Non-Resonant Structure Induces N-Rich Solid Electrolyte Interface toward Ultra-Stable Solid-State Lithium-Metal Batteries

The practical application of all-solid-state lithium metal batteries (ASSLMBs) is limited by lithium (Li) anode instability including Li dendrite formation and deteriorating interface with electrolytes. Here, a functional additive, isosorbide mononitrate (ISMN) with a non-resonant structure (O2-N-O-) is reported, which improves its reactivity and is utilized to build a stable N-rich solid electrolyte interface, effectively alleviating Li dendrite and side reactions for poly(vinylidene fluoride) (PVDF)-lithium bis(trifluoromethane sulfonyl) imide (LiTFSI)-based electrolyte (PLE-ISMN). In addition, the ion-dipole interaction between ISMN and Li ions facilitates the dissociation of LiTFSI to form carrier ions, improving the ionic conductivity (4.4 x 10-4 S cm-1) and transference number (0.50) of PLE-ISMN. Consequently, the Li/Li symmetric cell delivers a high critical current density of 2.0 mA cm-2 and stable Li stripping/plating cycling over 5000 h with a capacity of 1.0 mAh cm-2. Moreover, the Li|LiFePO4 cell delivers an excellent initial discharge capacity of 154.0 mAh g-1 with an outstanding capacity retention of 88.9% after 500 cycles at 0.5 C. The Li|LiNi0.8Co0.1Mn0.1O2 cell also exhibits a good cycling performance at 4.4 V at 1 C. A non-resonant nitrate ester, isosorbide mononitrate (ISMN) is introduced into PVDF-based polymer solid-state electrolyte, which breaks the resonance of three equal O atoms by connecting an ether-based group and the improve its reactivity. During the electrochemical process, the NO bond in non-resonant structure of ISMN is broken, inducing a N-rich solid electrolyte interface toward ultra-stable solid-state lithium-metal batteries. image