Liquid‐Phase Electrochemical Scanning Electron Microscopy for In Situ Investigation of Lithium Dendrite Growth and Dissolution

Rong, Genlan; Zhang, Xinyi; Zhao, Wen; Qiu, Yongcai; Liu, Meinan; Ye, Fangmin; Xu, Yan; Chen, Jiafan; Hou, Yuanjun; Li, Wanfei; Duan, Wenhui; Zhang, Yuegang

doi:10.1002/adma.201606187

Cited by 153 publications

(98 citation statements)

References 38 publications

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“…SEM has been the most widely used technique to analyze the surface modification of Li metal since 1970s because its resolution is as high as 1 nm and the size of battery for in operando tests is close to a normal battery. The SEM comprises of an electron source, a signal detector, lenses, a vacuum system and an observation platform that needs a visual battery structure and a thin film window (such as SiN x membrane mm in diameter and tens of nm in thickness) transparent to electron beams, as illustrated in Figure a . Recently, by using even thinner window materials such as 2D materials, it was possible to perform in situ liquid SEM without a vacuum sample chamber (airSEM), with only 2% drop in contrast …”

Section: Dynamic Characterizations Of Lithium Metal Anodementioning

confidence: 99%

Section: Dynamic Characterizations Of Lithium Metal Anodementioning

confidence: 99%

“…It is found that the nucleation sites of Li metal was at solid/solid interfaces, and therefore the nuclei has to fight for space by pushing either electrode or electrolyte away . Recently, the lithium deposition/dissolution behaviors in liquid electrolytes was systematically studied by Rong through an “in situ electrochemical scanning electronic microscopy (EC‐SEM)” (Figure b), who demonstrated that the additives in the electrolytes greatly affected the LMI growth rate and mechanisms. Specifically, a coaddition of both lithium nitrate and lithium polysulfide in the ether‐based electrolyte remarkably minimized LMI growth.…”

Section: Dynamic Characterizations Of Lithium Metal Anodementioning

confidence: 99%

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Developing High‐Performance Lithium Metal Anode in Liquid Electrolytes: Challenges and Progress

et al. 2018

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Lithium metal anodes are potentially key for next-generation energy-dense batteries because of the extremely high capacity and the ultralow redox potential. However, notorious safety concerns of Li metal in liquid electrolytes have significantly retarded its commercialization: on one hand, lithium metal morphological instabilities (LMI) can cause cell shorting and even explosion; on the other hand, breaking of the grown Li arms induces the so-called "dead Li"; furthermore, the continuous consumption of the liquid electrolyte and cycleable lithium also shortens cell life. The research community has been seeking new strategies to protect Li metal anodes and significant progress has been made in the last decade. Here, an overview of the fundamental understandings of solid electrolyte interphase (SEI) formation, conceptual models, and advanced real-time characterizations of LMI are presented. Instructed by the conceptual models, strategies including increasing the donatable fluorine concentration (DFC) in liquid to enrich LiF component in SEI, increasing salt concentration (ionic strength) and sacrificial electrolyte additives, building artificial SEI to boost self-healing of natural SEI, and 3D electrode frameworks to reduce current density and delay Sand's extinction are summarized. Practical challenges in competing with graphite and silicon anodes are outlined.

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Section: Dynamic Characterizations Of Lithium Metal Anodementioning

confidence: 99%

Section: Dynamic Characterizations Of Lithium Metal Anodementioning

confidence: 99%

Section: Dynamic Characterizations Of Lithium Metal Anodementioning

confidence: 99%

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Developing High‐Performance Lithium Metal Anode in Liquid Electrolytes: Challenges and Progress

et al. 2018

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“…For example, lithium metal tends to grow a dendritic structure upon fast charging. In addition, the continuous reaction between lithium dendrite and the organic electrolyte leads to increase in impedance and results in poor Coulombic efficiency . As a consequence, excess lithium metal is usually needed for lithium metal batteries.…”

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confidence: 99%

Lithium Silicide Surface Enrichment: A Solution to Lithium Metal Battery

et al. 2018

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The propensity of lithium dendrite formation during the charging process of lithium metal batteries is linked to inhomogeneity on the lithium surface layer. The high reactivity of lithium and the complex surface structure of the native layer create "hot spots" for fast dendritic growth. Here, it is demonstrated that a fundamental restructuring of the lithium surface in the form of lithium silicide (Li Si) can effectively eliminate the surface inhomogeneity on the lithium surface. In situ optical microscopic study is carried out to monitor the electrochemical deposition of lithium on the Li Si-modified lithium electrodes and the bare lithium electrode. It is observed that a much more uniform lithium dissolution/deposition on the Li Si-modified lithium anode can be achieved as compared to the bare lithium electrode. Full cells paring the modified lithium anode with sulfur and LiFePO cathodes show excellent electrochemical performances in terms of rate capability and cycle stability. Compatibility of the anode enrichment method with mass production process also offers a practical way for enabling lithium metal anode for next-generation lithium batteries.

