Upgrading the Separators Integrated with Desolvation and Selective Deposition toward the Stable Lithium Metal Batteries.

A practical and effective approach to improve the cycle stability of high-energy density lithium metal batteries (LMBs) is to selectively regulate the growth of the lithium anode. The design of desolvation and lithiophilic structure have proved to be significant means to regulate the lithium deposition process. Here, a fluorinated polymer lithiophilic separator (LS) loaded with a metal-organic framework (MOF801) is designed, which facilitates the rapid transfer of Li+ within the separator owing to the MOF801-anchored PF6 - from the electrolyte, Li deposition is confined in the plane resulting from the polymer fiber layer rich in lithiophilic groups (C─F). The numerical simulation results confirm that LS induces a uniform electric field and Li+ concentration distribution. Visualization technology records the behavior of regular Li deposition in Li||Li and Li||Cu cells equipping LS. Therefore, LS exhibits an ultrahigh Li+ transference number (tLi + = 0.80) and a large exchange current density (j0 = 1.963 mA cm-2). LS guarantees the stable operation of Li||Li cells for over 1000 h. In addition, the LiNi0.8Co0.1Mn0.1O2||Li cell equipped with LS exhibits superior rate and cycle performances owing to the formation of LiF-rich robust SEI layers. This study provides a way forward for dendrite-free Li anodes from the perspective of separator engineering.

New Class of LAGP-Based Solid Polymer Composite Electrolyte for Efficient and Safe Solid-State Lithium Batteries.

Inorganic solid electrolytes (SEs) possess substantial safety and electrochemical stability, which make them as key components of safe rechargeable solid-state Li batteries with high energy density. However, complicated integrally molding process and poor wettability between SEs and active materials are the most challenging barriers for the application of SEs. In this regard, we explore composite SEs of the active ceramic Li1+xAlxGe2-x(PO4)3 (LAGP) as the main medium for ion conduction and the polymer P(VDF-HFP) as a matrix. Meanwhile, for the first time, we choice high chemical, thermal, and electrochemical stability of ionic liquid swelled in polymer, which significantly ameliorate the interface in the cell. In addition, a reduced crystallinity degree of the polymer in the electrolyte can also be achieved. All of these lead to good ionic conductivity of the composite electrolyte (LPELCE), at the same time, good compatibility with the lithium electrode. Especially, high mechanical strength and stable solid electrolyte interphase which suppressed the growth of lithium dendrites and high thermal safety stability can also be observed. For further illustration, the solid-state lithium battery of LiFePO4/LPELCE/Li shows relatively satisfactory performance, indicating the promising potentials of using this type of electrolyte to develop high safety and high energy density solid-state lithium batteries.