Advances, challenges and environmental impacts in metal-air battery electrolytes

Conventional lithium-ion batteries with inflammable organic liquid electrolytes are required to make a breakthrough regarding their bottlenecks of energy density and safety, as demanded by the ever-increasing development of electric vehicles and grids. In this context, solid-state lithium batteries (SSLBs), which replace liquid electrolytes with solid counterparts, have become a popular research topic due to their excellent potential in the realization of improved energy density and safety. However, in practice, the energy density of SSLBs is limited by the cathode mass loading, electrolyte thickness and anode stability. Moreover, the crucial interfacial issues related to the rigid and heterogeneous solid-solid contacts between the electrolytes and electrodes, including inhomogeneous local potential distributions, sluggish ion transport, side reactions, space charge barriers and stability degradation, severely deteriorate the cycle life of SSLBs. Solidification, which converts a liquid into a solid inside a solid battery, represents a powerful tool to overcome the aforementioned obstacles. The liquid precursors fully wet the interfaces and infiltrate the electrodes, followed by in-situ conformal solidification under certain conditions for the all-in-one construction of cells with highly conducting, closely contacted and sustainable electrode/electrolyte interfaces, thereby enabling high energy density and long cycle life. Therefore, in this review, we address the research progress regarding the latest strategies toward the solidification of the electrolyte layers and the interfaces between the electrodes and electrolytes. The critical challenges and future research directions are proposed for the solidification strategies in SSLBs from both science and engineering perspectives.

/pdf/solidification-for-solid-state-lithium-batteries-with-high-5900k7fj.pdf

Solidification for solid-state lithium batteries with high energy density and long cycle life

Succinonitrile‐based plastic crystal electrolytes have emerged for high‐energy‐density Li metal batteries in terms of their superior ambient ionic conductivity, low flammability, and benign compatibility with high voltage cathode, but are hampered by inherent instabilities toward Li anodes. Constructing hierarchical solid electrolytes structure is a fundamental approach to protect Li anode from succinonitrile attacks, with succinonitrile‐based oxidation‐resistance layer facing high voltage cathode and reduction‐tolerant layer contacting Li anode. However, free succinonitrile molecules in succinonitrile‐based electrolyte layer can diffuse across the electrolyte/electrolyte interface and further reach Li anode surface during the battery cycle. This chemical “crosstalk” cause reduction‐tolerant electrolyte layer to fail to protect the Li anode from the attacks of free succinonitrile molecules. Nano Li6.4La3Zr1.4Ta0.6O12 is introduced creatively into succinonitrile‐based electrolyte layer. By taking advantage of the complexation between La atoms in Li6.4La3Zr1.4Ta0.6O12 and N atoms in succinonitrile, the free succinonitrile molecules are successfully immobilized in succinonitrile‐based electrolyte layer. The resulting low resistance and highly durable solid electrolyte interphase and cathode electrolyte interphase endow NCM622||Li batteries with remarkable cycle stability. Our research provides a new idea for the real application of plastic crystal electrolytes in high voltage solid‐state lithium metal batteries.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/eem2.12367

Unveiling and Alleviating Chemical “Crosstalk” of Succinonitrile Molecules in Hierarchical Electrolyte for High‐Voltage Solid‐State Lithium Metal Batteries

With the increasing use of Li batteries for storage, their safety issues and energy densities are attracting considerable attention. Recently, replacing liquid organic electrolytes with solid‐state electrolytes (SSE) has been hailed as the key to developing safe and high‐energy‐density Li batteries. In particular, Li1+xAlxTi2−x(PO4)3 (LATP) has been identified as a very attractive SSE for Li batteries due to its excellent electrochemical stability, low production costs, and good chemical compatibility. However, interfacial reactions with electrodes and poor thermal stability at high temperatures severely restrict the practical use of LATP in solid‐state batteries (SSB). Herein, a systematic review of recent advances in LATP for SSBs is provided. This review starts with a brief introduction to the development history of LATP and then summarizes its structure, ion transport mechanism, and synthesis methods. Challenges (e.g., intrinsic brittleness, interfacial resistance, and compatibility) and corresponding solutions (ionic substitution, additives, protective layers, composite electrolytes, etc.) that are critical for practical applications are then discussed. Last, an outlook on the future research direction of LATP‐based SSB is provided.

Recent Advances in Conduction Mechanisms, Synthesis Methods, and Improvement Strategies for Li1+xAlxTi2−x(PO4)3 Solid Electrolyte for All‐Solid‐State Lithium Batteries

Interface Reconstruction via Lithium Thermal Reduction to Realize a Long Life All-solid-state Battery

Localization of electrons within interlayer stabilizes NASICON-type solid-state electrolyte

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Localization of electrons within interlayer stabilizes NASICON-type solid-state electrolyte