Present understanding of the stability of Li-stuffed garnets with moisture, carbon dioxide, and metallic lithium

Hofstetter, Kyle; Samson, Alfred Junio; Narayanan, Sumaletha; Thangadurai, Venkataraman

doi:10.1016/j.jpowsour.2018.04.016

Cited by 111 publications

(107 citation statements)

References 94 publications

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“…An intermediate layer is often included to enhance the adhesion between garnet SIEs and Li electrodes. Lithiophilic materials such as Si, Ge, ZnO, and Al 2 O 3 or polymers such as PVDF‐HFP and PEO are sandwiched at the interface to decrease the interfacial resistance . A Li‐Sn alloy layer was demonstrated to lower the interfacial resistance approximately 20 times .…”

Section: Solid‐state Electrolytesmentioning

confidence: 99%

Electrolytes for Rechargeable Lithium–Air Batteries

et al. 2019

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Lithium–air batteries are promising devices for electrochemical energy storage because of their ultrahigh energy density. However, it is still challenging to achieve practical Li–air batteries because of their severe capacity fading and poor rate capability. Electrolytes are the prime suspects for cell failure. In this Review, we focus on the opportunities and challenges of electrolytes for rechargeable Li–air batteries. A detailed summary of the reaction mechanisms, internal compositions, instability factors, selection criteria, and design ideas of the considered electrolytes is provided to obtain appropriate strategies to meet the battery requirements. In particular, ionic liquid (IL) electrolytes and solid‐state electrolytes show exciting opportunities to control both the high energy density and safety.

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Section: Solid‐state Electrolytesmentioning

confidence: 99%

Electrolytes for Rechargeable Lithium–Air Batteries

et al. 2019

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“…Several recent studies have suggested that intrashort circuits are likely to be formed because of the localized electrodeposition of lithium in pre‐existing flaws due to the build‐up of crack‐tip stress and the corresponding crack propagation that finally causes the solid electrolyte to mechanically fail 22–24. Other researchers have also proposed that the interfacial resistance between an electrode and LLZO is not only the source of slow SSB kinetics, but it significantly contributes to short‐circuit failure 20,25–29. Poor contact between lithium metal and LLZO has been reported to cause large interfacial resistance that results in an inhomogeneously distributed current that triggers such failure 19,26,27,30.…”

Section: Introductionmentioning

confidence: 99%

The Role of Interlayer Chemistry in Li‐Metal Growth through a Garnet‐Type Solid Electrolyte

Kim

Jung

Kim

et al. 2020

Advanced Energy Materials

150

130

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Securing the chemical and physical stabilities of electrode/solid‐electrolyte interfaces is crucial for the use of solid electrolytes in all‐solid‐state batteries. Directly probing these interfaces during electrochemical reactions would significantly enrich the mechanistic understanding and inspire potential solutions for their regulation. Herein, the electrochemistry of the lithium/Li7La3Zr2O12‐electrolyte interface is elucidated by probing lithium deposition through the electrolyte in an anode‐free solid‐state battery in real time. Lithium plating is strongly affected by the geometry of the garnet‐type Li7La3Zr2O12 (LLZO) surface, where nonuniform/filamentary growth is triggered particularly at morphological defects. More importantly, lithium‐growth behavior significantly changes when the LLZO surface is modified with an artificial interlayer to produce regulated lithium depositions. It is shown that lithium‐growth kinetics critically depend on the nature of the interlayer species, leading to distinct lithium‐deposition morphologies. Subsequently, the dynamic role of the interlayer in battery operation is discussed as a buffer and seed layer for lithium redistribution and precipitation, respectively, in tailoring lithium deposition. These findings broaden the understanding of the electrochemical lithium‐plating process at the solid‐electrolyte/lithium interface, highlight the importance of exploring various interlayers as a new avenue for regulating the lithium‐metal anode, and also offer insight into the nature of lithium growth in anode‐free solid‐state batteries.

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“…The use of Li metal with extremely large gravimetric specific capacity (3860 mAh g −1 ) with the lowest redox potential as an anode leads to the high energy density of a battery, but the formation of a solid-solid interface among garnet-type SE and Li metal electrodes is another challenging issue in achieving better electrochemical performance in solid-state batteries [32][33][34]. Many approaches have been introduced to reduce the interfacial charge-transfer resistance between garnet-type SE and Li, including the introduction of thin film layers of Au [35], Si [36], Ge [37], Al 2 O 3 [38], and ZnO [39], or eliminating the secondary phases, such as LiOH and Li 2 CO 3 , by polishing the surface of SE and using multiple thermal treatments at specific temperatures before and after contact with Li [40][41][42].…”

Section: Introductionmentioning

confidence: 99%

Formation and Stability of Interface between Garnet-Type Ta-doped Li7La3Zr2O12 Solid Electrolyte and Lithium Metal Electrode

et al. 2018

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Garnet-type Li 7-x La 3 Zr 2-x Ta x O 12 (LLZT) is considered a good candidate for the solid electrolyte in all-solid-state lithium batteries because of its reasonably high conductivity around 10 −3 S cm −1 at room temperature and stability against lithium (Li) metal with the lowest redox potential. In this study, we synthesized LLZT with a tantalum (Ta) content of 0.45 via a conventional solid-state reaction process and constructed a Li/LLZT/Li symmetric cell by attaching Li metal foils on the polished top and bottom surfaces of an LLZT pellet. We investigated the influence of heating temperatures and times on the interfacial charge-transfer resistance between LLZT and the Li metal electrode. In addition, the effect of the interface resistance on the stability for Li deposition and dissolution was examined using a galvanostatic cycling test. The lowest interfacial resistance of 25 Ω cm 2 at room temperature was obtained by heating at 175 • C (5 • C lower than the melting point of Li) for three to five hours. We confirmed that the current density at which the short circuit occurs in the Li/LLZT/Li cell via the propagation of Li dendrite into LLZT increases with decreasing interfacial charge transfer resistance.

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Present understanding of the stability of Li-stuffed garnets with moisture, carbon dioxide, and metallic lithium

Cited by 111 publications

References 94 publications

Electrolytes for Rechargeable Lithium–Air Batteries

Electrolytes for Rechargeable Lithium–Air Batteries

The Role of Interlayer Chemistry in Li‐Metal Growth through a Garnet‐Type Solid Electrolyte

Formation and Stability of Interface between Garnet-Type Ta-doped Li7La3Zr2O12 Solid Electrolyte and Lithium Metal Electrode

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