Ultra-High Energy-Density/Nonflammable Lithium Metal Full Cells Based on Coordinated Carbonate Electrolytes

Cho, Sung‐Ju; Yu, Dae-Eun; Pollard, Travis P.; Jang, Moongyu; Borodin, Oleg; Lee, Sang Young

doi:10.2139/ssrn.3405545

Cited by 7 publications

(10 citation statements)

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“…Improvements in the capacity retention of LMBs have been attributed to both decreasing the extent of SEI formation and to the formation of more dense Li deposits, the latter decreasing the dead Li and SEI formation. 4 , 12 − 14 Dead Li formation is thought to be caused by faster stripping of Li at sites with relatively low impedance, e.g., on fresh Li deposits with relatively thin SEI or where the SEI has ruptured. 15 , 16 Thus, electrolytes that result in fast SEI formation kinetics and ensure full and homogeneous SEI coverage on the Li metal surface, leading to more uniform plating, should stabilize these capacity losses in LMBs.…”

Section: Introductionmentioning

confidence: 99%

Noninvasive In Situ NMR Study of “Dead Lithium” Formation and Lithium Corrosion in Full-Cell Lithium Metal Batteries

et al. 2020

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Capacity retention in lithium metal batteries needs to be improved if they are to be commercially viable, the low cycling stability and Li corrosion during storage of lithium metal batteries being even more problematic when there is no excess lithium in the cell. Herein, we develop in situ NMR metrology to study “anode-free” lithium metal batteries where lithium is plated directly onto a bare copper current collector from a LiFePO4 cathode. The methodology allows inactive or “dead lithium” formation during plating and stripping of lithium in a full-cell lithium metal battery to be tracked: dead lithium and SEI formation can be quantified by NMR and their relative rates of formation are here compared in carbonate and ether-electrolytes. Little-to-no dead Li was observed when FEC is used as an additive. The bulk magnetic susceptibility effects arising from the paramagnetic lithium metal were used to distinguish between different surface coverages of lithium deposits. The amount of lithium metal was monitored during rest periods, and lithium metal dissolution (corrosion) was observed in all electrolytes, even during the periods when the battery is not in use, i.e., when no current is flowing, demonstrating that dissolution of lithium remains a critical issue for lithium metal batteries. The high rate of corrosion is attributed to SEI formation on both lithium metal and copper (and Cu+, Cu2+ reduction). Strategies to mitigate the corrosion are explored, the work demonstrating that both polymer coatings and the modification of the copper surface chemistry help to stabilize the lithium metal surface.

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Section: Introductionmentioning

confidence: 99%

Noninvasive In Situ NMR Study of “Dead Lithium” Formation and Lithium Corrosion in Full-Cell Lithium Metal Batteries

et al. 2020

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“…11 In recent years, high-concentration electrolytes have been shown to be able to stabilize Li-metal anode and cathodes by reducing the amount of free solvent and manipulating the interphase composition. [12][13][14] However, these high concentration electrolytes sacrifice cost, viscosity, wetting, and low-temperature operation. Localized high-concentration electrolytes (LHCE) were developed by diluting electrolytes with different non-solvating solvents, which presented more balanced properties.…”

Section: Introductionmentioning

confidence: 99%

Liquefied gas electrolytes for wide-temperature lithium metal batteries

Yang

Yin

Davies

et al. 2020

Energy Environ. Sci.

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139

118

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“…The electrochemical stability of the fs‐QSSE membrane was examined using linear sweep voltammetry analysis (Figure S7). The fs‐QSSE membrane showed good oxidation/reduction stability due to the coordinated Li + ‐FSI − solvent clusters 31 in the 4 M LiFSI‐PC/FEC electrolyte. Moreover, the ionic conductivity of the fs‐QSSE membrane was estimated in the temperature range of 25−80°C using electrochemical impedance spectroscopy (EIS) (Figure 1F).…”

Section: Resultsmentioning

confidence: 99%

“…The thermal stability of the fs-QSSE membrane was attributed to the nonflammable characteristic 31 of the coordinated electrolyte (4 M LiFSI in PC/FEC).…”

Section: Fabrication and Characterization Of The Fs-qsslmbsmentioning

confidence: 99%

Fibrous skeleton‐framed, flexible high‐energy‐density quasi‐solid‐state lithium metal batteries

et al. 2022

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Despite the extensive investigation on solid‐state lithium‐metal batteries (SSLMBs), their application in flexible electronic devices has been plagued mainly by the physicochemical/mechanical instability of their electrode–electrolyte interfaces. Here, we present a fibrous skeleton‐framed, quasi‐solid‐state LMB (fs‐QSSLMB) as a new cell architecture concept to simultaneously achieve the high‐energy‐density, mechanical flexibility, and safety. The fs‐QSSLMB is fabricated by embedding poly(ethylene terephthalate) (PET) nonwovens, stainless‐steel meshes, and metal‐coated conductive PET nonwovens with a lithiophilic‐gradient morphology as customized fibrous skeletons into quasi‐solid‐state electrolytes (QSSEs), high‐capacity LiNi0.8Co0.1Mn0.1O2 (NCM811) cathodes, and Li metal anodes, respectively. The stepwise printing of the NCM811 cathode/QSSE/Li anode assembly and the subsequent one‐pot ultraviolet curing of the gel electrolyte precursors in the assembly enable the formation of seamless interfaces between the electrodes and QSSE, thereby ensuring the electrochemical sustainability and mechanical deformability of the fs‐QSSLMB. In addition, owing to its fibrous skeleton‐based structural uniqueness and seamless interfaces, the fs‐QSSLMB exhibits electrochemical reliability, mechanical flexibility, safety (i.e., electrochemically active after being vertically cut in half and exposed to flame), and high (cell‐based) gravimetric/volumetric energy densities (385 Wh kgcell−1/451 Wh Lcell−1).

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Ultra-High Energy-Density/Nonflammable Lithium Metal Full Cells Based on Coordinated Carbonate Electrolytes

Cited by 7 publications

References 0 publications

Noninvasive In Situ NMR Study of “Dead Lithium” Formation and Lithium Corrosion in Full-Cell Lithium Metal Batteries

Noninvasive In Situ NMR Study of “Dead Lithium” Formation and Lithium Corrosion in Full-Cell Lithium Metal Batteries

Liquefied gas electrolytes for wide-temperature lithium metal batteries

Fibrous skeleton‐framed, flexible high‐energy‐density quasi‐solid‐state lithium metal batteries

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