has attracted great attention as a potential candidate to tackle the freshwater crisis, but its application is plagued by the lack of electrode materials with large desalination capacity and excellent durability. Herein, Mn dopant-reinforced NaTi2(PO4)3 (NT2–xMxP) composites with significantly enhanced structural stability and electronic/ionic conductivity were fabricated toward seawater desalination. Especially, the NT1.5M0.5P exhibits excellent desalination performance, affording a salt removal capacity (SRC) of 128.5 mg/g with a salt removal rate (SRR) of 18.4 mg g−1 min−1 and almost no capacity attenuation after 500 cycles. Furthermore, the NT1.5M0.5P further possesses favorable technical feasibility in different aqueous media, including desalination at various NaCl concentrations, temperature, solution pH, and natural seawater. Mechanism studies reveal that the NT1.5M0.5P undergoes a solid-solution reaction based on the reversible electrochemical reaction of the Ti4+/Ti3+ redox pair during the desalination/salination process. A rocking-chair desalination battery consisting of NT1.5M0.5P and NaFeHCF demonstrates a favorable desalination ability (average SRC of 49.4 mg/g and SRR of 1.73 mg g−1 min−1), outstanding cycling stability (92 % of capacity retention in 100 cycles), low energy consumption (0.288 kWh/kg-NaCl) and high average charging efficiency (86.9 %). This work sheds light on the rational design of advanced NASICON-type electrodes for seawater desalination with remarkable desalination capacity and long serving life.

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