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“…

hydrogen electrode). [7,8] The most critical issue is that deposition of lithium metal tends to be highly dendritic during the repeated plating and dissolution process, which not only continue to consume the electrolyte and induce the "dead lithium" leading to capacity fading, but also face the severe safety problems of short-circuit due to the crack of separator by continuous ramified growth of lithium dendrites. However, the further application of LMB is plagued with practical issues that puzzled researchers for more than 40 years.

…”

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confidence: 99%

S‐Doped Graphene‐Regional Nucleation Mechanism for Dendrite‐Free Lithium Metal Anodes

Wang

Zhai

Legut

et al. 2019

Advanced Energy Materials

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hydrogen electrode). [5,6] In fact, lithium metal has been applied in space exploration, petroleum prospecting in 1970s. However, the further application of LMB is plagued with practical issues that puzzled researchers for more than 40 years. [7,8] The most critical issue is that deposition of lithium metal tends to be highly dendritic during the repeated plating and dissolution process, which not only continue to consume the electrolyte and induce the "dead lithium" leading to capacity fading, but also face the severe safety problems of short-circuit due to the crack of separator by continuous ramified growth of lithium dendrites. [9,10] During the past half-century, many up-and-coming methods have been carried out to suppress dendrite growth and achieved partially success. These strategies can be broadly divided into three areas: i) electrolyte modification (such as selfhealing electrostatic shield mechanism by inducing Cs + , [11] replacing traditional liquid electrolyte by solid state electrolyte [12] ), ii) artificial solidelectrolyte interphase (SEI) (such as manufacturing the Li 3 N, [13] LiF, [14] Li-Sn alloy [15] layers to improve the mechanical strength, ionic diffusion performance, and stability to suppress the dendrite); iii) the multifunctional nanostructured anodes design to manipulate the nucleation of lithium (such as Ni foam, [16] 3D skeleton Cu matrix, [17] Cu-Zn alloy matrix [18] ). The former two strategies are based primarily on suppressing the protrusions, while the last one mainly focuses on modulating the initial nucleation process of dendrite, before the extension of dendrites into the electrolyte. Designing the excellent LMB requires the joint effort of these methods. However, if we can eliminate or mitigate the lithium dendrite from the initial nucleation process, it will be a highly efficient and convenient measure for its industrial production. Thus, finding an ideal nucleating anode material is very important to solve the dendrite problem.Based on Chazalviel's theory, [19,20] designing high-surface area anode can suppress the local current density and thus improve the electrical performance. Graphene, who possesses very high specific surface area, shows great advantage on its potential application in lithium metal anode field. [21][22][23] However, the pristine graphene (PG) shows poor performances in the actual application. [24][25][26] Doping or modulating the graphene can adjust its performance which has already made some Lithium metal is the most promising anode material for next-generation batteries, owing to its high theoretical specific capacity and low electrochemical potential. However, the practical application of lithium metal batteries (LMBs) has been plagued by the issues of uncontrollable lithium deposition. The multifunctional nanostructured anode can modulate the initial nucleation process of lithium before the extension of dendrites. By combing the theoretical design and experimental validation, a novel nucleation strategy is developed by introducing sulfur (S) to gr...

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Liquid‐Phase Electrochemical Scanning Electron Microscopy for In Situ Investigation of Lithium Dendrite Growth and Dissolution

Cited by 153 publications

References 38 publications

Developing High‐Performance Lithium Metal Anode in Liquid Electrolytes: Challenges and Progress

Developing High‐Performance Lithium Metal Anode in Liquid Electrolytes: Challenges and Progress

Lithium Silicide Surface Enrichment: A Solution to Lithium Metal Battery

S‐Doped Graphene‐Regional Nucleation Mechanism for Dendrite‐Free Lithium Metal Anodes

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