Reviving Sodium Tunnel Oxide Cathodes Based on Structural Modulation and Sodium Compensation Strategy Toward Practical Sodium?Ion Cylindrical Battery

An internal and external synergistic modulation strategy is proposed to slove the problems of surface residual alkali, multiple voltage plateaus, and low initial charge specific capacity in the tunnel oxide cathode material (Na0.44MnO2). In addition, Prussian blue analog (PBA)?Na0.44Mn1?xTixO2 composites are designed to construct practical sodium?ion cylindrical battery with hard carbon anodes for the first time, which displays excellent electrochemical performance and promotes the commercialization of SIBs.As a typical tunnel oxide, Na0.44MnO2 features excellent electrochemical performance and outstanding structural stability, making it a promising cathode for sodium?ion batteries (SIBs). However, it suffers from undesirable challenges such as surface residual alkali, multiple voltage plateaus, and low initial charge specific capacity. Herein, an internal and external synergistic modulation strategy is adopted by replacing part of the Mn with Ti to optimize the bulk phase and construct a Ti?containing epitaxial stabilization layer, resulting in reduced surface residual alkali, excellent Na+ transport kinetics and improved water/air stability. Specifically, the Na0.44Mn0.85Ti0.15O2 using water?soluble carboxymethyl cellulose as a binder can realize a capacity retention rate of 94.30% after 1,000 cycles at 2C, and excellent stability is further verified in kilogram large?up applications. In addition, taking advantage of the rich Na content in Prussian blue analog (PBA), PBA?Na0.44Mn1?xTixO2 composites are designed to compensate for the insufficient Na in the tunnel oxide and are matched with hard carbon to achieve the preparation of coin full cell and 18650 cylindrical battery with satisfactory electrochemical performance. This work enables the application of tunnel oxides cathode for SIBs in 18650 cylindrical batteries for the first time and promotes the commercialization of SIBs.

» Publication Date: 02/09/2024

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This project has received funding from the European Union's Horizon 2020 research and innovation programme under grant agreement Nº 768737


                   




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