Lithium Mechanics: Roles of Strain Rate and Temperature and Implications for Lithium Metal Batteries

LePage, William S.; Chen, Yuxin; Kazyak, Eric; Chen, Kuan‐Hung; Sanchez, Adrian J.; Poli, Andrea; Arruda, Ellen M.; Thouless, M.D.; Dasgupta, Neil P.

doi:10.1149/2.0221902jes

Cited by 275 publications

(317 citation statements)

References 45 publications

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“…Further studies are required to elucidate the nature of this deformation, which depends on the nonlinear mechanical properties of metallic lithium. [29][30][31][32][33] the lifetime so far is more than an order of magnitude higher than that of the untreated cells.…”

Section: Methodsmentioning

confidence: 88%

Extended Cycling through Rigid Block Copolymer Electrolytes Enabled by Reducing Impurities in Lithium Metal Electrodes

Maslyn

Frenck

Loo

et al. 2019

ACS Appl. Energy Mater.

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Successful prevention of lithium dendrite growth would enable the use of lithium metal as an anode material in next-generation rechargeable batteries. Mechanically stiff block copolymer electrolytes have been shown to prolong the life of lithium metal cells by suppressing lithium dendrite growth. However, impurity particles that are invariably present in the lithium metal nucleate electrodeposition defects that eventually lead to short-circuits. In this study, we use X-ray tomography to study the morphology of electrodeposited lithium in symmetric cells containing a block copolymer electrolyte. An "electrochemical filtering" treatment was performed on these cells in order to reduce the concentration of impurity particles near the electrode-electrolyte interface, and cells were cycled to determine the effects of the treatment on lifetime. Depending on the treatment details, average charge passed before failure was improved by 30-400%. For a cell in which the treatment was most effective, cycle life was increased by more than an order of magnitude and the measured defect density was negligible. Other treated cells, however, in which the treated lithium was imperfect, had a higher areal density of defects compared to control cells. A majority of the defects in treated cells were confined within the electrodes. In contrast, most of the defects seen in the control cells were protrusions that invaded the electrolyte phase. The increased lifetime in these imperfectly treated cells was not due to a reduction in defect density, but rather due to the differences in defect morphology. These results motivate the development of deposition defect-and impurity-free lithium metal electrodes.

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Section: Methodsmentioning

confidence: 88%

Extended Cycling through Rigid Block Copolymer Electrolytes Enabled by Reducing Impurities in Lithium Metal Electrodes

Maslyn

Frenck

Loo

et al. 2019

ACS Appl. Energy Mater.

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“…2019, 9,1902568 In stark contrast, the depletion time t 0 for the Li-Mg alloy is not significantly affected by external pressure. [28,60,61] The homologous temperature may be a good descriptor for the combined temperature and pressure dependency of the cycling behavior. This can be traced back to the different depletion mechanisms taking place during stripping.…”

Section: Pressure Dependencementioning

confidence: 99%

Diffusion Limitation of Lithium Metal and Li–Mg Alloy Anodes on LLZO Type Solid Electrolytes as a Function of Temperature and Pressure

