Understanding multi-scale battery degradation with a macro-to-nano zoom through its hierarchy

Zan, Guibin; Zhang, Jin; Monaco, Federico; Gul, Sheraz; Qian, Guannan; Li, Jizhou; Vine, D. J.; Cloetens, Peter; Yun, Wenbing; Pianetta, P.; Liu, Yijin

doi:10.1039/d1ta02262h

Cited by 17 publications

(23 citation statements)

References 40 publications

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“…The heterogeneous nature of electrochemical reactions and mechanical degradation places a daunting challenge in electron and X-ray characterizations. − Recent large-scale electrode studies have uncovered that particle cracking is highly heterogeneous in composite electrodes. There are fundamental reasons and practical implications of such heterogeneity, which is ubiquitous even in the best-optimized commercial battery electrodes. ,− Figure exemplifies such heterogeneity in a section of a practical electrode containing thousands of active particles. In a well-prepared academic electrode (Figure a), the degree of damage heterogeneity is overwhelmingly significant.…”

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Heterogeneous Reaction Activities and Statistical Characteristics of Particle Cracking in Battery Electrodes

2021

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Heterogeneous Reaction Activities and Statistical Characteristics of Particle Cracking in Battery Electrodes

2021

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“…Heterogeneity in cathode packing, the electrode polarization effect, and differences in particle size have been broadly reported. 43,44 The cause of heterogeneous performance can occur because of the interplay between the cathode and anode as observed in a previous study. 45 Improved performance in the cathode results in higher delithiation of the cathode, leading to higher lithiation of the anode after charge.…”

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confidence: 87%

“…Additionally, factors independent of both the cathode and anode such as separator porosity, electrolyte wetting, and uneven stack pressure can also influence local performance independent of the initial cathode and anode build. Local current heterogeneities have been linked to accelerated disintegration of cathode secondary particles and delamination of sections of the cathode . In large format cells, entire regions can underperform because of large-scale cell build defects .…”

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“…Local current heterogeneities have been linked to accelerated disintegration of cathode secondary particles and delamination of sections of the cathode. 44 In large format cells, entire regions can underperform because of large-scale cell build defects. 12 For the anode, heterogeneities in lithiation of graphite have been linked to increased probability of the electrodeposition of Li metal, especially for thicker electrodes where overcharging near the top of the electrode results in electrodeposition of Li metal when diffusion kinetics are insufficient to move enough lithium to the back of the electrode.…”

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Comprehensive Insights into Nucleation, Autocatalytic Growth, and Stripping Efficiency for Lithium Plating in Full Cells

et al. 2021

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Synchrotron high-energy X-ray diffraction is used to enable nondestructive detection and quantification of heterogeneous lithium plating in working batteries. In this study a Li-Ni 0.5 Mn 0.3 Co 0.2 O 2 /graphite pouch cell was operated under 6C fastcharge rate for greater than 1200 cycles. The magnitude and spatial distribution of lithium plating, lithium stripping, and the effect of metallic lithium deposition on lithium intercalation into graphite were quantified. Fully intercalated graphite (LiC 6 ) was detected after discharge with a lateral distribution closely correlated with lithium plating, which can be used as a higher-sensitivity indicator for lithium plating. Over an extended cycle life, the overall metallic lithium concentration followed a sigmoidal curve indicating two-stage continuous nucleation and autocatalytic growth. The lithium stripping efficiency underwent an exponential decay as a function of cycle life as the buildup of metallic lithium hindered the efficient dissolution back into the electrolyte. The findings provide direct insights into the characteristics of lithium plating and stripping under realistic fast-charge conditions.

