Post-mortem analysis of calendar aged large-format lithium-ion cells: Investigation of the solid electrolyte interphase

Storch, Mathias; Hahn, Severin; Stadler, Jochen; Swaminathan, Ramanathan; Vranković, Dragoljub; Krupp, Carsten; Riedel, Ralf

doi:10.1016/j.jpowsour.2019.227243

Cited by 30 publications

(9 citation statements)

References 57 publications

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“…The second most important finding is a similar behavior for ΔCT4, starting at 50 h. The increase is not as pronounced as for ΔCT1, but it exists. This means, Li plating occurs roughly in the middle of the graphite anode; a place where it would be expected [43] . The reversible stripping of plated Li can be expected but it overlays with our measurement protocol in such a weak manifestation that our setup is not able to detect it.…”

Section: Resultsmentioning

confidence: 79%

“…This means, Li plating occurs roughly in the middle of the graphite anode; a place where it would be expected. [43] The reversible stripping of plated Li can be expected but it overlays with our measurement protocol in such a weak manifestation that our setup is not able to detect it. Altough the formation of SEI/CEI overlays during cell dilatation measurement, its cell expansion slope is very different compared to the one of lithium plating.…”

Section: Identifying LI Platingmentioning

confidence: 83%

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An Experimental Method to Determine the Measurement Error of Reference Electrodes within Lithium‐Ion Batteries

et al. 2023

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Reference electrodes (REs) play a crucial role in the accurate assessment and control of battery potentials, but their confidence is overestimated. Researchers have tracked the source of the error to the RE design that blocks the lithium‐ion path between anode and cathode. These errors or potential deviations are mostly modeled or less‐frequently estimated after observing Li plating post‐mortem. This is the first study to showcase an experimental method that allows a more precise error quantification in‐operando of a RE. The key idea is to relate the error‐affected reference potential to an unaffected quantity, such as the cell dilatation. Although our experimental setups are special, this approach can also be applied to different setups and REs. Using the presented method, we provoked Li plating in NMC811/graphite pouch cells and determined the potential deviation of our perforated RE to be 12 mV under fast charging conditions. In contrast to previous studies, we found the error to be positive, offering a new explanation of the error mechanism of REs.

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Section: Resultsmentioning

confidence: 79%

Section: Identifying LI Platingmentioning

confidence: 83%

An Experimental Method to Determine the Measurement Error of Reference Electrodes within Lithium‐Ion Batteries

et al. 2023

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“…increases (Figure ). Thus, the decomposition of carbonates increases . The F–P (or P–F) peaks in F 1s spectra come from LiPF 6 in the electrolytes, and the aggravated decomposition of LiPF 6 can be observed along with the continuous increase of LiF and P–O in F 1s and P 2p spectra, respectively.…”

Section: Resultsmentioning

confidence: 99%

High-Temperature Storage Deterioration Mechanism of Cylindrical 21700-Type Batteries Using Ni-Rich Cathodes under Different SOCs

Zhang

Tian

et al. 2021

ACS Appl. Mater. Interfaces

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The safety and energy density of lithium-ion batteries (LIBs) are important concerns. The use of high-capacity cathode materials, such as Ni-rich cathodes, can greatly improve the energy density of LIBs, but it also brings some safety hazards. Cylindrical 21700-type batteries using Ni-rich cathodes were employed here to investigate their high-temperature storage deterioration mechanism under different states of charge (SOCs). Electrolyte decomposition was identified as the main problem. It can be worsened by elevated storage temperatures and battery SOCs, with the latter having a more significant influence. Specifically, the decomposition of the LiPF 6 solute and the carbonate solvent will induce hydrofluoric acid (HF) formation and solid−electrolyte interphase (SEI) film regeneration, respectively. HF erosion will aggravate the dissolution of transition metal ions and structural degradation of cathode materials, while the destruction/regeneration of SEI films will consume active lithium and hinder Li + diffusion at the anode side. Besides, the self-discharge behavior will also enlarge the graphite layer spacing, thus decreasing the graphitization degree of graphite anodes and causing anode failure. These findings will aid in the development of strategies for improving the safety of LIBs with high energy density.

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“…The depth dependent composition of the CEI was interrogated using Ar + (g) sputtering, where measurements were collected after 0, 1, 5, 10, and 30 min of sputtering time. Although there is a possibility of inducing chemical changes in the samples due to sputtering, Ar sputtering is an established method for providing depth resolved surface film information for state-of-the-art Li-ion anodes − and cathodes. , …”

Section: Resultsmentioning

confidence: 99%

Degradation in Ni-Rich LiNi_1–x–yMn_xCo_yO₂/Graphite Batteries: Impact of Charge Voltage and Ni Content

et al. 2023

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Ni-rich LiNi 1−x−y Mn x Co y O 2 (NMC) materials are attractive as cathodes for Li-ion batteries due to their high energy density and low Co content. However, these materials may display poor electrochemical reversibility relating to structural and interfacial instabilities. The influence of Ni content and level of delithiation during charge on degradation mechanisms and relevance to electrochemical cycling behavior are probed for LiNi 0.6 Mn 0.2 Co 0.2 O 2 (NMC622) and LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) cathode materials in a full cell configuration under two upper voltage limits (4.1 and 4.3 V). The combined use of dQ/dV analysis of electrochemical voltage profiles, operando XRD, and postcycling scanning electron microscopy (SEM) measurements indicates that a major contributor to capacity fade is the large anisotropic volume change from an H2 ⇄ H3 phase transition and associated mechanical degradation particularly for NMC811. Notably, transition metal dissolution and deposition on the negative electrode are found to correlate with the structural changes occurring in the cathode under high voltage charge. X-ray photoelectron spectroscopy (XPS) analyses of the cycled cathodes reveal a more organic-rich cathode−electrolyte interphase (CEI) when cycling to 4.3 V with lower relative amounts of LiF. Surface reconstruction is not a significant factor under these cycling conditions as determined by soft X-ray absorption spectroscopy (sXAS) analysis. The results emphasize the opportunity to match the electrochemical test parameters with the specific NMC active material to mitigate degradation and extend cycle life.

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Post-mortem analysis of calendar aged large-format lithium-ion cells: Investigation of the solid electrolyte interphase

Cited by 30 publications

References 57 publications

An Experimental Method to Determine the Measurement Error of Reference Electrodes within Lithium‐Ion Batteries

An Experimental Method to Determine the Measurement Error of Reference Electrodes within Lithium‐Ion Batteries

High-Temperature Storage Deterioration Mechanism of Cylindrical 21700-Type Batteries Using Ni-Rich Cathodes under Different SOCs

Degradation in Ni-Rich LiNi_1–x–yMn_xCo_yO₂/Graphite Batteries: Impact of Charge Voltage and Ni Content

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Post-mortem analysis of calendar aged large-format lithium-ion cells: Investigation of the solid electrolyte interphase

Cited by 30 publications

References 57 publications

An Experimental Method to Determine the Measurement Error of Reference Electrodes within Lithium‐Ion Batteries

An Experimental Method to Determine the Measurement Error of Reference Electrodes within Lithium‐Ion Batteries

High-Temperature Storage Deterioration Mechanism of Cylindrical 21700-Type Batteries Using Ni-Rich Cathodes under Different SOCs

Degradation in Ni-Rich LiNi1–x–yMnxCoyO2/Graphite Batteries: Impact of Charge Voltage and Ni Content

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Degradation in Ni-Rich LiNi_1–x–yMn_xCo_yO₂/Graphite Batteries: Impact of Charge Voltage and Ni Content