<i>In situ</i> observation of lithium metal plating in a sulfur-based solid electrolyte for all-solid-state batteries

Kim, Seong Heon; Kim, KiHong; Choi, Hyung Kook; Im, Dongmin; Heo, Sung; Choi, Hong Soo

doi:10.1039/c9ta02614b

Cited by 51 publications

(41 citation statements)

References 41 publications

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“…For sulfide-based SSEs, any high temperature treatment would promote unwanted reactions and form a thick solid electrolyte interface (SEI) that renders cells unusable. While some studies demonstrated good lithium-SSE contact by simple cold pressing 21,22 , the effectiveness of this methodology in lowering interfacial resistance and allowing uniform lithium plating especially in long term cell cycling is still unclear. Another solution could be the use of a thin Li + conductive polymer layer between the lithium anode and the SSE.…”

Section: Anode Interfacial Reactionsmentioning

confidence: 99%

From nanoscale interface characterization to sustainable energy storage using all-solid-state batteries

et al. 2020

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Section: Anode Interfacial Reactionsmentioning

confidence: 99%

From nanoscale interface characterization to sustainable energy storage using all-solid-state batteries

et al. 2020

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“…23 However, the morphological aspects of lithium-metal plating directly underneath current collectors on bulk-type SEs has yet only been investigated by Nagao et al on the glass ceramic Li 2 S-P 2 S 5 , who showed that homogeneous lithium plating is only possible at very low current densities (10 mA$cm À2 ), 44 and very recently by Kim et al on the argyrodite SE Li 6 PS 5 Cl, who highlighted the high impact of mechanical aspects for lithium plating. 45 Because of low or negligible interfacial reactivity with lithium-metal, garnet-type SEs are promising model systems for further investigations. 46 Lithium-metal-plating experiments on garnets using copper current-collector thin films are already reported on porous garnet host structures 47,48 and were analyzed on dense pellets by neutron-depth profiling.…”

Section: Context and Scalementioning

confidence: 99%

Lithium-Metal Growth Kinetics on LLZO Garnet-Type Solid Electrolytes

Krauskopf

Dippel

Hartmann

et al. 2019

Joule

352

391

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Li 7 La 3 Zr 2 O 12 (LLZO)-based garnet materials are recently being investigated as suitable electrolytes for solid-state batteries with lithium-metal electrodes. Unfortunately, lithium-metal penetration through polycrystalline garnet-type electrolytes limits the electric current density during cell charging. In this study, we introduce an electrochemical operando approach that is well suited to get insights into the early stage of lithium-metal penetration that was yet only accessible with very elaborate neutron measurements. Combined with in situ as well as ex situ electron microscopic techniques, we investigate the morphological instability of the lithium-metal anode on garnet-type solid electrolytes under cathodic load and demonstrate the inter-relationship between microkinetic aspects and lithium-penetration susceptibility.

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“…Meanwhile, in situ SEM has also been used to show magnified, high-resolved, and three-dimensional Li dendrite evolution with the accurate distinction of growth form and elements under electrochemical reactions. [241][242][243] The liquid cell used for the in situ electrochemical (EC)-SEM operation was initially assembled using a top silicon chip with a silicon nitride (SiN x ) membrane and bottom quartz chip with two injection orifices, followed by a sealing step using epoxy and liquid electrolyte injection (Figure 15c). [241] Then, the growth and dissolution mechanism were observed through an electron beam penetrating into the SiN x window when the electrochemical experiment was continuously carried out under LiTFSI in 1,3-dioxolane (DOL) and 1,2-dimethoxyethane (DME) electrolyte with a Li nitrate (LiNO 3 ) additive.…”

Section: In Situ Macroscopic Observationsmentioning

confidence: 99%

“…Beyond liquid cell operation in conjunction with electron microscopy, in situ Auger electron microscopy (AEM)/Auger electron spectroscopy (AES), an SEM analysis technique, has also been used to investigate AASBs, as shown in Figure 15e. [243] Real-time monitoring of Li metal and SSEs in AASBs, including sulfur-based Li 6 PS 5 Cl (LiPS) SSEs, was carried out to confirm Li-metal growth mechanism, volume expansion/contraction, and correlation with SSEs. The SEM images in Figure 15f show the Li dendrite morphology during the 2 nd cycle, where the Li metal protruded while extruding the SSEs after the charging process.…”

Section: In Situ Macroscopic Observationsmentioning

confidence: 99%

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Lithium Metal Interface Modification for High‐Energy Batteries: Approaches and Characterization

Lee

Song

Cho

et al. 2020

Batteries & Supercaps

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Rechargeable batteries have been a profoundly greater part of our lives than we could have ever imagined. The rechargeable Li‐ion batteries (LIBs) that have been developed for transport systems even put fossil fuels in the corner. However, state‐of‐the‐art Li‐ion batteries with graphite anodes are now approaching their theoretical specific energy limits, so they cannot meet the increasing demands of a range of portable electronics and large‐scale energy storage systems. Li metal is one of the most promising anode materials that could break through the energy density bottleneck of Li‐ion batteries due to its ultrahigh specific capacity and very low potential compared to other anode materials. Nonetheless, the direct use of Li metal in commercial battery systems has been hindered due to significant obstacles associated with it such as safety issues, corrosion from chemical reactions that occur inside the battery, or poor cycling performance. The fundamental reason for these problems is the dendritic growth of Li‐ions on the Li metal anode during cycling, as a result of the interfacial phenomena of Li metal and electrolytes. Modification of the Li metal interface with an electrolyte presents an efficient solution to solve these problems. In this review, the current challenges facing the development of Li metal anodes are presented in detail. The most recent advances in Li metal anodes using a controlled interface between the Li metal surface and an electrolyte are highlighted and an introduction on the synthesis and production methods for the application of high‐energy‐density battery systems such as Li‐oxygen (Li−O2), Li‐sulfur (Li−S), and Li metal batteries with high‐energy density cathodes is presented. Furthermore, the recent developments in the in situ/operando analysis tools adopted for the investigation of Li metal anodes such as the structural and chemical changes, dynamic properties, and solid–electrolyte interface (SEI) layer properties are described and summarized. Finally, some suggestions are given in the direction of the development of Li metal with artificial surface layers for use in future high‐energy batteries.

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In situ observation of lithium metal plating in a sulfur-based solid electrolyte for all-solid-state batteries

Abstract: The in situ AES/AEM technique for practical all-solid-state batteries with sulfur-based solid electrolytes was developed and the real time observation of Li dendrite growth was successfully achieved.

Cited by 51 publications

References 41 publications

From nanoscale interface characterization to sustainable energy storage using all-solid-state batteries

From nanoscale interface characterization to sustainable energy storage using all-solid-state batteries

Lithium-Metal Growth Kinetics on LLZO Garnet-Type Solid Electrolytes

Lithium Metal Interface Modification for High‐Energy Batteries: Approaches and Characterization

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