Mechanistic Analysis of Microstructural Attributes to Lithium Plating in Fast Charging

Kabra, Venkatesh; Parmananda, Mukul; Fear, Conner; Usseglio-Viretta, François; Colclasure, Andrew M.; Smith, Kandler; Mukherjee, Partha P.

doi:10.1021/acsami.0c15144

Cited by 27 publications

(17 citation statements)

References 57 publications

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“…A local voltage variation of up to 0.3 V during charge has been measured for graphite anodes. 106 This variation has been entirely attributed to kinetic limitations/ohmic losses; our predictions suggest that structural origins may also need to be explored.…”

Section: Dol Reductive Decomposition On Coated LImentioning

confidence: 88%

Galvanic Corrosion and Electric Field in Lithium Anode Passivation Films: Effects on Self-Discharge

2022

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Battery interfaces help govern rate capability, safety/stability, cycle life, and self-discharge, but significant gaps remain in our understanding at atomic length scales that can be exploited to improve the interfacial properties. In particular, Li partially plated on copper current collectors, relevant to the anodeless, lithium metal cell, which is a holy grail of high-density-energy battery research, has recently been reported to undergo galvanic corrosion and exhibit short shelf lives. We apply large-scale density functional theory (DFT) calculations and X-ray photoelectron spectroscopy to examine the reaction between the electrolyte and Li| Cu junctions coated with uniform, thin electrolyte interphase (SEI) passivating films at two applied voltages. The DFT galvanic corrosion calculations show that electrolyte degradation preferentially occurs on Li-plated regions and should lead to thicker SEI films. We find similarities but also fundamental differences between traditional metal localized pitting and Li-corrosion mechanisms due to overpotential and ionic diffusion rate disparities in the two cases. Furthermore, using the recently proposed, highly reactive lithium hydride (LiH) component SEI as an example, we distinguish between electrochemical and chemical degradation pathways that are partially responsible for self-discharge, with the chemical pathway found to exhibit slow kinetics. We also predict that electric fields should, in general, exist across natural SEI components like LiH and across artificial SEI films like LiI and LiAlO 2 often applied to improve battery cycling. Underlying and unifying these predictions is a framework of DFT voltage/overpotential definitions, which we have derived from electrochemistry disciplines like structural metal corrosion studies; our analysis can only be made using the correct electronic voltage definitions.

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Section: Dol Reductive Decomposition On Coated LImentioning

confidence: 88%

Galvanic Corrosion and Electric Field in Lithium Anode Passivation Films: Effects on Self-Discharge

2022

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“…The performance of LIBs is significantly affected by the interaction of temperature and C rate. 11,17,28 Figure 1 shows the charging−discharging voltage curves obtained for batteries cycled for 50 cycles at different temperatures and C rates, and the inset corresponds to the macroscopic morphology of the graphite anode after the 51st charging cycle. Figure 1a− °C and the macroscopic appearances of the graphite anodes, from which the performance deteriorates further.…”

Section: Plating Phenomenon Observationmentioning

confidence: 99%

“…Lithium-ion batteries (LIBs) are widely used in electronics, public transportation, and energy storage based on their high energy and power density, long cycle life, and environmental friendliness. − However, Li plating can easily lead to potential safety hazards, which is a problem that cannot be ignored. , Li plating occurs when lithium ions (Li + ) are reduced to metallic Li on the surface of the graphite anode during the charging process of the battery, which prevents normal intercalation. , Usually, poor battery balance, such as mismatched anode–cathode ratio (N/P) or manufacturing defects, and abuse of operating conditions, such as high C rate charging or low-temperature charging, will lead to Li plating. − Li plating can lead to a reduction in the battery capacity and the formation of strong Li dendrites, which can puncture the separator and cause a short circuit, resulting in thermal runaway or even explosion. , Therefore, prevention of Li plating is essential for the safety and performance of LIBs.…”

Section: Introductionmentioning

confidence: 99%

Pattern Investigation and Quantitative Analysis of Lithium Plating under Subzero Operation of Lithium-Ion Batteries

Sun

Zhang

et al. 2023

ACS Appl. Mater. Interfaces

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Safety hazards arising from lithium (Li) plating during the operation of lithium-ion batteries (LIBs) are a constant concern. Herein, this work explores the coaction of low temperatures and current rates (C rates) on Li plating in LIBs by electrochemical tests, material characterization, and numerical analysis. With a decrease in temperature and an increase in C rate, the battery charging process shifts from normal intercalation to Li plating and even ultimately fails at −20 °C and 0.5C. The morphology observations reveal the detailed growth process of individual plated Li through sand-like Li, whisker Li, dendritic Li, mossy Li, and finally bulk Li, as well as aggregated Li from sparse to dense. Through quantitative analysis, the dynamic pattern under long-term cycles is revealed. The low temperature and high C rate will lead to an increase in Li plating capacity and irreversibility, which are further deteriorated with the cycles. In addition, a critical condition of high Li plating and high reversibility at −10 °C and 0.2C is found, and further studies are needed to reveal the competition between kinetics and thermodynamics in the Li plating process. This work provides detailed information on the range and growth process of Li plating and quantifies Li plating, which can be used for practical Li plating prediction and regulation.

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“…[2,8] For a given electrolyte, the propensity of a graphite electrode to incur plating is strongly influenced by the electrode's microstructure. [9] During fast charging, severe Li concentration gradients in the electrolyte along the through-plane direction can lead to high currents being experienced by the graphite near the separator. [10][11][12][13] Li concentration gradients are particularly severe for electrodes with high tortuosity and thicknesses due to the increased ionic transport resistance.…”

Section: Introductionmentioning

confidence: 99%

Dynamic In‐Plane Heterogeneous and Inverted Response of Graphite to Fast Charging and Discharging Conditions in Lithium‐Ion Pouch Cells

et al. 2023

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Solutions for improving fast charging of lithium‐ion batteries have largely focused on alleviating through‐plane lithiation gradients while little is understood about in‐plane heterogeneities and how to resolve them. Herein, high‐speed synchrotron X‐ray diffraction (XRD) resolves graphite lithiation spatially and temporally during 6 C charging and 2 C discharging. At every point during operation, considerable differences in the state of lithiation across the pouch cell are present. Some regions are more responsive to operation than others, reaching full lithiation early during charge and full delithiation during discharge. Other regions within the cell never fully delithiate during discharge, despite a prolonged voltage hold at 2.8 V. Using time‐resolved XRD data, the calculated local current density (mA cm−2) at the graphite surface shows an unexpected occurrence of local inverted current densities where regions of graphite are observed to delithiate during charging and lithiate during discharging. A pseudo‐3D model is developed for the graphite electrode with spatially varying microstructural tortuosity to show how microstructural heterogeneity could influence spatial charge dynamics. The model could not predict the complex in‐plane charge behavior observed within the cell. Consequently physics‐based charging protocols based on homogeneous electrode assumptions may underestimate the local variations in charge dynamics and occurrence of lithium plating.

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Mechanistic Analysis of Microstructural Attributes to Lithium Plating in Fast Charging

Cited by 27 publications

References 57 publications

Galvanic Corrosion and Electric Field in Lithium Anode Passivation Films: Effects on Self-Discharge

Galvanic Corrosion and Electric Field in Lithium Anode Passivation Films: Effects on Self-Discharge

Pattern Investigation and Quantitative Analysis of Lithium Plating under Subzero Operation of Lithium-Ion Batteries

Dynamic In‐Plane Heterogeneous and Inverted Response of Graphite to Fast Charging and Discharging Conditions in Lithium‐Ion Pouch Cells

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