Regulation of SEI Formation by Anion Receptors to Achieve Ultra-Stable Lithium-Metal Batteries.

Despite high specific capacity (3860 mAh g-1 ), the utilization of Li-metal anodes in rechargeable batteries are still hampered due to their insufficient cyclability. Herein, we report an anion-receptor-mediated carbonate electrolyte with improved performance and can ameliorate the solid electrolyte interphase (SEI) composition comparing to the blank electrolyte. It demonstrates a high average Coulombic efficiency (97.94 %) over 500 cycles in the Li/Cu cell at a capacity of 1 mAh cm-2 . Raman spectrum and molecular modelling further clarify the screening effects of the anion receptor on the Li+ -PF6 - ion coupling that results in the enhanced ion dynamics. The X-ray photoelectron spectroscopy (XPS) distinguishes the disparities in the SEI components of the developed electrolyte and the blank one, which is rationalized by the molecular insights of the Li-metal/electrolyte interface. Thus, we prepare a 2.5 Ah prototype pouch cell, exhibiting a high energy density (357 Wh kg-1 ) with 90.90 % capacity retention over 50 cycles.

Image-spherizing-based planeness detecting method for a micro-channel plate.

Based on the mathematical models proposed by the image spherizing algorithm, a novel planeness detecting method for a micro-channel plate (MCP) is presented. After describing the theory of the image spherizing algorithm, a straight line image is chosen as a standard picture, and the imaging simulation for a deformed MCP is performed. According to the simulated results, the deformation characteristic of the MCP and the mechanism of the image twisting phenomenon were analyzed. Finally, the double lines method, which specializes in planeness detection, is proposed. The experimental result obtained by interferometer shows that the profile characteristics of a deformed MCP are consistent with the theoretical analysis. To verify the effectiveness of the double lines method, we measured the planeness of 100 pieces of MCP and then defined the detecting standard: a micro-channel plate will be treated as a defective product when the twisting angle of the two orthogonal lines in the reflected image is greater than 40°, whereas the product will meet the military standard when the twisting angle is smaller than 7°. In this method, the planeness detection could be completed only by observing the reflected image of the MCP, even in a harsh environment. In particular, the accuracy can reach 1 µm and it has been applied to the MCP production process.

Optimizing Li-ion Solvation in Gel Polymer Electrolytes to Stabilize Li-Metal Anode.

Gel polymer electrolytes (GPEs) have potential as substitutes for liquid electrolytes in lithium-metal batteries (LMBs). Their semi-solid state also makes GPEs suitable for various applications, including wearables and flexible electronics. Here, we report the initiation of ring-opening polymerization of 1,3-dioxolane (DOL) by Lewis acid and the introduction of diluent 1,1,2,2-tetrafluoroethyl 2,2,3,3-tetrafluoropropyl ether (TTE) to regulate electrolyte structure for a more stable interface. This diluent-blended GPE exhibits enhanced electrochemical stability and ion transport properties compared to a blank version without it. FTIR and NMR proved the effectiveness of monomer polymerization and further determined the molecular weight distribution of polymerization by gel permeation chromatography (GPC). Experimental and simulation results show that the addition of TTE enhances ion association and tends to distribute on the anode surface to construct a robust and low-impedance SEI. Thus, the polymer battery achieves 5 C charge-discharge at room temperature and 200 cycles at low temperature -20 °C. The study presents an effective approach for regulating solvation structures in GPEs, promoting advancements in the future design of GPE-based LMBs.

Composite electrolytes engineered by anion acceptors for boosted high-voltage solid-state lithium metal batteries.

Solid-state batteries (SSBs) are considered as the most promising option to replace commercial lithium-ion batteries due to their ability to address the flammability of liquid organic electrolytes and facilitate the energy density of lithium batteries. Herein, by introducing tris(trimethylsilyl) borate (TMSB) as anion acceptors, we successfully develop the light and thin electrolyte (TMSB-PVDF-HFP-LLZTO-LiTFSI, PLFB) with a wide voltage window to couple the lithium metal anode with the high-voltage cathodes. Consequently, as-prepared PLFB can greatly boost the generation of free Li+ and improve the Li+ transference numbers (tLi+=0.92) at room temperature. Moreover, combined with theoretical calculation and experimental results, the changes in the composition and properties of the composite electrolyte membrane with the addition of anionic receptors are systematically studied, which further implies the intrinsic mechanism of the stability difference. In addition, the PLFB-based SSB assembled by LiNi0.8Co0.1Mn0.1O2 cathode and lithium anode exhibits a high capacity retention of 86% after loop 400 cycles. This investigation on boosted battery performance by immobilized anions not only contributes to the directional construction of dendrite-free and lithium-ion permeable interface, but also brings new opportunities for the screening and design of the next generation of high-energy SSBs.

High-voltage lithium-metal batteries enabled by ethylene glycol bis(propionitrile) ether-LiNO3 synergetic additives.

The employment of Li metal anodes is a key to realizing ultra-high energy batteries. However, the commercialization of lithium metal batteries (LMBs) remains challenging partially due to the thermodynamic instability and competitive oxidative decomposition of the solvent. Herein, a bi-functional electrolyte for stabilizing the interfaces of both the Li metal anode and LiCoO2 (LCO) cathode is designed by introducing lithium nitrate (LiNO3) through Ethylene Glycol Bis(Propionitrile) Ether (DENE). For the anode, the C8H12N2O2-LiNO3 coordination-solvation contributes to forming a stable Li3N-enhanced solid electrolyte interphase (SEI), which increases the average Li coulombic efficiency (CE) up to 98.5%. More importantly, in situ electrochemical dilatometry further reveals that the highly reversible behavior and a low volume expansion of lithium deposition are related to the stable Li3N-enhanced SEI. The designed electrolyte enables the Li‖LCO cell to achieve an average CE of 99.2% and a high capacity retention of 88.2% up to 4.6 V after 100 cycles. This work provides a strategic guidance in developing high-voltage Li‖LCO batteries with dual electrolyte additives.