New insights into Li distribution in the superionic argyrodite Li<sub>6</sub>PS<sub>5</sub>Cl

Zhao, Enyue; He, Lunhua; Zhang, Zhigang; Doux, Jean-Marie; Tan, Darren H. S.; Wu, Erik A.; Deysher, Grayson; Chen, Yuting; Zhao, Jinkui; Wang, Fangwei; Meng, Ying Shirley

doi:10.1039/d1cc03083c

Cited by 14 publications

(19 citation statements)

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“…[335] The argyrodite family is among the superionic Li-ion conductors, and key SEs for SSBs. [336,337] The Zeier group continuously investigates the new mechanism, synthesis process, site order and disorder for argyrodite type SSEs for HV-SSBs applications. [287,294,328,338,339] Wang et al recently reported the structure and lithium-ion mechanism of argyrodite type Li 6-x PS 5-x Br 1+x with increasing Br − /S 2− sites.…”

Section: Ssesmentioning

confidence: 99%

Perspectives on Improving the Safety and Sustainability of High Voltage Lithium‐Ion Batteries Through the Electrolyte and Separator Region

Cavers

Molaiyan

Abdollahifar

et al. 2022

Advanced Energy Materials

105

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Lithium‐ion batteries (LIBs) are promising candidates within the context of the development of novel battery concepts with high energy densities. Batteries with high operating potentials or high voltage (HV) LIBs (>4.2 V vs Li+/Li) can provide high energy densities and are therefore attractive in high‐performance LIBs. However, a variety of challenges (including solid electrolyte interface (SEI), lithium plating, etc.) and related safety issues (such as gas formation or thermal runaway effects) must be solved for the practical, widespread application of HV‐LIBs. Most of these challenges arise in the region between the electrodes: the electrolyte region. This review provides an overview of recent development and progress on the electrolyte region, including liquid electrolytes, ionic liquids, gel polymer electrolytes, separators, and solid electrolytes for HV‐LIBs applications. A focus on improving the safety of these systems, with some perspectives on their relative cost and environmental impact, is given. Overall, the new information is encouraging for the development of HV‐LIBs, and this review serves as a guide for potential strategies to improve their safety, allowing the development of HV‐LIBs, including solid‐state batteries, to be accelerated to practical relevance.

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Section: Ssesmentioning

confidence: 99%

Perspectives on Improving the Safety and Sustainability of High Voltage Lithium‐Ion Batteries Through the Electrolyte and Separator Region

Cavers

Molaiyan

Abdollahifar

et al. 2022

Advanced Energy Materials

105

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“…1,4 It was proposed that the site disorder in the Li-argyrodite structures has a strong effect on their Liion diffusion properties. 24 Hence, this discrepancy in ionic conductivity can be explained by the varying Li-ion transport pathways resulting from the synthesis method.…”

mentioning

confidence: 99%

“…This is probably because of the lower site disorder between S 2− and Cl − in Li 6 PS 5 Br and Li 6 PS 5 I compared to Li 6 PS 5 Cl. 24 Hence, further characterization using techniques such as solid-state NMR must be performed to determine the mechanisms of Li conductivity in these materials. This could provide a new platform for a deep understanding of borohydride substitution behavior and even unique insight into halogen Li-argyrodites.…”

mentioning

confidence: 99%

“…However, we would point out that this conductivity in pure Li 6 PS 5 Cl is lower than some reported works. It is well-known that the ionic conductivity of Li 6 PS 5 Cl is closely related to the synthetic process as different preparation methods can result in changes to site-disorder between S 2– and Cl – . , It was proposed that the site disorder in the Li-argyrodite structures has a strong effect on their Li-ion diffusion properties . Hence, this discrepancy in ionic conductivity can be explained by the varying Li-ion transport pathways resulting from the synthesis method.…”

mentioning

confidence: 99%

“…Unfortunately, the ionic conductivities of Li 6 PS 5 Br 0.9 (BH 4 ) 0.1 and Li 6 PS 5 I 0.9 (BH 4 ) 0.1 were not satisfactory compared to that of Li 6 PS 5 Cl 0.9 (BH 4 ) 0.1 . This is probably because of the lower site disorder between S 2– and Cl – in Li 6 PS 5 Br and Li 6 PS 5 I compared to Li 6 PS 5 Cl . Hence, further characterization using techniques such as solid-state NMR must be performed to determine the mechanisms of Li conductivity in these materials.…”

mentioning

confidence: 99%

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Borohydride Substitution Effects of Li₆PS₅Cl Solid Electrolyte

Wang

Gao

et al. 2021

ACS Appl. Energy Mater.

