Predicting Calendar Aging in Lithium Metal Secondary Batteries: The Impacts of Solid Electrolyte Interphase Composition and Stability

Wood, Sean M.; Fang, Chengcheng; Dufek, Eric J.; Nagpure, Shrikant C.; Sazhin, Sergiy V.; Liaw, Bor Yann; Meng, Ying Shirley

doi:10.1002/aenm.201801427

Cited by 50 publications

(56 citation statements)

References 34 publications

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“…These resistive layers will hinder ion transport and increase cell overpotential, thus causing significant observed capacity fading at high current densities due to the reduced utilization of active material that occurs when voltage cutoffs are constant. [ 24 ] The consumption of electrolyte, including both salt and solvent, may affect the composition of SEI [ 25 ] and the conductivity of the electrolyte (Figure S2, Supporting Information), which may also change the impedance of the cell.…”

Section: Resultsmentioning

confidence: 99%

Fast Diagnosis of Failure Mechanisms and Lifetime Prediction of Li Metal Batteries

et al. 2020

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Wh kg −1 , and a life of 1000 cycles. [3] To meet these targets, large improvements in specific energy are critically needed. One promising route to increase the specific energy of batteries is to switch to Li metal anodes. Batteries with Li metal serving as the anode can deliver exceptionally high energy densities, [4] because of their advantages in having the lowest redox potential (−3.04 V vs standard hydrogen electrode) and a high theoretical specific capacity (3860 mAh g −1). Studies suggest that the energy density of batteries can be doubled or tripled relative to present technologies using Li metal anodes. [2] However, the practical applications of Li metal anodes are severely hindered by their rapid failure. This failure is primarily driven by parasitic reactions between Li metal and electrolyte. The common signatures of failure are the formation of dead/isolated Li, which is electrically disconnected from the bulk Li metal during uneven stripping on the anode surface, [5,6] the dendritic or mossy Li, which is induced by inhomogeneous distributions of space charge [7] on the anode surface which arise from uneven anode surfaces or cracks in the solid electrolyte interphase (SEI). [8] Rechargeable Li metal batteries (LMBs) cannot be deployed in automotive applications unless lifetime limitations are overcome. Numerous strategies have been explored to successfully extend the lifetime of LMBs. These include developing novel electrolytes that produce more stable SEI layers, creating artificial SEI layers on the Li metal surface, and applying external pressures. [9] While these and other methods provide pathways for improving the lifetime of batteries, none of them have succeeded in meeting industrial performance targets. In order to accelerate the development of viable LMB technologies, it is critically important to develop diagnostic techniques that can rapidly and easily identify the primary cause of battery failure and that can make useful predictions about the lifetime of a cell based on data collected early in its lifetime (instead of waiting long times for cells to reach their actual failure point before getting feedback). There are three commonly seen battery failure mechanisms for LMBs that reduce the capacity of a cell over its lifetime. [10] Lithium (Li) metal serving as an anode has the potential to double or triple stored energies in rechargeable Li batteries. However, they typically have short cycling lifetimes due to parasitic reactions between the Li metal and electrolyte. It is critically required to develop early fault-detection methods for different failure mechanisms and quick lifetime-prediction methods to ensure rapid development. Prior efforts to determine the dominant failure mechanisms have typically required destructive cell disassembly. In this study, non-destructive diagnostic method based on rest voltages and coulombic efficiency are used to easily distinguish the different failure mechanismsfrom loss of Li inventory, electrolyte depletion, and increased cell impedancewhich are deep...

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Section: Resultsmentioning

confidence: 99%

Fast Diagnosis of Failure Mechanisms and Lifetime Prediction of Li Metal Batteries

et al. 2020

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“…The thickness of PCNF mats was fixed at 40 µm and 60 µL of electrolyte [53] was added to each cell. The electrospun PCNFs were cut into round disks with a diameter of 16 mm, which were used as both the working electrode and the current collector for Li plating/stripping while 1 m lithium bis(trifluoromethanesulfonyl) imide (LiTFSI) dissolved in dioxolane (DOL)/ dimethoxyethane (DME) (1:1 by volume) with 1 wt% of LiNO 3 was used as the electrolyte.…”

Section: Methodsmentioning

confidence: 99%

“…The Li foil was replaced by a PCNF disk to function as the working electrode for the symmetric cell test. The thickness of PCNF mats was fixed at 40 µm and 60 µL of electrolyte was added to each cell. The EIS measurements were conducted on symmetric cells that were precycled for designated times at a frequency raging 0.1–10 5 Hz.…”

Section: Methodsmentioning

confidence: 99%

Correlation between Li Plating Behavior and Surface Characteristics of Carbon Matrix toward Stable Li Metal Anodes

