Na1+xMxTi2-x(PO4)3/MXene复合微卷构筑及其在Water-in-Salt复合电解液中储钠机制研究

水系钠离子电池（ANIBs）在规模储能中扮演着重要角色。针对ANIBs先天电化学稳定窗口窄及NaTi2(PO4)3负极高电子/离子电导、高容量/倍率和表界面稳定性不可兼顾等关键问题，本项目拟基于高储钠Na1+xMxTi2-x(PO4)3/MXene复合微卷电极和双离子Water-in-Salt复合电解液功能协同，构建新型高性能ANIBs。结合理论模拟、精准实验和（非）原位表征，揭示异离子掺杂对Na1+xMxTi2-x(PO4)3电子/离子输运、结构/表界面稳定性及储钠性能作用规律；建立单层/少层MXene组装体宏量制备策略及复合微卷结构演变和调控机制；阐释双离子Water-in-Salt电解液-电极相/表界面电子输运，离子竞争脱嵌本质及优化机理；发展并建立“电极组元/组分/微结构-双离子高浓度电解液-储钠性能”构效关系及调控机制，为高性能ANIBs关键材料及储荷体系设计和应用提供科学依据。

Nowadays, aqueous Na-ion batteries (ANIBs) are playing a significant role in large-scale energy storage sectors. Considering intrinsically narrow electrochemical stability window of ANIBs, and difficulties in simultaneously obtaining superior electron/ion transport, large capacities, high-rate behaviors and high sur-/interface stabilities of the NaTi2(PO4)3 anode for ANIBs, herein, we proposed the synergistic contribution from the Na1+xMxTi2-x(PO4)3/MXene hybrid microscrolls with high Na-storage properties and dual-ion “Water-in-Salt” hybrid electrolytes to smartly construct advanced ANIBs. With the elegant combination of theoretical modeling/simulation, fine experiments and in-/ex-situ characterizations, the interaction theory of the substitution of Ti4+ with other trivalent metal ions on the electron/ion transport, sur-/interface stability and Na-storage performance of the Na1+xMxTi2-x(PO4)3 will be revealed. Large-scale synthesis of single-layer/less-layer MXene assemblies, and evolution/regulation mechanisms of hybrid microscrolls are established. The influence of dual-ion “Water-in-Salt” hybrid electrolytes upon the phase interface and sur-/interface of anode/cathode materials, electronic transfer and competitive insertion/extraction of sodium and lithium ions, and general optimizations are demonstrated. The intrinsic relationships between electrode component/composition/microstructures, dual-ion high-concentration hybrid electrolytes, and electrochemical Na+-storage behaviors are rationally proposed. And the fundamentally scientific guidance will be provided for design and applications of high-performance key materials and charge-storage systems for high-performance ANIBs.