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“…[27][28][29][30] In the literature, X-ray tomography has been used to analyze the defects in commercial lithium batteries, to investigate different battery components, and to do so under extreme conditions, for example, high temperature, low temperature, ultra-fast charging, and thermal runaway. [31][32][33][34][35] Specific to Zn batteries, Yufit et al studied the Zn dendrite formation and dissolution in Zn-air battery using X-ray tomography and reported that the dendrite growth is promoted at the locations with high current density and with residual Zn deposits. The Zn dendrites can also be mechanically deformed by the separator, forming a more compact structure compared to the "open cell" scenario.…”

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Structural, Dynamic, and Chemical Complexities in Zinc Anode of an Operating Aqueous Zn‐Ion Battery

Qian

Zan

et al. 2022

Advanced Energy Materials

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motivated significant efforts to exploit alternative electrochemical processes for energy storage in order to meet the evergrowing demand for efficient energy storage. A promising candidate for EES is the rechargeable Zn aqueous battery, which is earth abundant, low cost, safe, and environmentally friendly. [3][4][5][6] However, despite of enormous research and engineering investments, the practical implementation and deployment of Zn aqueous batteries are still hindered by challenges concerning several different aspects of the electrochemical reaction involving Zn-ions.One of the main obstacles is that the Zn anode suffers from a low Coulombic efficiency, and the underlying mechanism is related with the non-ideal reversibility of the Zn plating/stripping process. [7,8] The behavior of Zn plating and stripping is sophisticated and can be modulated by several co-existing and interrelated factors, including the electrode configurations, [9][10][11] the charging/discharging protocols, [12] and the electrolyte formulations. [13][14][15][16][17] For example, it has been demonstrated that the anode morphology can affect the dendrite growth. By fabricating a Zn anode with a 3D sponge structure, the Ni-Zn cells could exhibit an improved cycle performance and a suppressed dendrite formation. [18] Plating with high current density can exacerbate the electrochemical polarization and tends to form Zn dendrites. As a mitigation, the Zn dendrites can be dissolved by applying a small current during the stripping process. [12] In addition, surface chemistry on the anode plays a critical role in the Zn plating/stripping process. [19,20] The reactions involving the solid-liquid interphase are often complicated and may vary depending on the electrolyte used. For example, in alkaline electrolytes, Zn electrodes suffer from surface self-corrosion, in which metallic Zn is oxidized into a Zn (OH) 4 2− ion and is further decomposed into the by-product ZnO during plating. The insulating ZnO layer on the Zn electrode surface could impede the Zn-ion transfer between electrolyte and electrode. [21] Corrosion of the Zn electrode could also occur in mild electrolytes, for example, ZnSO 4 aqueous electrolyte, but through different surface chemical reactions. [22] The insoluble Zn 4 SO 4 (OH) 6 •xH 2 O could be deposited on the electrode surface in ZnSO 4 electrolyte, together with irreversible H 2 release, resulting in poor Coulombic efficiency and capacity fade. [23][24][25] To tackle this issue, Cao et al. used an alkylammonium Aqueous Zn-ion battery is a promising technology for electrochemical energy storage. The formation of Zn dendrites, however, can jeopardize the cell cycle life and thus, hinders the industrial adoption of this technology. A fundamental understanding of the kinetic mechanisms is crucial for improving the Zn-ion battery. Here, in situ and operando X-ray microscopy methods are utilized to visualize the Zn plating and stripping behaviors under different electrochemical conditions. It is demonstrated that the substrate cur...

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Understanding multi-scale battery degradation with a macro-to-nano zoom through its hierarchy

Abstract: Lithium-ion battery (LIB) is featured by structural and chemical complexities across a broad range of length scales. Ultimately, it is the hierarchy of the battery structure that determines its functionality....

Cited by 17 publications

References 40 publications

Heterogeneous Reaction Activities and Statistical Characteristics of Particle Cracking in Battery Electrodes

Heterogeneous Reaction Activities and Statistical Characteristics of Particle Cracking in Battery Electrodes

Comprehensive Insights into Nucleation, Autocatalytic Growth, and Stripping Efficiency for Lithium Plating in Full Cells

Structural, Dynamic, and Chemical Complexities in Zinc Anode of an Operating Aqueous Zn‐Ion Battery

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