Xue Zhixin, Zhang Tao, Li Xiao, Wang Fei, Xu Guiyin, Zhu Meifang
State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai, 201620, China.
Department of Materials Science, Fudan University, Shanghai, 200433, China.
Angew Chem Int Ed Engl. 2025 Jan 15;64(3):e202415283. doi: 10.1002/anie.202415283. Epub 2024 Nov 2.
Uncontrollable side reactions at the metal interface have been identified as the root cause of the formation of a fragile solid electrolyte interphase, leading to irreversible sodium loss in sodium metal batteries. Here, we proposed an interface engineering strategy that employed a carboxyl functionalized cellulose separator to provide strong dipole moments and induce the cleavage of P-F bond to construct a solid electrolyte interphase (SEI) rich in NaF. In addition, we employed nuclear magnetic resonance technology confirmed that the separator with strong dipole moments prevented the reduction of organic solvents by attracting electrons, thereby inhibiting the formation of organic oligomers. SEI with high NaF content and few oligomers is smooth and robust, obviously decreasing the interface impedance of the Na anode. The symmetric Na||Na cells, equipped with the functionalized separator, efficiently operated for 1400 hours with a stable 72 mV overpotential at 0.25 mA cm, exhibiting low energy barrier and fast ion transport kinetics. The Na||NaV(PO) cell also showed stable cycling performance, with the capacity remaining at 94.83 % of the initial capacity after 1000 cycles at 1C. The proposed separator could control the formation and composition of SEI, paving the way for the development of long-life sodium metal batteries.
金属界面处无法控制的副反应已被确定为钠金属电池中形成脆弱的固体电解质界面的根本原因,导致钠不可逆损失。在此,我们提出了一种界面工程策略,即采用羧基功能化的纤维素隔膜来提供强偶极矩并诱导P-F键的断裂,以构建富含NaF的固体电解质界面(SEI)。此外,我们采用核磁共振技术证实,具有强偶极矩的隔膜通过吸引电子阻止了有机溶剂的还原,从而抑制了有机低聚物的形成。具有高NaF含量和少量低聚物的SEI光滑且坚固,明显降低了Na阳极的界面阻抗。配备功能化隔膜的对称Na||Na电池在0.25 mA cm下以稳定的72 mV过电位高效运行1400小时,表现出低能垒和快速的离子传输动力学。Na||NaV(PO)电池也显示出稳定的循环性能,在1C下1000次循环后容量保持在初始容量的94.83%。所提出的隔膜可以控制SEI的形成和组成,为长寿命钠金属电池的发展铺平了道路。