Understanding capacity fading mechanism of thick electrodes for lithium-ion rechargeable batteries

Park, Kyu‐Young; Park, Ji Won; Seong, Won Mo; Yoon, Kyungho; Hwang, Taehyun; Ko, Kun-Hee; Han, Jae-Il; Jaedong, Yang; Kang, Kisuk

doi:10.1016/j.jpowsour.2020.228369

Cited by 63 publications

(43 citation statements)

References 35 publications

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“…Cells with thick-film electrodes suffer severe capacity fade with increasing discharge current, losing over 60% of the capacity at C/2 compared to capacities at C/20. This may due to the limited lithium-ion charge transfer resistance, local material degradation, and micro-cracks formation on the electrode surface owing to the inhomogeneity of applied current [ 26 ]. Although cells with electrodes without acid (slurry pH value of 12.1) show the highest discharge capacity after C/10, the extremely high porosity around 60% hinders the possibility of achieving high volumetric energy densities.…”

Section: Discussionmentioning

confidence: 99%

“…The costs of other manufacturing steps during assembling such as cutting, welding, and stacking, will be reduced [ 9 ]. However, the lithium-ion diffusion kinetics inside thick-film electrodes will be the bottleneck to enable high power operation at high charging/discharging rates [ 26 ]. In order to solve this problem, structuring of thick-film electrodes (“3-dimensional battery”) using ultrafast laser ablation opens a new path to simultaneously increase energy density and power density [ 27 , 28 , 29 , 30 ].…”

Section: Introductionmentioning

confidence: 99%

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Characterization and Laser Structuring of Aqueous Processed Li(Ni0.6Mn0.2Co0.2)O2 Thick-Film Cathodes for Lithium-Ion Batteries

2021

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Lithium-ion batteries have led the revolution in portable electronic devices and electrical vehicles due to their high gravimetric energy density. In particular, layered cathode material Li(Ni0.6Mn0.2Co0.2)O2 (NMC 622) can deliver high specific capacities of about 180 mAh/g. However, traditional cathode manufacturing involves high processing costs and environmental issues due to the use of organic binder polyvinylidenfluoride (PVDF) and highly toxic solvent N-methyl-pyrrolidone (NMP). In order to overcome these drawbacks, aqueous processing of thick-film NMC 622 cathodes was studied using carboxymethyl cellulose and fluorine acrylic hybrid latex as binders. Acetic acid was added during the mixing process to obtain slurries with pH values varying from 7.4 to 12.1. The electrode films could be produced with high homogeneity using slurries with pH values smaller than 10. Cyclic voltammetry measurements showed that the addition of acetic acid did not affect the redox reaction of active material during charging and discharging. Rate capability tests revealed that the specific capacities with higher slurry pH values were increased at C-rates above C/5. Cells with laser structured thick-film electrodes showed an increase in capacity by 40 mAh/g in comparison to cells with unstructured electrodes.

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Section: Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Characterization and Laser Structuring of Aqueous Processed Li(Ni0.6Mn0.2Co0.2)O2 Thick-Film Cathodes for Lithium-Ion Batteries

2021

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“…Furthermore, such Li content heterogeneity will induce an increase in the local current density and abrupt structural changes in the crystal domains. As reaction heterogeneity also limits capacity utilization, [16][17][18] the phase transformation dynamics, particularly at fast cycling conditions, must be understood and controlled.…”

Section: Introductionmentioning

confidence: 99%

Suppressing High‐Current‐Induced Phase Separation in Ni‐Rich Layered Oxides by Electrochemically Manipulating Dynamic Lithium Distribution