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We report an electrochemically stable borohydride (BH 4 − )-substituted Liargyrodite solid electrolyte prepared by a mechanical ball-milling method. The crystal structure of BH 4 − -substituted argyrodite remains unchanged with x < 0.3 (Li 6 PS 5 Cl 1−x (BH 4 ) x ), whereas a complex phase (Li 2 S-P 2 S 5 -LiCl-LiBH 4 ) was obtained with x > 0.3. The highest ionic conductivity of 0.12 mS cm −1 at 25 °C was observed with x = 0.1 in Li 6 PS 5 Cl 1−x (BH 4 ) x , whereas there was virtually no change in the complex phase. The electrochemical window of Li 6 PS 5 Cl 0.9 (BH 4 ) 0.1 is between 1 and 4 V against lithium metal.

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Influence Mechanism of Interfacial Oxidation of Li₃YCl₆ Solid Electrolyte on Reduction Potential

Wang,

Yang,

et al. 2024

Chemistry A European J

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Halide‐based solid electrolytes are promising candidates for all solid‐state lithium‐ion batteries (ASSLBs) due to their high ionic conductivity, wide electrochemical window, and excellent chemical stability with cathode materials. However, when tested in practice, their intrinsic electrochemical stability windows do not well match the conditions for stable operation of ASSBs. Existing literature reports halide‐based ASSBs that still operate well outside the electrochemical stability window, while ASSBs that do not operate within the window are not well studied or the studies are based on the cathode material interface. In this study, we aim to elucidate the mechanism behind all‐solid‐state battery failure by investigating how the reduction potential of Li3YCl6 solid‐state electrolyte itself changes under overcharging conditions. Our findings demonstrate that in Li‐In|Li3YCl6|Li3YCl6‐C half‐cells during the first state of charge, Cl ions participate in charge compensation, resulting in a depletion of ligands. This phenomenon significantly affects the reduction potential of Y3+, causing it to be reduced to Y2Cl3 and ultimately to Y0 at conditions far exceeding its actual reduction potential. Furthermore, we analyze the interfacial impedance induced by this process and propose a novel perspective on battery failure.

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New insights into Li distribution in the superionic argyrodite Li₆PS₅Cl

Abstract: By using temperature-dependent neutron powder diffraction combined with maximum entropy method analysis, a previously unreported Li lattice site was discovered in the argyrodite Li6PS5Cl solid-state electrolyte. This new finding enables...

Cited by 14 publications

References 29 publications

Perspectives on Improving the Safety and Sustainability of High Voltage Lithium‐Ion Batteries Through the Electrolyte and Separator Region

Perspectives on Improving the Safety and Sustainability of High Voltage Lithium‐Ion Batteries Through the Electrolyte and Separator Region

Borohydride Substitution Effects of Li₆PS₅Cl Solid Electrolyte

Influence Mechanism of Interfacial Oxidation of Li₃YCl₆ Solid Electrolyte on Reduction Potential

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New insights into Li distribution in the superionic argyrodite Li6PS5Cl

Abstract: By using temperature-dependent neutron powder diffraction combined with maximum entropy method analysis, a previously unreported Li lattice site was discovered in the argyrodite Li6PS5Cl solid-state electrolyte. This new finding enables...

Cited by 14 publications

References 29 publications

Perspectives on Improving the Safety and Sustainability of High Voltage Lithium‐Ion Batteries Through the Electrolyte and Separator Region

Perspectives on Improving the Safety and Sustainability of High Voltage Lithium‐Ion Batteries Through the Electrolyte and Separator Region

Borohydride Substitution Effects of Li6PS5Cl Solid Electrolyte

Influence Mechanism of Interfacial Oxidation of Li3YCl6 Solid Electrolyte on Reduction Potential

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Product

Resources

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New insights into Li distribution in the superionic argyrodite Li₆PS₅Cl

Borohydride Substitution Effects of Li₆PS₅Cl Solid Electrolyte

Influence Mechanism of Interfacial Oxidation of Li₃YCl₆ Solid Electrolyte on Reduction Potential