Resolving Nanoscopic and Mesoscopic Heterogeneity of Fluorinated Species in Battery Solid-Electrolyte Interphases by Cryogenic Electron Microscopy

Huang, William; Wang, Hansen; Boyle, David T.; Li, Yuzhang; Cui, Yi

doi:10.1021/acsenergylett.0c00194

Cited by 232 publications

(230 citation statements)

References 59 publications

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“…However, we refrain from drawing in‐depth insights from the depth‐profile feature of XPS because it does not completely capture in‐plane heterogeneities, especially when sensitive materials are analyzed. [ 48 ]…”

Section: Resultsmentioning

confidence: 99%

“…However, we refrain from drawing in-depth insights from the depthprofile feature of XPS because it does not completely capture in-plane heterogeneities, especially when sensitive materials are analyzed. [48] To further verify the chemical role of TiO 2 , we perform SEM-EDS mapping of 0.6 mAh cm −2 of Li plated on a 5 nm TiO 2 -modified cell. SEM-EDS affords us the ability to visualize the surface of the plated Li, as well as the Cu foil regions that remain exposed after plating.…”

Section: Chemical Role Of Tiomentioning

confidence: 99%

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Revealing and Elucidating ALD‐Derived Control of Lithium Plating Microstructure

Oyakhire

Huang

Wang

et al. 2020

Advanced Energy Materials

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The practical implementation of Li metal batteries is hindered by difficulties in controlling the Li metal plating microstructure. While previous atomic layer deposition (ALD) studies have focused on directly coating Li metal with thin films for the passivation of the electrode–electrolyte interface, a different approach is adopted, situating the ALD film beneath Li metal and directly on the copper current collector. A mechanistic explanation for this simple strategy of controlling the Li metal plating microstructure using TiO2 grown on copper foil by ALD is presented. In contrast to previous studies where ALD‐grown layers act as artificial interphases, this TiO2 layer resides at the copper–Li metal interface, acting as a nucleation layer to improve the Li metal plating morphology. Upon lithiation of TiO2, a LixTiO2 complex forms; this alloy provides a lithiophilic surface layer that enables uniform and reversible Li plating. The reversibility of lithium deposition is evident from the champion cell (5 nm TiO2), which displays an average Coulombic efficiency (CE) of 96% after 150 cycles at a moderate current density of 1 mA cm−2. This simple approach provides the first account of the mechanism of ALD‐derived Li nucleation control and suggests new possibilities for future ALD‐synthesized nucleation layers.

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Section: Resultsmentioning

confidence: 99%

Section: Chemical Role Of Tiomentioning

confidence: 99%

Revealing and Elucidating ALD‐Derived Control of Lithium Plating Microstructure

Oyakhire

Huang

Wang

et al. 2020

Advanced Energy Materials

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“…More recently, Huang et al revealed a new model for SEI formed in carbonate electrolyte with FEC additives. [57] As shown in Figure 4d, LiF which is always considered to be a key component within the inner inorganic SEI, passivating the anode, is instead found to precipitate outside of the compact SEI, in an "indirect SEI." Li 2 O dominates the inorganic components within the compact SEI.…”

Section: Structural Modelsmentioning

confidence: 99%

“…More recently, Huang and co-workers mapped the spatial distribution of SEI components across the surface of metallic Li anode using cryo-STEM. [57] It was surprisingly found that LiF, an SEI component widely believed to play an important role in Li metal passivation, is absent within the compact SEI film (≈15 nm, Figure 7g); instead, LiF particles (100-400 nm) with a Li 2 O-rich outer layer precipitate (Figure 7h) across the anode surface in the carbonate electrolyte of 1.0 m LiPF 6 or LiClO 4 in EC/DEC with 10% FEC (Figure 7i). These observations refined the traditional SEI structure and indicated that LiF might neither play a dominant role in the passivation of Li metal, nor influence the transport of Li + through the SEI.…”

Section: Atomic Structurementioning

confidence: 99%

Interface Engineering for Lithium Metal Anodes in Liquid Electrolyte

Zhai

Liu

et al. 2020

Advanced Energy Materials

297

194

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Interfacial chemistry between lithium metal anodes and electrolytes plays a vital role in regulating the Li plating/stripping behavior and improving the cycling performance of Li metal batteries. Constructing a stable solid electrolyte interphase (SEI) on Li metal anodes is now understood to be a requirement for progress in achieving feasible Li‐metal batteries. Recently, the application of novel analytical tools has led to a clearer understanding of composition and the fine structure of the SEI. This further promoted the development of interface engineering for stable Li metal anodes. In this review, the SEI formation mechanism, conceptual models, and the nature of the SEI are briefly summarized. Recent progress in probing the atomic structure of the SEI and elucidating the fundamental effect of interfacial stability on battery performance are emphasized. Multiple factors including current density, mechanical strength, operating temperature, and structure/composition homogeneity that affect the interfacial properties are comprehensively discussed. Moreover, strategies for designing stable Li‐metal/electrolyte interfaces are also reviewed. Finally, new insights and future directions associated with Li‐metal anode interfaces are proposed to inspire more revolutionary solutions toward commercialization of Li metal batteries.

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“…Recently, Huang used Cryo-STEM to study the spatial distribution of SEI components such as LiF and Li 2 O in the SEI of the Li metal anode. Cryo-STEM EELS confirmed that the dense SEI connected with the negative electrode material does not contain LiF (William et al, 2020).…”

Section: Original Structure Of Interfacial Films Characterized By Crymentioning

confidence: 91%

Regulating the Performance of Lithium-Ion Battery Focus on the Electrode-Electrolyte Interface

Zhao

2020

Front. Chem.

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The development of lithium-ion battery (LIB) has gone through nearly 40 year of research. The solid electrolyte interface film in LIBs is one of most vital research topics, its behavior affects the cycle life and safety of LIBs significantly. Progress in understanding the interfacial layer on the negative and positive electrodes in LIBs has been the focus of considerable research in the past few decades, but there remains a number of problem to be understood at the fundamental level, and there is still a great deal of controversy regarding the composition and formation mechanism of the interfacial film. In this article, we summarize recent research conducted on the interfacial film in LIBs, including the film formation mechanism, the composition, and stability of the interfacial film on the positive electrodes (in both diluted and high-concentration electrolytes). And the methodologies and advanced techniques implemented for the characterization of the interfacial film. Finally, we put forward some of the future development direction for the interfacial film and urgent problems that need to be solved.

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Resolving Nanoscopic and Mesoscopic Heterogeneity of Fluorinated Species in Battery Solid-Electrolyte Interphases by Cryogenic Electron Microscopy

Cited by 232 publications

References 59 publications

Revealing and Elucidating ALD‐Derived Control of Lithium Plating Microstructure

Revealing and Elucidating ALD‐Derived Control of Lithium Plating Microstructure

Interface Engineering for Lithium Metal Anodes in Liquid Electrolyte

Regulating the Performance of Lithium-Ion Battery Focus on the Electrode-Electrolyte Interface

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