Commercial lithium-ion (Li-ion) batteries suffer from low energy density and do not meet the growing demands of the energy storage market. Therefore, building next-generation rechargeable Li and Li-ion batteries with higher energy densities, better safety characteristics, lower cost and longer cycle life is of outmost importance. To achieve smaller and lighter next-generation rechargeable Li and Li-ion batteries that can outperform commercial Li-ion batteries, several new energy storage chemistries are being extensively studied. In this review, we summarize the current trends and provide guidelines towards achieving this goal, by addressing batteries using high-voltage cathodes, metal fluoride electrodes, chalcogen electrodes, Li metal anodes, high-capacity anodes as well as useful electrolyte solutions. We discuss the choice of active materials, practically achievable energy densities and challenges faced by the respective battery systems. Furthermore, strategies to overcome remaining challenges for achieving energy characteristics are addressed in the hope of providing a useful and balanced assessment of current status and perspectives of rechargeable Li and Li-ion batteries.

Guidelines and trends for next-generation rechargeable lithium and lithium-ion batteries.

Commercialization of Lithium Battery Technologies for Electric Vehicles

Solid-state batteries have been attracting wide attention for next generation energy storage devices due to the probability to realize higher energy density and superior safety performance compared with the state-of-the-art lithium ion batteries. However, there are still intimidating challenges for developing low cost and industrially scalable solid-state batteries with high energy density and stable cycling life for large-scale energy storage and electric vehicle applications. This review presents an overview on the scientific challenges, fundamental mechanisms, and design strategies for solid-state batteries, specifically focusing on the stability issues of solid-state electrolytes and the associated interfaces with both cathode and anode electrodes. First, we give a brief overview on the history of solid-state battery technologies, followed by introduction and discussion on different types of solid-state electrolytes. Then, the associated stability issues, from phenomena to fundamental understandings, are intensively discussed, including chemical, electrochemical, mechanical, and thermal stability issues; effective optimization strategies are also summarized. State-of-the-art characterization techniques and in situ and operando measurement methods deployed and developed to study the aforementioned issues are summarized as well. Following the obtained insights, perspectives are given in the end on how to design practically accessible solid-state batteries in the future.

Approaching Practically Accessible Solid-State Batteries: Stability Issues Related to Solid Electrolytes and Interfaces

All-solid-state batteries (ASSBs) have attracted enormous attention as one of the critical future technologies for safe and high energy batteries. With the emergence of several highly conductive solid electrolytes in recent years, the bottleneck is no longer Li-ion diffusion within the electrolyte. Instead, many ASSBs are limited by their low Coulombic efficiency, poor power performance, and short cycling life due to the high resistance at the interfaces within ASSBs. Because of the diverse chemical/physical/mechanical properties of various solid components in ASSBs as well as the nature of solid-solid contact, many types of interfaces are present in ASSBs. These include loose physical contact, grain boundaries, and chemical and electrochemical reactions to name a few. All of these contribute to increasing resistance at the interface. Here, we present the distinctive features of the typical interfaces and interphases in ASSBs and summarize the recent work on identifying, probing, understanding, and engineering them. We highlight the complicated, but important, characteristics of interphases, namely the composition, distribution, and electronic and ionic properties of the cathode-electrolyte and electrolyte-anode interfaces; understanding these properties is the key to designing a stable interface. In addition, conformal coatings to prevent side reactions and their selection criteria are reviewed. We emphasize the significant role of the mechanical behavior of the interfaces as well as the mechanical properties of all ASSB components, especially when the soft Li metal anode is used under constant stack pressure. Finally, we provide full-scale (energy, spatial, and temporal) characterization methods to explore, diagnose, and understand the dynamic and buried interfaces and interphases. Thorough and in-depth understanding on the complex interfaces and interphases is essential to make a practical high-energy ASSB.

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Interfaces and Interphases in All-Solid-State Batteries with Inorganic Solid Electrolytes.

Low Resistance–Integrated All-Solid-State Battery Achieved by Li7La3Zr2O12 Nanowire Upgrading Polyethylene Oxide (PEO) Composite Electrolyte and PEO Cathode Binder

Solid composite electrolytes (SCEs) that combine the advantages of solid polymer electrolytes (SPEs) and inorganic ceramic electrolytes (ICEs) present acceptable ionic conductivity, high mechanical strength, and favorable interfacial contact with electrodes, which greatly improve the electrochemical performance of all-solid-state batteries compared to single SPEs and ICEs. However, there are many challenges to overcome before the practical application of SCEs, including the low ionic conductivity less than 10-3 S cm-1 at ambient temperature, poor interfacial stability, and high interfacial resistance, which greatly restrict the room temperature performance. Herein, the advances of SCEs applied in all-solid-state lithium batteries are presented, including the Li ion migration mechanism of SCEs, the strategies to enhance the ionic conductivity of SCEs by various morphologies of ICEs, and construction methods of the low resistance and stable interfaces of SCEs with both cathode and anode. Finally, some typical applications of SCEs in lithium batteries are summarized and future development directions are prospected. This work presents how it is quite significant to further enhance the ionic conductivity of SCEs by developing the novel SPEs with the special morphology of ICEs for advanced all-solid-state lithium batteries.

https://onlinelibrary.wiley.com/doi/epdf/10.1002/advs.201903088

Progress and Perspective of Ceramic/Polymer Composite Solid Electrolytes for Lithium Batteries

Progress and Perspective of Solid-State Lithium–Sulfur Batteries

Constructing Multifunctional Interphase between Li1.4Al0.4Ti1.6(PO4)3 and Li Metal by Magnetron Sputtering for Highly Stable Solid-State Lithium Metal Batteries

The garnet electrolyte presents poor wettability with Li metal, resulting in an extremely large interfacial impedance and drastic growth of Li dendrites. Herein, a novel ultra-stable conductive composite interface (CCI) consisting of Liy Sn alloy and Li3 N is constructed in situ between Li6.4 La3 Zr1.4 Ta0.6 O12 (LLZTO) pellet and Li metal by a conversion reaction of SnNx with Li metal at 300 °C. The Liy Sn alloy as a continuous and robust bridge between LLZTO and Li metal can effectively reduce the LLZTO/Li interfacial resistance from 4468.0 Ω to 164.8 Ω. Meanwhile, the Li3 N as a fast Li-ion channel can efficiently transfer Li ions and give their uniform distribution at the LLZTO/Li interface. Therefore, the Li/LLZTO@CCI/Li symmetric battery stably cycles for 1200 h without short circuit, and the all-solid-state high-voltage Li/LLZTO@CCI/LiNi0.5 Co0.2 Mn0.3 O2 battery achieves a specific capacity of 161.4 mAh g-1 at 0.25 C with a capacity retention rate of 92.6 % and coulombic efficiency of 100.0 % after 200 cycles at 25 °C.

Lu Shen

Papers

Low Resistance–Integrated All-Solid-State Battery Achieved by Li7La3Zr2O12 Nanowire Upgrading Polyethylene Oxide (PEO) Composite Electrolyte and PEO Cathode Binder

Progress and Perspective of Ceramic/Polymer Composite Solid Electrolytes for Lithium Batteries

Progress and Perspective of Solid-State Lithium–Sulfur Batteries

Constructing Multifunctional Interphase between Li1.4Al0.4Ti1.6(PO4)3 and Li Metal by Magnetron Sputtering for Highly Stable Solid-State Lithium Metal Batteries

In Situ Construction of an Ultra‐Stable Conductive Composite Interface for High‐Voltage All‐Solid‐State Lithium Metal Batteries