Capturing the swelling of solid-electrolyte interphase in lithium metal batteries

Zhang, Zewen; Li, Yuzhang; Xu, Rong; Zhou, Weijiang; Li, Yanbin; Oyakhire, Solomon T.; Wu, Yecun; Xu, Jingdong; Wang, Hansen; Yu, Zhiao; Boyle, David T.; Huang, William; Ye, Yusheng; Chen, Hao; Wan, Jiayu; Bao, Zhenan; Chiu, Wah; Cui, Yi

doi:10.1126/science.abi8703

Cited by 214 publications

(194 citation statements)

References 38 publications

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“…Moreover, the existence of poly(CO 3 ) species indicates significant decomposition of solvents, leading to a less protective SEI on LMA. Although inorganic LiF emerges from anion decomposition, a large proportion of organic species tends to impair the mechanical stability of SEI 51 .…”

Section: Resultsmentioning

confidence: 99%

Tackling realistic Li+ flux for high-energy lithium metal batteries

Zhang

et al. 2022

Nat Commun

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Electrolyte engineering advances Li metal batteries (LMBs) with high Coulombic efficiency (CE) by constructing LiF-rich solid electrolyte interphase (SEI). However, the low conductivity of LiF disturbs Li+ diffusion across SEI, thus inducing Li+ transfer-driven dendritic deposition. In this work, we establish a mechanistic model to decipher how the SEI affects Li plating in high-fluorine electrolytes. The presented theory depicts a linear correlation between the capacity loss and current density to identify the slope k (determined by Li+ mobility of SEI components) as an indicator for describing the homogeneity of Li+ flux across SEI, while the intercept dictates the maximum CE that electrolytes can achieve. This model inspires the design of an efficient electrolyte that generates dual-halide SEI to homogenize Li+ distribution and Li deposition. The model-driven protocol offers a promising energetic analysis to evaluate the compatibility of electrolytes to Li anode, thus guiding the design of promising electrolytes for LMBs.

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Section: Resultsmentioning

confidence: 99%

Tackling realistic Li+ flux for high-energy lithium metal batteries

Zhang

et al. 2022

Nat Commun

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“…However, the practical application of Li anodes is limited by dendritic Li growth ( 3 , 4 ), leading to safety concerns and fast capacity fading of Li metal batteries (LMBs) ( 5 , 6 ). Among the efforts to inhibit the formation of Li dendrites, modification or rebuilding of the solid-electrolyte interphase (SEI) might be the most crucial ( 7 , 8 ) because the SEI, which is spontaneously derived from the reaction between chemically active Li metal and the electrolyte, is responsible for Li + transport and mechanical accommodation of rapid Li growth ( 9 , 10 ). Functional fluorinated electrolyte constituents—such as Li bis(trifluoromethanesulfonyl)imide (LiTFSI) ( 11 ), Li bis(fluorosulfonyl)imide ( 12 ), 1,2-difluorobenzene ( 13 ), and fluoroethylene carbonate ( 14 )—have been designed to perform interface engineering to regulate the nanostructure and chemical composition of the SEI.…”

mentioning

confidence: 99%

Self-assembled monolayers direct a LiF-rich interphase toward long-life lithium metal batteries

Liu

Yuan

Wang

et al. 2022

Science

425

287

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High–energy density lithium (Li) metal batteries (LMBs) are promising for energy storage applications but suffer from uncontrollable electrolyte degradation and the consequently formed unstable solid-electrolyte interphase (SEI). In this study, we designed self-assembled monolayers (SAMs) with high-density and long-range–ordered polar carboxyl groups linked to an aluminum oxide–coated separator to provide strong dipole moments, thus offering excess electrons to accelerate the degradation dynamics of carbon-fluorine bond cleavage in Li bis(trifluoromethanesulfonyl)imide. Hence, an SEI with enriched lithium fluoride (LiF) nanocrystals is generated, facilitating rapid Li + transfer and suppressing dendritic Li growth. In particular, the SAMs endow the full cells with substantially enhanced cyclability under high cathode loading, limited Li excess, and lean electrolyte conditions. As such, our work extends the long-established SAMs technology into a platform to control electrolyte degradation and SEI formation toward LMBs with ultralong life spans.

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“…[17,103] It could be used to prepare cross-section specimen or lamella of Li-electrolyte interface containing (frozen) liquid electrolyte for cryo-STEM, without rinsing and drying processes. Very recently, Zhang et al [104] has captured the swollen state of SEI with cryo-STEM by preserving the SEI in its native organic liquid electrolyte environment with the original thin film vitrification method. However, the presence of frozen liquid electrolyte would cause difficulty in distinguishing the SEI in TEM analysis, because the electrolyte, which contains Li salt(s) and solvent, has a similar contrast to the SEI under TEM.…”

Section: Elusive Chemistry and Structure Of Seimentioning

confidence: 99%

Promoting Mechanistic Understanding of Lithium Deposition and Solid‐Electrolyte Interphase (SEI) Formation Using Advanced Characterization and Simulation Methods: Recent Progress, Limitations, and Future Perspectives

Dong

Jie

et al. 2022

Advanced Energy Materials

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In recent years, due to its great promise in boosting the energy density of lithium batteries for future energy storage, research on the Li metal anode, as an alternative to the graphite anode in Li‐ion batteries, has gained significant momentum. However, the practical use of Li metal anodes has been plagued by unstable Li (re)deposition and poor cyclability. Although tremendous efforts have been devoted to the stabilization of Li metal anodes, the mechanisms of electrochemical (re‐)deposition/dissolution of Li and solid‐electrolyte‐interphase (SEI) formation remain elusive. This article highlights the recent mechanistic understandings and observations of Li deposition/dissolution and SEI formation achieved from advanced characterization techniques and simulation methods, and discusses major limitations and open questions in these processes. In particular, the authors provide their perspectives on advanced and emerging/potential methods for obtaining new insights into these questions. In addition, they give an outlook into cutting‐edge interdisciplinary research topics for Li metal anodes. It pushes beyond the current knowledge and is expected to accelerate development toward a more in‐depth and comprehensive understanding, in order to guide future research on Li metal anodes toward practical application.

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Capturing the swelling of solid-electrolyte interphase in lithium metal batteries

Cited by 214 publications

References 38 publications

Tackling realistic Li+ flux for high-energy lithium metal batteries

Tackling realistic Li+ flux for high-energy lithium metal batteries

Self-assembled monolayers direct a LiF-rich interphase toward long-life lithium metal batteries

Promoting Mechanistic Understanding of Lithium Deposition and Solid‐Electrolyte Interphase (SEI) Formation Using Advanced Characterization and Simulation Methods: Recent Progress, Limitations, and Future Perspectives

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