Li metal deposition and stripping in a solid-state battery via Coble creep

Chen, Yuming; Wang, Ziqiang; Li, Xiaoyan; Yao, Xiahui; Wang, Chao; Li, Yutao; Xue, Weimin; Yu, Daiwei; Kim, So Yeon; Yang, Fu‐Mei; Kushima, Akihiro; Zhang, Guoge; Huang, Haitao; Wu, Nan; Wing, Yiu; Goodenough, John B.; Li, Ju

doi:10.1038/s41586-020-1972-y

Cited by 382 publications

(304 citation statements)

References 36 publications

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“…All‐solid‐state lithium batteries using an inorganic ceramic solid electrolyte (SE) with a Li metal anode have attracted great attention for their potential to significantly increase the energy density of next‐generation energy storage systems. [ 1–11 ] However, current Li metal anodes with SEs are limited to a low areal current density of less than 1 mA cm −2 and operate for only a small number of cycles, due to the cell failure of short circuiting and lithium dendrite penetration through the SE. [ 12–15 ] A key strategy to improve the performance of Li metal anode in solid‐state batteries is to engineer the Li–SE interface by pre‐treating the SE surfaces [ 9,19,20 ] and adding interfacial coating layers to achieve good interfacial contact and low interfacial resistance.…”

Section: Introductionmentioning

confidence: 99%

Interfacial Atomistic Mechanisms of Lithium Metal Stripping and Plating in Solid‐State Batteries

et al. 2021

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All‐solid‐state batteries based on a Li metal anode represent a promising next‐generation energy storage system, but are currently limited by low current density and short cycle life. Further research to improve the Li metal anode is impeded by the lack of understanding in its failure mechanisms at lithium–solid interfaces, in particular, the fundamental atomistic processes responsible for interface failure. Here, using large‐scale molecular dynamics simulations, the first atomistic modeling study of lithium stripping and plating on a solid electrolyte is performed by explicitly considering key fundamental atomistic processes and interface atomistic structures. In the simulations, the interface failure initiated with the formation of nano‐sized pores, and how interface structures, lithium diffusion, adhesion energy, and applied pressure affect interface failure during Li cycling are observed. By systematically varying the parameters of solid‐state lithium cells in the simulations, the parameter space of applied pressures and interfacial adhesion energies that inhibit interface failure during cycling are mapped to guide selection of solid‐state cells. This study establishes the atomistic modeling for Li stripping and plating, and predicts optimal solid interfaces and new strategies for the future research and development of solid‐state Li‐metal batteries.

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Section: Introductionmentioning

confidence: 99%

Interfacial Atomistic Mechanisms of Lithium Metal Stripping and Plating in Solid‐State Batteries

et al. 2021

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“…[ 21 ] However, Li dendrites still grow in SSEs even though the interface resistance is reduced. [ 22,23 ]…”

