All-solid-state battery (ASSB) has been widely recognized as the critical next-generation energy storage technology due to its high energy density and safety. However, stable cycling at high cathode loadings is...

High-Areal-Capacity and Long-Cycle-Life All-Solid-State Battery Enabled By Freeze Drying Technology

Realizing long-cycling all-solid-state Li-In||TiS2 batteries using Li6+xMxAs1-xS5I (M=Si, Sn) sulfide solid electrolytes

In recent years, solid-state lithium batteries (SSLBs) using solid electrolytes (SEs) have been widely recognized as the key next-generation energy storage technology due to its high safety, high energy density, long cycle life, good rate performance and wide operating temperature range. However, SSLBs still suffer from many obstacles that hinder their practical application. This review discusses typical lithium-ion conductors and their in-depth lithium-ion conduction mechanism. The key interfacial problems of electrolytes and electrodes for SSLBs are comprehensively elaborated and several possible solution methods are proposed. Furthermore, three viable manufacturing strategies for free-standing thin SE membranes are discussed in details. Moreover, for the first time, the government policies and latest company industrialization process relative to SSLBs worldwide are systematically summarized. Finally, several potential strategies are identified for the future development of high-energy-density SSLBs. 

Solid-State Lithium Batteries-From Fundamental Research to Industrial Progress

All-solid-state Li-metal batteries (ASSLBs) using inorganic solid electrolyte (SE) are considered as promising alternatives to conventional Li-ion batteries, offering improved safety and boosted energy density. While significant progress has been made on improving the ionic conductivity of SEs, the degradation and instability of Li metal/inorganic SE interfaces have become the critical challenges that limit the coulombic efficiency, power performance and cycling stability of ASSLBs. Understanding the mechanisms of complex/dynamic interfacial phenomena is of great importance to addressing these issues. Herein, recent studies on identifying, understanding and solving interfacial issues on anode side in ASSLBs are comprehensively reviewed. Typical issues at Li metal/SE interface include Li dendrite growth/propagation, SE cracking, physical contact loss and electrochemical reactions, which lead to high interfacial resistance and cell-failure. The causes of these issues relating to the chemical, physical and mechanical properties of Li metal and SEs are systematically discussed. Furthermore, effective mitigating strategies are summarized and their effects on suppressing interfacial reactions, improving interfacial Li ion transport, maintaining interfacial contact and stabilizing Li plating/stripping are highlighted. The in-depth mechanistic understanding of interfacial issues and complete investigations on current solutions provide foundations and guidance for future research and development to realize practical application of high-performance ASSLB. 

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/eem2.12613

Anode Interfacial Issues in
 Solid‐State
 Li Batteries: Mechanistic Understanding and Mitigating Strategies

Machine learning (ML) exhibits substantial potential for predicting the properties of solid‐state electrolytes (SSEs). By integrating experimental or/and simulation data within ML frameworks, the discovery and development of advanced SSEs can be accelerated, ultimately facilitating their application in high‐end energy storage systems. This review commences with an introduction to the background of SSEs, including their explicit definition, comprehensive classification, intrinsic physical/chemical properties, underlying mechanisms governing their conductivity, challenges, and future developments. An in‐depth explanation of the ML methodology is also elucidated. Subsequently, the key factors that influence the performance of SSEs are summarized, including thermal expansion, modulus, diffusivity, ionic conductivity, reaction energy, migration barrier, band gap, and activation energy. Finally, it is offered perspectives on the design prerequisites for upcoming generations of SSEs, focusing on real‐time property prediction, multi‐property optimization, multiscale modeling, transfer learning, automation and high‐throughput experimentation, and synergistic optimization of full battery, all of which are crucial for accelerating the progress in SSEs. This review aims to guide the design and optimization of novel SSE materials for the practical realization of efficient and reliable SSEs in energy storage technologies.

