Evolving contact mechanics and microstructure formation dynamics of the lithium metal-Li7La3Zr2O12 interface

Chang, Wesley; May, Richard; Wang, Michael J.; Thorsteinsson, Gunnar; Sakamoto, Jeff; Marbella, Lauren E.; Steingart, Dan

doi:10.1038/s41467-021-26632-x

Cited by 32 publications

(28 citation statements)

References 45 publications

(42 reference statements)

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“…This ex situ method is difficult to extend to SSBs systems, because disassembling SSBs will inevitably damage the interphases and interfaces. Operando nondestructive techniques, including X-ray computed tomography (X-ray CT) 32 , neutron depth profiling (NDP) 33 , nuclear magnetic resonance (NMR) and magnetic resonance imaging (MRI) 34 , have been confirmed to be capable of noninvasively probing the interphase/interior of SSEs. Among them, NMR and MRI are well-suited for this task 35 , 36 .…”

Section: Introductionmentioning

confidence: 99%

“…Unlike liquid electrolyte LMBs, SSBs require extra stacking pressure to maintain good solid-solid contact. Previous operando NMR/MRI studies for SSBs have widely adopted the Li|SSEs|Li or Li|SSEs|Cu cells 34 , 39 , 40 . A more practical cell configuration with lithium transition metal oxide as the cathode has not yet been reported in operando NMR/MRI studies in SSBs.…”

Section: Introductionmentioning

confidence: 99%

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Understanding the failure process of sulfide-based all-solid-state lithium batteries via operando nuclear magnetic resonance spectroscopy

et al. 2023

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The performance of all-solid-state lithium metal batteries (SSLMBs) is affected by the presence of electrochemically inactive (i.e., electronically and/or ionically disconnected) lithium metal and solid electrolyte interphase (SEI), which are jointly termed inactive lithium. However, the differentiation and quantification of inactive lithium during cycling are challenging, and their lack limits the fundamental understanding of SSLMBs failure mechanisms. To shed some light on these crucial aspects, here, we propose operando nuclear magnetic resonance (NMR) spectroscopy measurements for real-time quantification and evolution-tracking of inactive lithium formed in SSLMBs. In particular, we examine four different sulfide-based solid electrolytes, namely, Li10GeP2S12, Li9.54Si1.74P1.44S11.7Cl0.3, Li6PS5Cl and Li7P3S11. We found that the chemistry of the solid electrolyte influences the activity of lithium. Furthermore, we demonstrate that electronically disconnected lithium metal is mainly found in the interior of solid electrolytes, and ionically disconnected lithium metal is found at the negative electrode surface. Moreover, by monitoring the Li NMR signal during cell calendar ageing, we prove the faster corrosion rate of mossy/dendritic lithium than flat/homogeneous lithium in SSLMBs.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Understanding the failure process of sulfide-based all-solid-state lithium batteries via operando nuclear magnetic resonance spectroscopy

et al. 2023

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“…Furthermore, deformable materials are used between cells to reduce pressure variance from expansion and contraction [1]. Based on current research on lithium-metal [6,18] and Silicon [5,10,19] cells, future battery packs will likely benefit from higher stack pressure applied to cells. Presently, studies focusing on lithium-ion batteries [1][2][3] aim to influence pack design by improving understanding of stack pressure and performance.…”

Section: Introductionmentioning

confidence: 99%

“…However, because the width between each plate is essentially fixed, stack pressure varies during charging and discharging due to elastic swelling, with SOC due to differences in electrode volumes, and over time increases due to negative electrode growth [1,[21][22][23]. These variations in pressure over time can cause premature breakdown of the cell materials [18]. Hahn et al [1] studied the long-term effects of mechanical pressure by using a hydraulic cylinder and foam to act as a spring element.…”

Section: Introductionmentioning

confidence: 99%

Investigation of Constant Stack Pressure on Lithium-Ion Battery Performance

Leonard¹,

Planden²,

Lukow³

2023

Preprint

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Current research involving applying stack pressure to lithium-pouch cells has shown both performance and lifetime benefits. Fixtures are used to mimic this at the cell level and conventionally prescribe a constant displacement onto the cell. This increases stack pressure but also causes pressure to vary. Despite this, applying an initial stack pressure improves cell conductivity, as well as cell lifetime [1, 2]. In this paper, a fixture was designed that applies constant pressure to the cell independent of displacement. Thefixture uses pneumatics to apply a constant stack pressure independent of elastic andplastic swelling. Cells constrained by the constant pressure fixture (CPF) fixture anda conventional fixture (MBPF) were evaluated using a Hybrid Pulse Power Characterization (HPPC) test, to measure internal resistance and maximum deliverable power. Multiple stack pressures were applied to investigate differences in pressure variation and performance between constant pressure and constant displacement, while all tests were additionally compared to control tests with no applied stack pressure. The CPF reduced pressure variation during charging and discharging. revealing the performance effects of maintaining uniform pressure. Applying constant stack pressure reduced the discharge impedance and improved discharged power of the tested cell but did not improve charge performance. Additionally, all constraining methods reported lower internal resistance with maximum current compared to 50% maximum current. Discharge performance benefits from constant pressure could influence pack design to improve vehicle performance.

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“…There are few direct and quantitative studies on evolution kinetics at practical current densities and capacities. Some powerful methods such as synchrotron x-ray computed tomography or solidstate nuclear magnetic resonance can help to evaluate the void-induced contact loss and dendrite failures in a nondestructive way (22)(23)(24)(25)(26)(27). Considering the buried Li/SSE interfaces, the observations still confront dilemmas (28), where the resolution is insufficient to unravel the key morphological features of voids.…”

Section: Introductionmentioning

confidence: 99%

The void formation behaviors in working solid-state Li metal batteries

Zhao

et al. 2022

Sci. Adv.

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The fundamental understanding of the elusive evolution behavior of the buried solid-solid interfaces is the major barrier to exploring solid-state electrochemical devices. Here, we uncover the interfacial void evolution principles in solid-state batteries, build a solid-state void nucleation and growth model, and make an analogy with the bubble formation in liquid phases. In solid-state lithium metal batteries, the lithium stripping–induced interfacial void formation determines the morphological instabilities that result in battery failure. The void-induced contact loss processes are quantified in a phase diagram under wide current densities ranging from 1.0 to 10.0 milliamperes per square centimeter by rational electrochemistry calculations. The in situ–visualized morphological evolutions reveal the microscopic features of void defects under different stripping circumstances. The electrochemical-morphological relationship helps to elucidate the current density– and areal capacity–dependent void nucleation and growth mechanisms, which affords fresh insights on understanding and designing solid-solid interfaces for advanced solid-state batteries.

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Evolving contact mechanics and microstructure formation dynamics of the lithium metal-Li7La3Zr2O12 interface

Cited by 32 publications

References 45 publications

Understanding the failure process of sulfide-based all-solid-state lithium batteries via operando nuclear magnetic resonance spectroscopy

Understanding the failure process of sulfide-based all-solid-state lithium batteries via operando nuclear magnetic resonance spectroscopy

Investigation of Constant Stack Pressure on Lithium-Ion Battery Performance

The void formation behaviors in working solid-state Li metal batteries

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