Section: Figurementioning

confidence: 99%

Solid‐State Electrolyte Design for Lithium Dendrite Suppression

et al. 2020

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More importantly, the high mechanical strength is expected to block the lithium dendrite penetration. [5] The unit transference number of Li-ions in SSEs should prevent concentration gradient-induced Li dendrite growth in SSEs. [6] However, extensive investigations demonstrated that Li dendrites still easily grow in inorganic SSEs, including Li 3 PS 4 (LPS), [7] and Li 7 La 3 Zr 2 O 12 (LLZO), [8] whatever they are in single crystal, [9] amorphous or multicrystal structures. The SSEs with much higher mechanical strength show even lower dendrite suppression capability than that in conventional organic electrolytes. [10] Both intergranularly [11] and intragranularly Li dendrite growth are found in SSEs. [12] However, the mechanism for Li dendrite growth in SSEs is not fully understood. Hypotheses, such as poor interfacial contact, electronic conductivity of bulk electrolytes, and the presence of the grain boundaries (GBs), are proposed to illustrate the counterintuitive dendrite growth in SSEs. [13] The high interfacial resistance and non-uniformity at Li/SSE interface, introducing by GBs, voids, and cracks, are often blamed to be responsible for the Li dendrite growth in SSEs. [13] However, reduction of the non-uniformity by densifying SSE, [14] amorphous SSE, and single crystal SSE [15] cannot block the Li dendrite growth. In addition, to reduce the interfacial resistance, lithiophilic Au, [16] Al 2 O 3 , [17] ZnO, [18] Ge, [19] and Li 3 N, [20] which bridges the energy gap between Li and SSE, were coated on SSEs and lithiophobic Li 2 CO 3 was removed from LLZO surface by polishing and heating. [21] However, Li dendrites still grow in SSEs even though the interface resistance is reduced. [22,23] In sharp contrast to lithiophilic coating and enhancement of the uniformity of SSEs, herein, we design a lithiophobic porous SSE that has a high interface energy against Li, a high ionic conductivity and low electronic conductivity to enhance the dendrite suppression capability. Based on the total energy analyses, we established dendrite suppression criterion: the electrolytes or formed interphases should: 1) be electrochemically stable with Li; 2) have a high ionic conductivity and a low electronic conductivity; and 3) have a high interface energy against Li to suppress Li nucleation and growth inside electrolytes. Li 3 N has a high ion conductivity and is stable with Li metal. However, All-solid-state Li metal batteries have attracted extensive attention due to their high safety and high energy density. However, Li dendrite growth in solid-state electrolytes (SSEs) still hinders their application. Current efforts mainly aim to reduce the interfacial resistance, neglecting the intrinsic dendrite-suppression capability of SSEs. Herein, the mechanism for the formation of Li dendrites is investigated, and Li-dendrite-free SSE criteria are reported. To achieve a high dendrite-suppression capability, SSEs should be thermodynamically stable with a high interface energy against Li, and they should have a low electronic conducti...

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“…The trapped interface charges during lithiation of LiCoO 2 , [ 16 ] Ge nanowire, [ 17 ] and Li 4 Ti 5 O 12 [ 18 ] were visualized, which revealed many detailed lithiation mechanisms. Chen et al [ 19 ] used in situ TEM to study the lithium metal deposition and stripping behavior within a large number of parallel hollow tubules made of a mixed ionic‐electronic conductor (MIEC), proposed that Coble creep happened along the MIEC/metal phase boundary, which can help to effectively relieve stress, maintain electronic and ionic contacts and eliminate solid‐electrolyte interphase debris. However, ion liquids and solid electrolyte are not common electrolytes used in commercial LIBs.…”

Section: Electron Microscopy Imaging Techniquementioning

confidence: 99%

Recent Progress on Advanced Imaging Techniques for Lithium‐Ion Batteries

Deng

Xing

Huang³

et al. 2020

Advanced Energy Materials

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Lithium‐ion batteries are the most commercially successful electrochemical devices, extensively used in intelligent electronics, electric vehicles, grid energy storages, etc. However, there still needs to be further improvement of their performance such as in energy density, cyclability, rate capability, and safety. To do so, it is necessary to understand the detailed structural evolution progress inside the battery. Many advanced imaging techniques have been developed to directly monitor the status and get some key information inside the battery. For advanced imaging techniques, superhigh resolution, fully informative function, nondestruction of the sample, and in situ observation are required. This review introduces and discusses some recent important progress on a variety of advanced imaging techniques for battery research. These imaging techniques have enabled the visualization of sub‐micrometer level chemical valence distribution, evolution of solid‐electrolyte interface, Li dendrite growth, and trace amount of gassing, etc., which greatly promote the development of rechargeable batteries. Of particular note, a new ultrasonic imaging technique has been recently developed to monitor gas generation, the electrolyte wetting process, and the state of charge in the battery. Finally, a perspective is given on some future developments in the imaging techniques for Li‐ion batteries and other rechargeable batteries.

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Li metal deposition and stripping in a solid-state battery via Coble creep

Cited by 382 publications

References 36 publications

Interfacial Atomistic Mechanisms of Lithium Metal Stripping and Plating in Solid‐State Batteries

Interfacial Atomistic Mechanisms of Lithium Metal Stripping and Plating in Solid‐State Batteries

Solid‐State Electrolyte Design for Lithium Dendrite Suppression

Recent Progress on Advanced Imaging Techniques for Lithium‐Ion Batteries

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