et al. 2021

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cathode materials and improve their stability and energy density. [1,2] In particular, Ni-rich NCM (LiNi x Co y Mn 1−x−y O 2 , x > 0.5) is a promising cathode material with high reversible capacity and has been successfully implemented in commercial energy storage systems, such as mobile devices and electric vehicles. [1] For Ni-rich layered oxides, the whole reaction pathway has been described as proceeding through a series of isostructural hexagonal phases, conventionally labeled as H1, H2, and H3 phases depending on the depth of charge. [3,4] The fundamental difference between H1 and H2 is the Li-content-dependent in-plane structure in the Li layer. [3,5] Because of the structural similarities of these evolving phases during cycling, the solid solution reaction has been predicted to be a thermodynamically favorable reaction pathway by first-principle studies [6] and was also observed by operando X-ray diffraction (XRD) experiments at moderate cycling rates in Ni-rich layered oxides, such as LiNi 0.6 Co 0.2 Mn 0.2 O 2 (NCM622) [7] and LiNi 0.8 Co 0.1 Mn 0.1 O 2 . [3,4] Homogeneous Li transport, characterized by solid solution behaviors, is considered to be advantageous for obtaining a long cycle lifetime. [8] However, in dynamic situations such as fast cycling, limited Li diffusivity can induce a heterogeneous Li distribution within Understanding the cycling rate-dependent kinetics is crucial for managing the performance of batteries in high-power applications. Although high cycling rates may induce reaction heterogeneity and affect battery lifetime and capacity utilization, such phase transformation dynamics are poorly understood and uncontrollable. In this study, synchrotron-based operando X-ray diffraction is performed to monitor the high-current-induced phase transformation kinetics of LiNi 0.6 Co 0.2 Mn 0.2 O 2 . The sluggish Li diffusion at high Li content induces different phase transformations during charging and discharging, with strong phase separation and homogeneous phase transformation during charging and discharging, respectively. Moreover, by exploiting the dependence of Li diffusivity on the Li content and electrochemically tuning the initial Li content and distribution, phase separation pathway can be redirected to solid solution kinetics at a high charging rate of 7 C. Finite element analysis further elucidates the effect of the Li-content-dependent diffusion kinetics on the phase transformation pathway. The findings suggest a new direction for optimizing fast-cycling protocols based on the intrinsic properties of the materials.

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“…Secondary NCM111 particles 2.38 g cm −3 166.99 mAh g −1 @ 16 mA g −1 93% @ 16 mA g −1 after 30 cycles - [162] LiNi 0.6 Co 0.2 Mn 0.2 O 2 secondary particles 28 mg cm −2 2.8-2.9 g cm −3 150 mAh g −1 @ 1 C 4.2 mAh cm −2 [163] Commercial LiNi x Mn y Co z O 2 15-20 mg cm −2 ≈2.0-2.5 g cm −3…”

Section: Improving Adhesion Between Active Materials and Current Collectormentioning

confidence: 99%

Commercialization‐Driven Electrodes Design for Lithium Batteries: Basic Guidance, Opportunities, and Perspectives

Cao

Liang

Zhang

et al. 2021

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vehicles (HEVs), because of their high energy density and long lifetime. [1][2][3] In recent years, the ever-growing demand on electric vehicles contributes to the continuous growth of the battery market, and the energy storage devices of EVs/HEVs raise stern demands on higher energy density (>300 Wh kg −1 ) and lower cost (500 Wh kg −1 ), and the standard parameters for different electrode systems toward this high energy density goal are well summarized in the previous works. [7][8][9] In particular, the innovative battery chemistries (i.e., Li-metal battery and all-solid-state lithium battery) using Li metal as anode, exhibit much higher energy density than current lithium-ion batteries, whereas some technological issues are needed to be addressed first, such as dendrite formation suppression, industrial battery Current lithium-ion battery technology is approaching the theoretical energy density limitation, which is challenged by the increasing requirements of ever-growing energy storage market of electric vehicles, hybrid electric vehicles, and portable electronic devices. Although great progresses are made on tailoring the electrode materials from methodology to mechanism to meet the practical demands, sluggish mass transport, and charge transfer dynamics are the main bottlenecks when increasing the areal/volumetric loading multiple times to commercial level. Thus, this review presents the state-of-the-art developments on rational design of the commercialization-driven electrodes for lithium batteries. First, the basic guidance and challenges (such as electrode mechanical instability, sluggish charge diffusion, deteriorated performance, and safety concerns) on constructing the industry-required high mass loading electrodes toward commercialization are discussed. Second, the corresponding design strategies on cathode/anode electrode materials with high mass loading are proposed to overcome these challenges without compromising energy density and cycling durability, including electrode architecture, integrated configuration, interface engineering, mechanical compression, and Li metal protection. Finally, the future trends and perspectives on commercializationdriven electrodes are offered. These design principles and potential strategies are also promising to be applied in other...

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Understanding capacity fading mechanism of thick electrodes for lithium-ion rechargeable batteries

Cited by 63 publications

References 35 publications

Characterization and Laser Structuring of Aqueous Processed Li(Ni0.6Mn0.2Co0.2)O2 Thick-Film Cathodes for Lithium-Ion Batteries

Characterization and Laser Structuring of Aqueous Processed Li(Ni0.6Mn0.2Co0.2)O2 Thick-Film Cathodes for Lithium-Ion Batteries

Suppressing High‐Current‐Induced Phase Separation in Ni‐Rich Layered Oxides by Electrochemically Manipulating Dynamic Lithium Distribution

Commercialization‐Driven Electrodes Design for Lithium Batteries: Basic Guidance, Opportunities, and Perspectives

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