Machine Learning‐Assisted Property Prediction of Solid‐State Electrolyte

Rechargeable FeS2 battery has been regarded as a promising energy storage device, due to its potentially high energy density and ultralow cost. However, the short lifespan associated with the shuttle effect of polysulfides, large volume change, agglomeration of Fe0 nanoparticles, narrow operating temperature range, and sluggish reaction kinetics, greatly impede the application of rechargeable FeS2 lithium‐ion batteries. Herein, an all‐solid‐state battery (ASSB) coupling commercialized FeS2 is proposed with a novel superionic conductor Li6.8Si0.8As0.2S5I (LASI‐80Si) to overcome these challenges. The shuttle effect of polysulfides and volume change of FeS2 are suppressed or completely eliminated in ASSB, due to solid‐solid conversion of Li2S/S and large stacking pressure, respectively. Furthermore, the operating temperature range (−60–60 °C) is significantly expanded by the ultra‐high and temperature‐insensitive ionic conductivity of LASI‐80Si (Ea = 0.20 eV), along with the superior FeS2/LASI‐80Si interface stability. Thanks to the extra Li+ provided by Li2S and LiI functional phases, the “bridge” effect of LiI on facile interfacial Li‐ion conduction, and the enhanced reaction kinetics of LASI‐80Si ( σLi+=${\sigma _{L{i^ + }}} = $ 10.4 mS cm−1), ASSBs with LASI‐80Si deliver long cycle life (244 cycles at 0.1 C and 600 cycles at 1 C), superior rate capability (20 C), high areal mass loading (13.37 mg cm−2), and ultrahigh areal capacity (9.05 mAh cm−2). These inspiring results demonstrate the enormous potential of LASI‐80Si and FeS2 combination for practical application of wide‐temperature and large‐capacity ASSBs.

Wide‐Temperature, Long‐Cycling, and High‐Loading Pyrite All‐Solid‐State Batteries Enabled by Argyrodite Thioarsenate Superionic Conductor

Metal fluoride–lithium batteries with potentially high‐energy densities are regarded as promising candidates for next‐generation low‐cost rechargeable batteries. However, liquid‐electrolyte metal fluoride–lithium batteries suffer from sluggish reaction kinetics, high voltage hysteresis due to side reactions, poor rate capability, and rapid capacity drop during cycling. Moreover, the research on sulfide all‐solid‐state batteries (ASSBs) with metal fluoride cathode is still lacking. Herein, four kinds of iron fluoride materials are applied to the sulfide all‐solid‐state lithium battery system for the first time to investigate the best cathode and corresponding methods. Electrochemical tests showed the cycling performance at different current densities (0.1, 0.3, and 1 C) and rate performance of the four cathodes with the following rules: FeF3‐HT > FeF3‐RT > FeF3·0.33H2O > FeF3·3H2O. The reversible capacities of FeF3‐HT AASB are 519.9 mAh g−1 after 120 cycles at 0.3C and still maintains 340.7 mAh g−1 after 400 cycles even at a high rate of 1 C. In addition, electro impedence spectroscopy and cyclic voltammetry tests of the above four cathodes show that different contents of crystal water, morphologies, and particle sizes have a great influence on the lithium storage mechanism of cathode. Moreover, the reason for the FeF3‐HT cathode's superior specific capacity and rate performance compared with other cathodes at high current densities is revealed, according to cyclic voltammogram tests under different scan rates. The cause is that FeF3‐HT has the highest proportion of the contribution capacity of the cathode surface control process. The above research opens up a new avenue for FeF3‐HT, FeF3‐RT, FeF3·0.33H2O, and FeF3·3H2O cathodes in sulfide ASSBs.

High‐Capacity, Long‐Life Iron Fluoride All‐Solid‐State Lithium Battery with Sulfide Solid Electrolyte

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Wide‐Temperature, Long‐Cycling, and High‐Loading Pyrite All‐Solid‐State Batteries Enabled by Argyrodite Thioarsenate Superionic Conductor

High‐Capacity, Long‐Life Iron Fluoride All‐Solid‐State Lithium Battery with Sulfide Solid Electrolyte