Mechanical regulation of lithium intrusion probability in garnet solid electrolytes

McConohy, Geoff; Xu, Xin; Cui, Teng; Barks, Edward; Wang, Sunny; Kaeli, Emma; Melamed, Celeste; Gu, Xiaowei; Chueh, William C.

doi:10.1038/s41560-022-01186-4

Cited by 42 publications

(67 citation statements)

References 49 publications

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“…Different protocols for regeneration of LLZO have been reported, wherein the samples have been treated under a variety of gases and temperatures. ,− Despite this, the minimum temperature needed to regenerate the surface has not been definitively established, and the effect of different gases has not yet been systematically studied. It has also been reported that excessive heating of LLZO results in pyrochlore formation.…”

Section: Gixrd Measurements Under Different Gas Environmentsmentioning

confidence: 99%

Understanding the Surface Regeneration and Reactivity of Garnet Solid-State Electrolytes

et al. 2023

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Garnet solid-electrolyte-based Li-metal batteries can be used in energy storage devices with high energy densities and thermal stability. However, the tendency of garnets to form lithium hydroxide and carbonate on the surface in an ambient atmosphere poses significant processing challenges. In this work, the decomposition of surface layers under various gas environments is studied by using two surface-sensitive techniques, near-ambient-pressure X-ray photoelectron spectroscopy and grazing incidence X-ray diffraction. It is found that heating to 500 °C under an oxygen atmosphere (of 1 mbar and above) leads to a clean garnet surface, whereas low oxygen partial pressures (i.e., in argon or vacuum) lead to additional graphitic carbon deposits. The clean surface of garnets reacts directly with moisture and carbon dioxide below 400 and 500 °C, respectively. This suggests that additional CO2 concentration controls are needed for the handling of garnets. By heating under O2 along with avoiding H2O and CO2, symmetric cells with less than 10 Ωcm2 interface resistance are prepared without the use of any interlayers; plating currents of >1 mA cm–2 without dendrite initiation are demonstrated.

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Section: Gixrd Measurements Under Different Gas Environmentsmentioning

confidence: 99%

Understanding the Surface Regeneration and Reactivity of Garnet Solid-State Electrolytes

et al. 2023

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“…Second, inherent defects in the solid electrolytes could render the anode interface non-uniform. Therefore, these defects could potentially lead to the redox reaction preferentially occurring at the interface, [88,89] which would eventually result in the formation of dendrites. [90] Even if the interlayers discussed in this section were used to stabilize the interface, this irregularity at the surface of solid electrolytes could undermine the efficacy of the interlayers.…”

Section: Strategies To Maintain a Conformal Interface During Prolonge...mentioning

confidence: 99%

Design Strategies for Anodes and Interfaces Toward Practical Solid‐State Li‐Metal Batteries

Yoon

Kim

2023

Advanced Science

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Solid‐state Li–metal batteries (based on solid‐state electrolytes) offer excellent safety and exhibit high potential to overcome the energy‐density limitations of current Li–ion batteries, making them suitable candidates for the rapidly developing fields of electric vehicles and energy‐storage systems. However, establishing close solid–solid contact is challenging, and Li‐dendrite formation in solid‐state electrolytes at high current densities causes fatal technical problems (due to high interfacial resistance and short‐circuit failure). The Li metal/solid electrolyte interfacial properties significantly influence the kinetics of Li–metal batteries and short‐circuit formation. This review discusses various strategies for introducing anode interlayers, from the perspective of reducing the interfacial resistance and preventing short‐circuit formation. In addition, 3D anode structural‐design strategies are discussed to alleviate the stress caused by volume changes during charging and discharging. This review highlights the importance of comprehensive anode/electrolyte interface control and anode design strategies that reduce the interfacial resistance, hinder short‐circuit formation, and facilitate stress relief for developing Li–metal batteries with commercial‐level performance.

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“…Due to the complexity and instability of the SEI layer formed in liquid electrolytes, its composition and properties are difficult to regulate. To avoid problems caused by liquid electrolytes, solid-state electrolytes have been widely used in lithium ion batteries. − However, their low electrical conductivity and weak mechanical stability limit their large-scale practical application. − This limitation is primarily attributed to nanocracking and the subsequent formation of lithium dendrites, which can occur either due to preexisting flaws or external forces . The presence of lithium dendrites further diminishes the electrical conductivity and mechanical stability of the electrolyte.…”

Section: All-solid-state Lithium Batterymentioning

confidence: 99%

“…Lithium dendrites are generally rodlike, treelike, and mossylike lithium deposits. Dendrite growth leads to three critical problems: (1) Dendrites can puncture the cathode-side membrane, leading to cell short circuits, fires, and even explosions. − (2) Dendrites constantly have a large surface area and react readily with electrolytes, which drastically consume active materials and lower the efficiency of cells, and the uneven dissolution of lithium dendrites will produce “dead lithium” (SEI film-wrapped lithium metal that is unable to continue taking part in electrochemical processes). , (3) The unstable SEI and the decomposition of “dead lithium” cause significant volume changes. This dramatic volume expansion can severely damage the electrode–electrolyte interface.…”

Section: Introductionmentioning

confidence: 99%

Recent Progress on Nanomodification Applied in Anodes of Rechargeable Li Metal Batteries

Yao,

Li,

Chen

et al. 2023

ACS Appl. Energy Mater.

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Lithium metal anodes (LMAs) are considered one of the most promising anode materials for lithium metal batteries due to their high theoretical specific capacity (3860 mAh g −1 ) and low anode potential (−3.04 V compared to the standard hydrogen potential). However, the further application of lithium metal batteries is hindered by problems such as lithium dendrite growth and volume change of the anode. Fortunately, to address these issues in lithium metal batteries, various applications of nanomodification technologies have been proposed for lithium metal anodes, such as using nanomaterials and constructing nanostructures. These nanomodification technologies have standardized the plating/stripping behavior of lithium, significantly improving the electrochemical performance and lithium morphology of LMAs. This brief review systematically summarizes the latest research progress in LMA nanomodification technology to inhibit lithium dendrite growth. First, the problems of LMAs in practical applications are analyzed. Then, we summarize the forward-looking strategies and the latest research progress based on nanomaterials and nanostructures from the perspectives of current collectors, protection of the interface layer, separators, and all-solid-state lithium batteries. Finally, the future development of nanomodification technology for the protection of lithium metal batteries is summarized and prospected.

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Mechanical regulation of lithium intrusion probability in garnet solid electrolytes

Cited by 42 publications

References 49 publications

Understanding the Surface Regeneration and Reactivity of Garnet Solid-State Electrolytes

Understanding the Surface Regeneration and Reactivity of Garnet Solid-State Electrolytes

Design Strategies for Anodes and Interfaces Toward Practical Solid‐State Li‐Metal Batteries

Recent Progress on Nanomodification Applied in Anodes of Rechargeable Li Metal Batteries

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