Probing electrical degradation of cathode materials for lithium-ion batteries with nanoscale resolution

Park, Sung Yong; Baek, Woon Joong; Lee, Seung Yeon; Seo, Jin Ah; Kang, Youn‐Bae; Koh, Meiten; Kim, Seong Heon

doi:10.1016/j.nanoen.2018.04.005

Cited by 52 publications

(35 citation statements)

References 23 publications

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“…[21][22][23][24] Even though the intergranular cracking can already be observed after only a few cycles, 11,16 the degree generally changes as a function of the cycle number, 18,25 the upper cutoff voltage, [26][27][28][29] operating temperature, 15 C-rate 30 and storage time. 31 Intergranular fracturing can result in reduced electrical contact of active material and, thus, increased electrical resistance, 18 and intensified side reactions, e.g., electrolyte decomposition and transition metal dissolution, 11,16,32 due to the increase in the exposed electrode surface area. These effects collectively expedite capacity fade and impedance rise in the cell.…”

Section: Introductionmentioning

confidence: 99%

Mesoscale Chemomechanical Interplay of the LiNi_0.8Co_0.15Al_0.05O₂ Cathode in Solid-State Polymer Batteries

et al. 2018

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Complex chemomechanical interplay exists over a wide range of length scales within the hierarchically structured lithium-ion battery. At the mesoscale, the interdependent structural complexity and chemical heterogeneity collectively govern the local chemistry and, as a result, critically influence the cell level performance. Here we investigate the morphology and state of charge (SOC) inhomogeneity within secondary NCA particles that were cycled in solid polymer batteries. We observe substantial inhomogeneity in the nickel oxidation state (a proxy for SOC) and loss of structural integrity within secondary particles after only 20 cycles due to significant intergranular cracking. The formation of mesoscale cracks causes loss of ionic and electrical contact within cathode particles, triggering increases in local impedance and rearrangement of transport pathways for charge carriers. This can eventually lead to deactivation of sub-particle level domains in solid-state lithium-ion batteries. Our findings highlight the importance of proper mesoscale strain and defect management in polymer lithium-ion batteries.

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Section: Introductionmentioning

confidence: 99%

Mesoscale Chemomechanical Interplay of the LiNi_0.8Co_0.15Al_0.05O₂ Cathode in Solid-State Polymer Batteries

et al. 2018

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“…Therefore, this SPM current measurements reveal the nanoscale electronic/ionic transportation properties and underline mechanism of SEI formation in a charging battery, providing new insights for understanding the conductivity polarization and CEI formation of cathode electrodes [11] . Similarly, the degradation studies by using post-mortem SSRM on Ar ion polished composite electrodes were also reported in Ref. [18] , which could also be realized by using BEXP +SSRM.…”

Section: Methods Validationmentioning

confidence: 74%

“…The post-mortem SPM conducted in a controlled environment is also becoming a powerful technique for battery degradation research [18] . For the commercial composite electrodes, during the repeated ion intercalation/deintercalation or after the long charge/discharge cycles, the insights into the internal structure and components evolutions is vitally important for better understanding their capacity fading mechanisms [19 , 20] .…”

Section: Methods Detailsmentioning

confidence: 99%

Complementary sample preparation strategies (PVD/BEXP) combining with multifunctional SPM for the characterizations of battery interfacial properties

et al. 2021

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The cathode/anode-electrolyte interfaces in lithium/sodium ion batteries act as the “gate” for the ion exchange between the solid electrode and liquid electrolyte. Understanding the interfacial properties of these solid-liquid interfaces is essential for better design high-performance lithium/sodium ion batteries. Here, we provide a novel method for studying solid-liquid interfacial properties of battery materials through combining physical vapor deposition (PVD) and beam-exit cross-sectional polishing (BEXP) followed by controlled environment multifunctional Scanning Probe Microscope (SPM). In this method, commercial battery materials can be either directly grown on the current collector substrates, or polished by obliqued Ar-ion beams to get a nanoscale flat surface which allows the multifunctional SPM to study sample directly in the liquid electrolyte or in protective oxygen/H 2 O free environment. This approach allows to investigate wide range of interfacial properties, including surface morphology, internal cracks, mechanical properties, electronic/ionic conductivity and surface potential, with nanoscale resolution in-operando during the battery cycles as well as post-mortem. PVD and novel BEXP methods were introduced to prepare battery powder materials as perfect specimens for nanoscale SPM characterization. Various physical/chemical properties of battery materials can be probed on the as-prepared specimens under liquid electrolyte using in situ/operando SPM techniques. Ex situ/post-mortem analyses based on the controlled environment multifunction SPM characterizations can be achieved in the BEXP polished degradation battery electrodes.

