LLZTO Nanoparticle- and Cellulose Mesh-Coreinforced Flexible Composite Electrolyte for Stable Li Metal Batteries.

Composite electrolytes have been regarded as the most prospective electrolytes for commercial application because they acquire the advantages of both polymer and inorganic electrolytes, commonly exhibiting appreciated flexibility and suitable ionic conductivity. Nevertheless, the conventional solution-casting method with toxic solvent and poor interfacial contact still hamper their commercialization process. Moreover, electrolytes with higher ionic conductivity and transference number are urgently needed for satisfying fast-charging batteries. Herein, a novel composite electrolyte (LZEC) reinforced by mechanically robust LLZTO nanoparticles and flexible cellulose mesh was fabricated by a simple and advanced in situ thermal polymerization method, with adding of highly ion-conductive liquid plasticizer. Consequently, the rationally designed LZEC composite electrolyte exhibits superior flexibility and remarkable electrochemical properties in the form of high ionic conductivity, wide electrochemical stability window, and high Li+ transference number. Importantly, the in situ synthesis method is expected to help construct an enhanced electrolyte/electrode interface inside the battery, and the LZEC composite electrolyte is capable of suppressing Li dendrite growth effectively, as evidenced by the prolonged stable cycling of the Li/Li symmetric cell. Therefore, the LFP/LZEC/Li full cell exhibits superior rate performance and long cyclic life. These attractive properties make LZEC a potential composite electrolyte for boosting the practical application of safe and long-life Li metal batteries.

Laponite-Supported Gel Polymer Electrolyte with Multiple Lithium-Ion Transport Channels for Stable Lithium Metal Batteries.

Lithium metal batteries have emerged as a promising candidate for next-generation power systems. However, the high reactivity of lithium metal with liquid electrolytes has resulted in decreased battery safety and stability, which poses a significant challenge. Herein, we present a modified laponite-supported gel polymer electrolyte (LAP@PDOL GPE) that was fabricated using in situ polymerization initiated by a redox-initiating system at ambient temperature. The LAP@PDOL GPE effectively facilitates the dissociation of lithium salts via electrostatic interaction and simultaneously constructs multiple lithium-ion transport channels within the gel polymer network. This hierarchical GPE demonstrates a remarkable ionic conductivity of 5.16 × 10-4 S cm-1 at 30 °C. Furthermore, the robust laponite component of the LAP@PDOL GPE forms a barrier against Li dendrite growth while also participating in the establishment of a stable electrode/electrolyte interface with Si-rich components. The in situ polymerization process further improves the interfacial contact, enabling the LiFePO4/LAP@PDOL GPE/Li cell to exhibit an impressive capacity of 137 mAh g-1 at 1C, with a capacity retention of 98.5% even after 400 cycles. In summary, the developed LAP@PDOL GPE shows great potential in addressing the critical issues of safety and stability associated with lithium metal batteries while also delivering improved electrochemical performance.

Bifunctional Solid-State Copolymer Electrolyte with Stabilized Interphase for High-Performance Lithium Metal Battery in a Wide Temperature Range.

Solid-state polymer electrolytes (SPEs) are expected to guarantee safe and durable operations of lithium metal batteries (LMBs). Herein, inspired by the salutary poly(vinyl ethylene carbonate) (PVEC) component in the solid electrolyte interphase, cross-linking vinyl ethylene carbonate and ionic liquid copolymers were synthesized by in-situ polymerization to serve as polymer electrolyte for LMBs. On one hand, due to rich ester bonds of PVEC, Li+ could transfer by coupling/decoupling with oxygen atoms. On the other hand, the imidazole ring of ionic liquid could facilitate the dissociation of lithium salt to promote the free movement of Li+ . The bifunctional component synergistically increased the ionic conductivity of the SPE to 1.97×10-4  S cm-1 at 25 °C. Meanwhile, it also showed a wide electrochemical window, superior mechanical properties, outstanding non-combustibility, and excellent interfacial compatibility. The bifunctional copolymer-based LiFePO4 batteries could normally operate at 0 to 60 °C, making them a promising candidate for wide-temperature-rang LMBs.

A LiAlO2/nitrogen-doped hollow carbon spheres (NdHCSs) modified separator for advanced lithium-sulfur batteries.

Lithium-sulfur (Li-S) batteries have gained significant attention due to their ultrahigh theoretical specific capacity and energy density. However, their practical commercialization is still facing many intractable problems, of which the most difficult is the shuttle effect of dissolved polysulfides. To restrict the shuttle of polysulfides, herein, a novel double-layer lithium aluminate/nitrogen-doped hollow carbon sphere (LiAlO2/NdHCSs)-modified separator was designed. The upper NdHCSs layer on the separator works as the first barrier to physically and chemically adsorb polysulfides, whereas the bottom LiAlO2 layer acts as the second barrier to physically block the polysulfides without restricting the Li+ transport due to the high ionic conductivity of LiAlO2. Cells with the LiAlO2/NdHCSs-modified separator showed an initial discharge capacity of 1500 mA h g-1 at 0.2C, and a discharge capacity of 543.3 mA h g-1 was obtained after 500 cycles at 2C. Especially, when the areal density of the active material was increased to 4.5 mg cm-2, the cells retained a discharge capacity of 538.6 mA h g-1 after 100 cycles at 0.5C. The outstanding electrochemical performance of Li-S cells with the LiAlO2/NdHCSs-modified separators show a new approach for the applications of Li-S batteries.