Direct Observation of a Li‐Ionic Space‐Charge Layer Formed at an Electrode/Solid‐Electrolyte Interface

Nomura, Yoshihiko; Yamamoto, Kazuo; Hirayama, Tsukasa; Ouchi, Satoru; Igaki, Emiko; Saitoh, Koh

doi:10.1002/ange.201814669

Cited by 28 publications

(29 citation statements)

References 28 publications

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“…It thus delivers a high capacity of 140 mAh g −1 and shows excellent cycling stability which retains 83% capacity after 200 cycles at 0.1 C. In comparison, the ASSB with a pristine cathode exhibits a capacity of 98 mAh g −1 and only delivers poor stability (22.4% capacity after 100 cycles at 0.1 C). Moreover, interposing coating layer is also an effective strategy to restrain the formation of space charge layer (SCL) to some extent, which is generally regarded as one of the reasons for the sluggish interfacial charge transport kinetics in SSBs [112,113]. Particularly, chemical potential coupling strategy via coating dielectric materials, such as BaTiO 3 nanoparticles, can establish the built-in electric field, greatly suppressing the SCL effect [114,115].…”

Section: Reconstructing Cam-se Interface Structure At Atomic Scalementioning

confidence: 99%

Multiscale understanding of high-energy cathodes in solid-state batteries: from atomic scale to macroscopic scale

et al. 2022

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In the crucial area of sustainable energy storage, solid-state batteries (SSBs) with nonflammable solid electrolytes stand out due to their potential benefits of enhanced safety, energy density, and cycle life. However, the complexity within the composite cathode determines that fabricating an ideal electrode needs to link chemistry (atomic scale), materials (microscopic/mesoscopic scale), and electrode system (macroscopic scale). Therefore, understiang solid-state composite cathodes covering multiple scales is of vital importance for the development of practical SSBs. In this review, the challenges and basic knowledge of composite cathodes from the atomic scale to the macroscopic scale in SSBs are outlined with a special focus on the interfacial structure, charge transport, and mechanical degradation. Based on these dilemmas, emerging strategies to design a high-performance composite cathode and advanced characterization techniques are summarized. Moreover, future perspectives toward composite cathodes are discussed, aiming to facilitate the develop energy-dense solid-state batteries.

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Section: Reconstructing Cam-se Interface Structure At Atomic Scalementioning

confidence: 99%

Multiscale understanding of high-energy cathodes in solid-state batteries: from atomic scale to macroscopic scale

et al. 2022

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“…However, the conclusions are contradictory and range from: i) layers of a few hundred nanometers thickness and significant impact [ 16,17 ] to ii) negligible impact and only a single nanometer thickness. [ 18,19 ]…”

Section: Introductionmentioning

confidence: 99%

Characterization and Quantification of Depletion and Accumulation Layers in Solid‐State Li⁺‐Conducting Electrolytes Using In Situ Spectroscopic Ellipsometry

et al. 2021

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The future of mobility depends on the development of next‐generation battery technologies, such as all‐solid‐state batteries. As the ionic conductivity of solid Li+‐conductors can, in some cases, approach that of liquid electrolytes, a significant remaining barrier faced by solid‐state electrolytes (SSEs) is the interface formed at the anode and cathode materials, with chemical instability and physical resistances arising. The physical properties of space charge layers (SCLs), a widely discussed phenomenon in SSEs, are still unclear. In this work, spectroscopic ellipsometry is used to characterize the accumulation and depletion layers. An optical model is developed to quantify their thicknesses and corresponding concentration changes. It is shown that the Li+‐depleted layer (≈190 nm at 1 V) is thinner than the accumulation layer (≈320 nm at 1 V) in a glassy lithium‐ion‐conducting glass ceramic electrolyte (a trademark of Ohara Corporation). The in situ approach combining electrochemistry and optics resolves the ambiguities around SCL formation. It opens up a wide field of optical measurements on SSEs, allowing various experimental studies in the future.

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“…The cycling and rate performance are, however, not satisfactory and should be improved. The capacityfading mechanism is unclear; it could result from oxidative degradation [45][46][47] or space charge layer formation at the interface of LGPS/NCM, [48,49] microcrack formation and/or surface degradation of the nickel-rich NCM cathode material. [50] In the LCBIM-cathode sheet, the oxidative side reaction of PEO can also degrade the interface in the cathode.…”

Section: Introductionmentioning

confidence: 99%

Sulfide‐Compatible Conductive and Adhesive Glue‐Like Interphase Engineering for Sheet‐Type All‐Solid‐State Battery

Cho

Park

Kim

et al. 2019

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An all‐solid‐state lithium battery based on a sulfide electrolyte is one of the most promising next‐generation energy storage systems. However, the high interfacial impedance, particularly due to the internal pores in the electrode or electrolyte layers, is the major limiting factor to the development of sheet‐type all‐solid‐state batteries. In this study, a low‐resistance integrated all‐solid composite electrode is developed using a hybrid of a pyrrolidinium‐based ionic liquid and a polyethylene oxide polymer with lithium salt as a multifunctional interphase material, which is engineered to be compatible with the sulfide electrolyte as well as the fabrication process of sheet‐type composite electrode. The interphase material fills the pore in the composite sheet while binding the components together, which effectively increases the interfacial contact area and strengthens the physical network between the components, thereby enabling enhanced ion transport throughout the electrode. The interphase‐engineered sheet‐type LiNi0.8Co0.1Mn0.1O2 /Li10GeP2S12 electrode shows a high reversible capacity of 166 mAh g−1 at 25 °C, corresponding to 92% of the observed capacity in a current liquid‐based cathode system, as well as enhanced cycle and rate performances. This study proposes a novel and practical method for the development of high‐performance sheet‐type all‐solid‐state lithium batteries.

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Direct Observation of a Li‐Ionic Space‐Charge Layer Formed at an Electrode/Solid‐Electrolyte Interface

Abstract: Supportinginformation and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.

Cited by 28 publications

References 28 publications

Multiscale understanding of high-energy cathodes in solid-state batteries: from atomic scale to macroscopic scale

Multiscale understanding of high-energy cathodes in solid-state batteries: from atomic scale to macroscopic scale

Characterization and Quantification of Depletion and Accumulation Layers in Solid‐State Li⁺‐Conducting Electrolytes Using In Situ Spectroscopic Ellipsometry

Sulfide‐Compatible Conductive and Adhesive Glue‐Like Interphase Engineering for Sheet‐Type All‐Solid‐State Battery

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Direct Observation of a Li‐Ionic Space‐Charge Layer Formed at an Electrode/Solid‐Electrolyte Interface

Abstract: Supportinginformation and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.

Cited by 28 publications

References 28 publications

Multiscale understanding of high-energy cathodes in solid-state batteries: from atomic scale to macroscopic scale

Multiscale understanding of high-energy cathodes in solid-state batteries: from atomic scale to macroscopic scale

Characterization and Quantification of Depletion and Accumulation Layers in Solid‐State Li+‐Conducting Electrolytes Using In Situ Spectroscopic Ellipsometry

Sulfide‐Compatible Conductive and Adhesive Glue‐Like Interphase Engineering for Sheet‐Type All‐Solid‐State Battery

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Product

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Characterization and Quantification of Depletion and Accumulation Layers in Solid‐State Li⁺‐Conducting Electrolytes Using In Situ Spectroscopic Ellipsometry