Water‐Mediated Synthesis of a Superionic Halide Solid Electrolyte

Li, Xiaona; Liang, Jianwen; Chen, Ning; Luo, Jing; Adair, Keegan R.; Wang, Changhong; Banis, Mohammad Norouzi; Sham, Tsun‐Kong; Zhang, Li; Zhao, Shangqian; Lu, Shigang; Huang, Huan; Li, Ruying; Sun, Xueliang

doi:10.1002/anie.201909805

Cited by 307 publications

(336 citation statements)

References 44 publications

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“…Recently, lithium chlorides were demonstrated as an emerging class of solid electrolytes with high ionic conductivity and good electrochemical stability . In order to develop new solid electrolyte materials with good moisture stability while maintaining good electrochemical stability and ionic conductivity, the effects of different cations, anions, and compositions on moisture stability need to be systematically studied and understood …”

Section: Figurementioning

confidence: 99%

Materials Design Principles for Air‐Stable Lithium/Sodium Solid Electrolytes

Zhu

2020

Angewandte Chemie

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Sulfide solid electrolytes are promising inorganic solid electrolytes for all‐solid‐state batteries. Despite their high ionic conductivity and desirable mechanical properties, many known sulfide solid electrolytes exhibit poor air stability. The spontaneous hydrolysis reactions of sulfides with moisture in air lead to the release of toxic hydrogen sulfide and materials degradation, hindering large‐scale manufacturing and applications of sulfide‐based solid‐state batteries. In this work, we systematically investigate the hydrolysis and reduction reactions in Li‐ and Na‐containing sulfides and chlorides by applying thermodynamic analyses based on a first principles computation database. We reveal the stability trends among different chemistries and identify the effect of cations, anions, and Li/Na content on moisture stability. Our results identify promising materials systems to simultaneously achieve desirable moisture stability and electrochemical stability, and provide the design principles for the development of air‐stable solid electrolytes.

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Section: Figurementioning

confidence: 99%

Materials Design Principles for Air‐Stable Lithium/Sodium Solid Electrolytes

Zhu

2020

Angewandte Chemie

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“…Many SSEs have been reported, including lithium phosphorus oxynitride (LiPON) 3 , sul de-type 4 , sodium superionic conductor (NASICON)-type 5,6 , perovskite-type 7 , halide-type 8 , and garnet-type 9 . Among them, garnet-type Li 7 La 3 Zr 2 O 12 (LLZO) is promising because of its excellent chemical/electrochemical stability with Li metal and its high ionic conductivity at room temperature 10,11 .…”

Section: Introductionmentioning

confidence: 99%

A Flexible Electron-blocking Interfacial Shield for Dendrite-free Solid Lithium Metal Batteries

Huo

Gao

Zhao

et al. 2020

Preprint

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Solid-state batteries (SSBs) are considered to be the next-generation lithium-ion battery technology due to their enhanced energy density and safety. However, the high electronic conductivity of solid-state electrolytes (SSEs) leads to Li dendrite nucleation and proliferation. Uneven electric-field distribution resulting from poor interfacial contact can further promote dendritic deposition and lead to rapid short circuiting of SSBs. Herein, a flexible electron-blocking interfacial shield (EBS) is proposed to protect garnet electrolytes from the electronic degradation. The EBS formed by an in-situ substitution reaction can not only increase lithiophilicity but also stabilize the Li volume change, maintaining the integrity of the interface during repeated cycling. Density functional theory calculations show a high electron-tunneling energy barrier from Li metal to the EBS, indicating an excellent capacity for electron-blocking. EBS protected cells exhibit an improved critical current density of 1.2 mA cm-2 and stable cycling for over 400 h at 1 mA cm-2 (1 mAh cm-2) at room temperature. These results demonstrate an effective strategy for the suppression of Li dendrites and present fresh insight into the rational design of the SSE and Li metal interface.

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“…123,124 Another potential type of coating material include halide-based SEs such as Li 3 InCl 6 and Li 3 YCl 6 since recently they were found to be stable with LCO. 48,125,126 Chloride-based SEs have shown significant electrochemical stability (4.2 V vs Li/Li + ) compared with other oxide-based coating materials. However, considering 5 V cathodes such as Lirich layered oxides or spinel cathodes, coatings with even higher oxidation stability are required; in this case, fluoride-based SEs may be considered.…”

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confidence: 99%

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

et al. 2020

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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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Water‐Mediated Synthesis of a Superionic Halide Solid Electrolyte

Cited by 307 publications

References 44 publications

Materials Design Principles for Air‐Stable Lithium/Sodium Solid Electrolytes

Materials Design Principles for Air‐Stable Lithium/Sodium Solid Electrolytes

A Flexible Electron-blocking Interfacial Shield for Dendrite-free Solid Lithium Metal Batteries

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

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