Krauskopf

Mogwitz

Rosenbach

et al. 2019

Advanced Energy Materials

316

421

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enable the lithium metal anode with high rate capability. [1][2][3][4] While in LIBs with liquid electrolytes, lithium dendrite growth and low Coulombic efficiency prevent the use of lithium metal as an anode material, [3,[5][6][7][8][9][10][11] solid electrolytes (SEs) had been predicted to be able to block dendrite growth due to their high shear modulus. [12,13] In this context, Li 7 La 3 Zr 2 O 12 (LLZO) type garnet SEs [14] have attracted great attention as they combine high ionic conductivity with sufficient electrochemical stability against lithium metal, which prevents fast degradation and growth of a resistive interphase. [15,16] Nevertheless, certain issues at the lithium|solid electrolyte interface remain unsolved. [17,18] Lithium penetration through garnet-type SEs currently limits the possible charge rates. [19][20][21][22][23] In this context, it was found that good contact to a small reservoir of lithium metal is highly beneficial to prevent inhomogeneous lithium nucleation, which then reduces the lithium penetration susceptibility. [24] All previous results underline the need for sufficient and homogeneous contact between metal and SE during battery operation. Thus, it is of upmost importance for lithium metal solid-state battery development to prevent pore formation and growth at the anode interface during battery discharge. [24][25][26] Indeed, while the intrinsic charge transfer kinetics of the lithium|LLZO interface was found to be sufficiently fast for practical applications (R int < 2 Ωcm²), [26,27] recent work shows that the morphological instability of the (pure) lithium metal anode on solid electrolytes under anodic load is an inherent, fundamental problem that needs to be solved for battery designs that do not allow high operation pressures in the MPa range. [26,28] The morphological instability stems from the vacancy injection into lithium metal during anodic dissolution, which is a general phenomenon of parent metal electrodes. [29,30] It leads to contact loss and unwanted local current constriction during cell discharge. Therefore, transport of lithium in the lithium metal anode itself needs to be better understood and tuned to further increase the rate capability of cells with a lithium metal anode (i.e., to per-cycle areal capacities of 5 mAh cm −2 at current densities ranging to 10 mA cm −2 ). [31] However, the currently run, predominantly short-term lithium shuttling experiments onThe morphological instability of the lithium metal anode is the key factor restricting the rate capability of lithium metal solid state batteries. During lithium stripping, pore formation takes place at the interface due to the slow diffusion kinetics of vacancies in the lithium metal. The resulting current focusing increases the internal cell resistance and promotes fast lithium penetration. In this work, galvanostatic electrochemical impedance spectroscopy is used to investigate operando the morphological changes at the interface by analysis of the interface capacitances. Therewith, the effect of temper...

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“…At this size, the major features of the surface are included, and CPU times for these 3D calculations are reasonable. We assume that the Li is elastic-perfectly-plastic for these low to moderate strain rates [65].…”

Section: Fft-based Elastic-perfectly-plastic Contact Modelingmentioning

confidence: 99%

“…It has recently been demonstrated [65,75,76] that creep plays a critical role in understanding the mechanics of Li metal. Unfortunately for the purposes of our analysis, most creep work has examined more-or-less pure Li metal [65,70,75,76].…”

Section: Creep Of LImentioning

confidence: 99%

“…Once a mechanical situation such as that shown in Figure 5 is created, Li metal will begin to creep away from regions of high stress to regions of low stress during intervals (which could be many hours) such as after charging but before discharging, or even during a slow charge. Thus, creep will also tend to smooth out Li metal surfaces and homogenize stress over time scales on the order of hours [65]. This possibility can be tested by rapidly charging multiple cells under identical electrochemical and pressure conditions.…”

Section: Creep Of LImentioning

confidence: 99%

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Rethinking How External Pressure Can Suppress Dendrites in Lithium Metal Batteries

Zhang

Wang

Harrison

et al. 2019

J. Electrochem. Soc.

134

115

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Lithium metal anodes are critical enablers for high energy density next generation batteries, but they suffer from poor morphology control and parasitic reactions. Recent experiments have shown that an external packing force on Li metal batteries with liquid electrolytes extends their lifetimes by inhibiting the growth of dendritic structures during Li deposition. However, the mechanisms by which pressure affects dendrite formation and growth have not been fully elucidated. For

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Lithium Mechanics: Roles of Strain Rate and Temperature and Implications for Lithium Metal Batteries

Cited by 275 publications

References 45 publications

Extended Cycling through Rigid Block Copolymer Electrolytes Enabled by Reducing Impurities in Lithium Metal Electrodes

Extended Cycling through Rigid Block Copolymer Electrolytes Enabled by Reducing Impurities in Lithium Metal Electrodes

Diffusion Limitation of Lithium Metal and Li–Mg Alloy Anodes on LLZO Type Solid Electrolytes as a Function of Temperature and Pressure

Rethinking How External Pressure Can Suppress Dendrites in Lithium Metal Batteries

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