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“…Although scanning probe microscopy (SPM) can be used to directly investigate the electrical properties of composite electrodes [13][14][15][16][17] , it has not been applied to study bulk-type sul de ASSLBs because of challenges associated with handling sul de SEs in air. Masuda et al conducted operando Kelvin probe force microscopy (KPFM) on bulk-type oxide ASSLBs 18,19 .…”

Section: Introductionmentioning

confidence: 99%

“…Scanning spreading resistance microscopy (SSRM) and conductive-atomic force microscopy (C-AFM), which measure current and resistance distributions, respectively, are also based on SPM. These techniques have been used for investigating high-resistance areas to understand the degradation in electrode active materials 15,20 . Zhu et al 21 and Yang et al 22 used a C-AFM technique of measuring I-V characteristics to investigate Li-ion diffusion energy barriers related to charge-discharge reactions in electrode active materials.…”

Section: Introductionmentioning

confidence: 99%

Visualizing Local Electrical Properties of Composite Electrodes in Sulfide All-Solid-State Batteries by Scanning Probe Microscopy

Otoyama

Yamaoka

Ito

et al. 2020

Preprint

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Studies on local conduction paths in composite electrodes are essential to the realization of high-performance sulfide all-solid-state lithium batteries. Here, we directly evaluate the electrical properties of individual LiNi1/3Mn1/3Co1/3O2 (NMC) electrode active material particles in composite positive electrodes by scanning probe microscopy (SPM) techniques. Kelvin probe force microscopy (KPFM) and scanning spreading resistance microscopy (SSRM) were combined. The results indicated that all NMC particles exhibit a charged state with increasing potential, but low electronic conduction paths exist at point contacts of some NMC particles. Furthermore, the I-V characteristics measured by conductive-atomic force microscopy (C-AFM) suggest that these specific NMC particles show low charge-discharge reactivity. The results of the SPM techniques indicate that poor conduction locally limits the charge-discharge reactivity of electrode active materials, leading to the degradation of battery performance. Such SPM combination accelerates the morphological optimization of composite electrodes by facilitating the investigation of the intrinsic electrical properties of the electrodes.

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Probing electrical degradation of cathode materials for lithium-ion batteries with nanoscale resolution

Cited by 52 publications

References 23 publications

Mesoscale Chemomechanical Interplay of the LiNi_0.8Co_0.15Al_0.05O₂ Cathode in Solid-State Polymer Batteries

Mesoscale Chemomechanical Interplay of the LiNi_0.8Co_0.15Al_0.05O₂ Cathode in Solid-State Polymer Batteries

Complementary sample preparation strategies (PVD/BEXP) combining with multifunctional SPM for the characterizations of battery interfacial properties

Visualizing Local Electrical Properties of Composite Electrodes in Sulfide All-Solid-State Batteries by Scanning Probe Microscopy

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Probing electrical degradation of cathode materials for lithium-ion batteries with nanoscale resolution

Cited by 52 publications

References 23 publications

Mesoscale Chemomechanical Interplay of the LiNi0.8Co0.15Al0.05O2 Cathode in Solid-State Polymer Batteries

Mesoscale Chemomechanical Interplay of the LiNi0.8Co0.15Al0.05O2 Cathode in Solid-State Polymer Batteries

Complementary sample preparation strategies (PVD/BEXP) combining with multifunctional SPM for the characterizations of battery interfacial properties

Visualizing Local Electrical Properties of Composite Electrodes in Sulfide All-Solid-State Batteries by Scanning Probe Microscopy

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Mesoscale Chemomechanical Interplay of the LiNi_0.8Co_0.15Al_0.05O₂ Cathode in Solid-State Polymer Batteries

Mesoscale Chemomechanical Interplay of the LiNi_0.8Co_0.15Al_0.05O₂ Cathode in Solid-State Polymer Batteries