Cui

Yao

Ihsan‐Ul‐Haq

et al. 2018

Advanced Energy Materials

118

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anodes. These new anodes promise an almost 100% increase in practical energy density compared to those of conventional LIB counterparts. [3][4][5][6][7][8][9] While developing cathodes for the next-generation batteries has made a significant progress, relatively fewer research efforts have thus far been devoted to Li metal anodes because of the formation of Li dendrites which is considered a critical drawback instigating devastating safety issues of batteries. [10] Along with recent studies on Li plating behaviors, there have been renewed interests in developing Li metal anodes. [11][12][13] In particular, the dendrite-free Li metal anode was made possible by rationally designing the electrolyte composition and electrode morphologies. [14,15] Nevertheless, the current Li metal anodes are far from being viable because of several reasons. Namely, (1) the dendritic Li emerges when the current density raises above the percolation value; (2) the Coulombic efficiencies (CEs) of Li metal anodes are too low to maintain good cyclic stability of batteries; and (3) the design of Li metal anodes is still inadequate, making it difficult to integrate into the existing LIB configurations, such as pouch and cylindrical cells. [12] Most of the strategies currently exercised for dendrite-free Li metal anodes usually fail to resolve all the above mentioned issues. For example, the all-solid-state Li-metal battery requires certain prestress to reduce the interfacial resistance between the solid-state electrolyte and the electrode, but such a prestress is difficult to apply on pouch cells. [16,17] The feasibility of artificial solid electrolyte interphase (SEI) protection on Li foil remains doubtful because the Li foil alone cannot be used as current collector in practical cells due to its hostless nature and huge volume changes during the repeated cycles. [11,18] Among all potential strategies, the incorporation of conductive substrates to function as both the Li host and current collector is considered an ideal approach for further development of practical Li metal anodes. [19] The growth of Li dendrites at high current densities was mitigated by means of reduced local current densities using conductive substrates. [12] Moreover, the conductive substrates also functioned as the current collector, which is compatible with the existing LIB configurations. While copper has been widely studied as the matrix material for hosting Li metal, carbon is considered a more promising candidate than copper Carbonaceous materials are widely employed to host Li for stable and safe Li metal batteries while relatively little effort is devoted to tailoring the surface properties of carbon to facilitate uniform Li plating. Herein, the correlation between Li plating behavior and the surface characteristics of electrospun porous carbon nanofibers (PCNFs) is systemically elucidated through experiments and theoretical calculations. It is revealed that the neat carbon surface suffers from severe lattice mismatch with Li metal, hindering uniform Li plating....

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“…Carbon‐ and silicon‐based anodes will not form SEI at open circuit, rather needing to be lithiated to below 1.0 V. In some Li metal systems the SEI is sufficiently unstable that its ongoing formation during storage has been reported to limit cell life. [ 14 ] In our view, how much of the previous understanding or modeling on carbon SEI can be directly applied to metal SEI remains an open question. Less stable interfaces and more severe side reactions of Na and K metal anodes have been reported.…”

Section: Introductionmentioning

confidence: 99%

Review of Emerging Concepts in SEI Analysis and Artificial SEI Membranes for Lithium, Sodium, and Potassium Metal Battery Anodes

Liu

Mitlin

2020

Advanced Energy Materials

376

250

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Lithium metal batteries (LMBs), sodium metal batteries (SMBs), and potassium metal batteries (KMBs) are receiving extensive attention in scientific literature. [1,2] The specific capacity of lithium, sodium, and potassium metal anodes is 3861 − , 1165 − , and 678 mAh g −−1 , which is substantially higher than that of graphite or hard carbons employed for ion battery anodes. For all three metal battery systems, achieving long-term stable and safe metal anode performance would be potentially transformative. However, growth of dendrites is a ubiquitous problem for each system, to date inhibiting wide scale commercial application of LMBs, SMBs, and KMBs in rechargeable cells. [3-6] The well-known risk is that dendrites will penetrate the separator and reach the cathode, resulting in a short circuit, potentially causing thermal runaway, burning, and even explosions. This is largely why Li metal anodes were originally abandoned in favor of graphite. [2,7] Less dramatically, dendrites result in a severe cell impedance increase, pouch swelling, as well as electrolyte drying. [3,8] The science around Li, Na, and K metal anodes is rapidly advancing. It is recognized that the structure of the solid electrolyte interface (SEI) plays a crucial role in determining the cyclability of metal anodes. [4,5] The SEI serves multiple roles, including limiting further side-reactions between the metal and the electrolyte, as well as promoting uniform metal deposition by regulating the solid-state ion flux. An ideal SEI layer has properties along the following: High cation conductance but also high electrical resistance, stable thickness close to a few nanometers, high mechanical toughness (combination of strength and ductility) leading to a tolerance to charginginduced volumetric changes, insolubility in the electrolyte, and stability over a wide range of operating temperatures and voltages. A stable SEI is an accepted prerequisite for safe battery performance, be it with a metal or an ion insertion anode. [6] The characteristics of SEI growth, gradual and uniform versus rapid and heterogeneous, is a key indicator whether or not dendrites form. [9-11] The dominant focus of many reports is on the spatially averaged SEI chemistry. [12,13] However recent progress brings fourth site-specific concepts in the SEI analysis, Anodes for lithium metal batteries, sodium metal batteries, and potassium metal batteries are susceptible to failure due to dendrite growth. This review details the structure-chemistry-performance relations in membranes that stabilize the anodes' solid electrolyte interphase (SEI), allowing for stable electrochemical plating/stripping. Case studies involving Li, Na, and K are presented to illustrate key concepts. "Classical" versus "modern" understandings of the SEI are described, with an emphasis on the new structural insights obtained through novel analytical techniques, including in situ liquid-secondary ion mass spectroscopy, titration gas chromatography, and tip-enhanced Raman spectroscopy. This Review highlights diver...

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Predicting Calendar Aging in Lithium Metal Secondary Batteries: The Impacts of Solid Electrolyte Interphase Composition and Stability

Cited by 50 publications

References 34 publications

Fast Diagnosis of Failure Mechanisms and Lifetime Prediction of Li Metal Batteries

Fast Diagnosis of Failure Mechanisms and Lifetime Prediction of Li Metal Batteries

Correlation between Li Plating Behavior and Surface Characteristics of Carbon Matrix toward Stable Li Metal Anodes

Review of Emerging Concepts in SEI Analysis and Artificial SEI Membranes for Lithium, Sodium, and Potassium Metal Battery Anodes

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