Initiation of dendritic failure of LLZTO <i>via</i> sub-surface lithium deposition

Siniscalchi, Marco; Shi, Yifu; Li, Guanchen; Gibson, Joshua S.; Weatherup, Robert S.; Bonilla, Ruy S.; Speller, Susannah C.; Grovenor, Chris R. M.

doi:10.1039/d3ee03916a

Cited by 5 publications

(1 citation statement)

References 46 publications

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“…As a direct consequence, during cycling, the local current density at the active regions of the Li/LLZTO interface becomes much larger than the nominal applied value. This local current density concentration can result in adverse effects, such as cell polarization and formation of lithium dendrites through the SE, , inevitably compromising the overall battery performance.…”

Section: Introductionmentioning

confidence: 99%

Removal and Reoccurrence of LLZTO Surface Contaminants under Glovebox Conditions

Siniscalchi,

Gibson,

Tufnail

et al. 2024

ACS Appl. Mater. Interfaces

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The reactivity of Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) solid electrolytes to form lithio-phobic species such as Li 2 CO 3 on their surface when exposed to trace amounts of H 2 O and CO 2 limits the progress of LLZTO-based solid-state batteries. Various treatments, such as annealing LLZTO within a glovebox or acid etching, aim at removing the surface contaminants, but a comprehensive understanding of the evolving LLZTO surface chemistry during and after these treatments is lacking. Here, glovebox-like H 2 O and CO 2 conditions were recreated in a near ambient pressure X-ray photoelectron spectroscopy chamber to analyze the LLZTO surface under realistic conditions. We find that annealing LLZTO at 600 °C in this atmosphere effectively removes the surface contaminants, but a significant level of contamination reappears upon cooling down. In contrast, HCl (aq) acid etching demonstrates superior Li 2 CO 3 removal and stable surface chemistry post treatment. To avoid air exposure during the acid treatment, an anhydrous HCl solution in diethyl ether was used directly within the glovebox. This novel acid etching strategy delivers the lowest lithium/LLZTO interfacial resistance and the highest critical current density.

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Section: Introductionmentioning

confidence: 99%

Removal and Reoccurrence of LLZTO Surface Contaminants under Glovebox Conditions

Siniscalchi,

Gibson,

Tufnail

et al. 2024

ACS Appl. Mater. Interfaces

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View full text Add to dashboard Cite

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Pyrite‐Based Solid‐State Batteries: Progresses, Challenges, and Perspectives

Bai,

Jiang,

Yin

et al. 2024

Adv Funct Materials

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Pyrite (FeS2), as a transition metal sulfide, has a promise application in the field of secondary batteries due to its abundant reserves, high theoretical capacity, safety, and non‐toxicity. However, serious volume expansion and shuttle effect of FeS2 in liquid secondary batteries limit its further development. Solid‐state batteries offer effective solutions to these challenges. In this review, the synthesis methods of FeS2 and recent progress in FeS2‐based solid‐state lithium/sodium batteries are presented, and the effects of FeS2 size and morphology, solid electrolyte type, and battery structure design on the electrochemical performance of solid‐state batteries are discussed. By analyzing and summarizing the problems in applying FeS2 in solid‐state batteries, the remaining challenges in this field are discussed and future directions are proposed. This review aims to guide research on high‐performance solid‐state batteries based on FeS2 and promote further development of FeS2 in electrochemical energy storage.

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Generalized Interphase Design for Stabilized Li/Inorganic Electrolyte Interfaces

Liu,

Li,

Dong

et al. 2024

Advanced Energy Materials

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All‐solid‐state Li metal batteries (ASSLMBs) using inorganic solid‐state electrolytes (ISEs) are considered promising energy storage technologies owing to their intrinsic safety and high energy density. Nevertheless, one critical challenge confronting ASSLMBs is the inability of the ISEs to prevent Li dendrite growth, which has not yet been fully addressed. Herein, general design principles of artificial solid electrolyte interphases (ASEI) for suppressing Li dendrites in ASSLMBs are proposed by systematically exploring the formation mechanism of Li dendrites. Subsequently, a tailored LiF‐Li3N ASEI is constructed to inspect the Li‐dendrite‐free design principles. The LiF‐Li3N modified Li (LFN‐Li) can effectively inhibit the side reactions and suppress the growth of Li dendrites, thus boosting the critical current densities of Li10GeP2S12 (LGPS) to a record‐high value of 3.4 mA cm−2. Furthermore, the LFN‐Li/LGPS/LFN‐Li can cycle stably for over 5000 h at 0.2 mA cm−2. Crucially, the versatility of the designed ASEI is highlighted as it ensures outstanding long‐term stability in symmetric cells featuring oxide Li1.3Al0.3Ti1.7(PO)3 or halide Li2ZrCl6 ISEs. As a result, the ASEI enables LiNi0.8Mn0.1Co0.1O2/LGPS/LFN‐Li and FeS2/LGPS/LFN‐Li cells to achieve high discharge‐specific capacities and desirable cyclic stability at room temperature. The generalized ASEI design principles rationalize the development of high‐energy ASSLBMs.

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Initiation of dendritic failure of LLZTO via sub-surface lithium deposition

Abstract: Mg is used as the tracer element in the Li plating electrode to confirm that pure Li metal can plate in isolated pores near the solid electrolyte surface. This results in an internal pressure buildup and in the spallation of the LLZTO solid electrolyte, initiating the dendritic process.

Cited by 5 publications

References 46 publications

Removal and Reoccurrence of LLZTO Surface Contaminants under Glovebox Conditions

Removal and Reoccurrence of LLZTO Surface Contaminants under Glovebox Conditions

Pyrite‐Based Solid‐State Batteries: Progresses, Challenges, and Perspectives

Generalized Interphase Design for Stabilized Li/Inorganic Electrolyte Interfaces

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