A surfactant-assisted strategy to tailor Li-ion charge transfer interfacial resistance for scalable all-solid-state Li batteries

Zhou, Chengtian; Samson, Alfred Junio; Hofstetter, Kyle; Thangadurai, Venkataraman

doi:10.1039/c8se00234g

Cited by 53 publications

(36 citation statements)

References 41 publications

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“…R CT values in the present study are higher than the values reported for a SPS-processed garnet without alkaline earth ions − As reported by Sharafi, Li metal exhibits poorer wettability on Li 2 CO 3 surface than pristine garnet solid electrolyte . Although vacuum-deposited Li causes close contact on the pellets, Li 2 CO 3 domains on the pellets hinder the charge transfer on that region.…”

Section: Resultscontrasting

confidence: 67%

Microstructural and Electrochemical Properties of Alkaline Earth Metal-Doped Li Garnet-Type Solid Electrolytes Prepared by Solid-State Sintering and Spark Plasma Sintering Methods

Kammampata

Basappa

Ito

et al. 2019

ACS Appl. Energy Mater.

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Li-stuffed garnet-type solid Li-ion electrolytes have been considered as a promising candidate for all-solid-state Li batteries. In this work, alkaline earth metal-doped Li garnet-type solid Li-ion electrolytes, Li6.5La2.5A0.5TaZrO12 (A = Ca, Sr, Ba) were prepared by conventional solid-state sintering (CSS) and spark plasma sintering (SPS) methods. The effect of sintering methods on the structural and electrochemical properties of the solid electrolytes was investigated by powder X-ray diffraction (PXRD), scanning electron microscopy (SEM), and electrochemical impedance spectroscopy (EIS). Among the investigated compounds, Sr-doped garnet-type Li6.5La2.5Sr0.5TaZrO12 prepared by the SPS method showed the highest Li-ion conductivity of 3.08 × 10–4 S cm–1 at 20 °C and the lowest activation energy of 0.35 eV. Both Sr- and Ba-doped samples exhibited a critical current density of 0.15 mA cm–2, and the Sr-doped Li6.5La2.5Sr0.5TaZrO12 sample showed the lowest Li-ion charge-transfer resistance of 139 Ω cm2 at room temperature.

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Section: Resultscontrasting

confidence: 67%

Microstructural and Electrochemical Properties of Alkaline Earth Metal-Doped Li Garnet-Type Solid Electrolytes Prepared by Solid-State Sintering and Spark Plasma Sintering Methods

Kammampata

Basappa

Ito

et al. 2019

ACS Appl. Energy Mater.

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“…Benefiting from the enhanced lithiophilicity, the interfacial resistance between Li metal and LLZTO is significantly decreased. [29,30] As shown in Figure 2c, the symmetric Li/LLZTO/Li cell delivers a large resistance of 2046 Ω cm 2 , where the interfacial resistance between original LLZTO and Li metal is calculated to be 908 Ω cm 2 (see detailed calculation in the Supporting Information). [9] In contrast, the interfacial resistance of the symmetric Li/c * sCOF-modified LLZTO/Li cell (Li/c * sCOF@LLZTO/Li) is dramatically decreased to 99 Ω cm 2 .…”

Section: Resultsmentioning

confidence: 99%

Building Lithiophilic Ion‐Conduction Highways on Garnet‐Type Solid‐State Li⁺ Conductors

Cheng

Xie

Mao

et al. 2020

Advanced Energy Materials

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more stable interface against Li metal among SSEs. [3][4][5][6] The latter opens the door for safe use of Li metal anodes that have a high theoretical capacity (3860 mAh g −1 ) and a lowest electrochemical potential (−3.04 V vs standard hydrogen electrode), which is expected to maximize the energy-density advantage of SSLBs. [7] However, the large interfacial resistance between the rigid garnet solids and Li metal anodes is a huge challenge for fabricating high-performance SSLBs. [5,8] Although high-pressure treatment or vacuum evaporation have been used to deposit Li metal onto garnet solid to minimize the interfacial resistance, their complicated operations and procedures greatly limit the technological applications. Currently, melting Li metal integrated with garnet electrolytes, with the assistance of an intermediate layer between the garnet and Li metal, has been widely reported to overcome the lithiophobicity of garnet and consequently facilitated the interfacial resistance. [5] The intermediate layers mainly include Al 2 O 3 , Si, Au, Sn, ZnO, and polymers. [9][10][11][12][13][14] Although the interfacial resistance has been significantly decreased, numerous SSLBs reported to date are still unable to operate at high current densities (generally less than 0.5 mA cm −2 , see Table S1, Supporting Information), which would specifically inhibit the practical applications in power backups, portable power tools, or electric vehicles require much higher power densities. The poor power density of SSLBs is still neglected by battery community to date, at least, the current state-of-the-art interfacial modification strategies is a key bottleneck for the high-power SSLBs. The intermediate layers without sufficient ionic conductivity, such as Al 2 O 3 , ZnO, and polymers, may result in a unfavorable polarization resistance during operation under high current density, [9,15,16] while the other intermediate layers like Au and Sn are electronically conducting, [10,11,17] thus tending to result in Li penetration across the layer. And even worse, volume changes are inevitable when lithiating these inorganic layers with molten Li metal through the alloying-conversion reactions. [10] An ideal intermediate layer should, in principle, not only change the garnet from lithiophobic to lithiophilic, and also could be a fast and stable Li + conducting interphase when operating under high rate conditions.

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“…Much of this work, for example, has focused on stabilizing the interface between the solid electrolyte and lithium metal anodes through the use of artificial interlayers. Buffer layers have been incorporated through a variety of methods including liquid phase deposition 30,33,[41][42][43]47 , evaporation 32,33,39,40 , atomic layer deposition 34,34,48 , sputtering 35,38,49,50 , powder pressing 44 , and melt deposition 37 . Similar strategies have also been applied to improve the interface between cathode active material particles and various solid electrolytes.…”

Section: Introductionmentioning

confidence: 99%

Manufacturing scalability implications of materials choice in inorganic solid-state batteries

Huang

Ceder

Olivetti

2021

Joule

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The pursuit of scalable and manufacturable all-solid-state batteries continues to intensify, motivated by the rapidly increasing demand for safe, dense electrical energy storage. In this Perspective, we describe the numerous, often conflicting, implications of materials choices that have been made in the search for effective mitigations to the interfacial instabilities plaguing solid-state batteries. Specifically, we show that the manufacturing scalability of solid-state batteries can be governed by at least three principal consequences of materials selection: (1) the availability, scaling capacity, and price volatility of the chosen materials' constituents, (2) the manufacturing processes needed to integrate the chosen materials into full cells, and (3) the cell performance that may be practically achieved with the chosen materials and processes. While each of these factors is, in isolation, a pivotal determinant of manufacturing scalability, we show that consideration and optimization of their collective effects and tradeoffs is necessary to more completely chart a scalable pathway to manufacturing. Context & Scale With examples pulled from recent developments in solid-state batteries, we illustrate the consequences of materials choice on materials availability, processing requirements and challenges, and resultant device performance. We demonstrate that while each of these factors is, by itself, essential to understanding manufacturing scalability, joint consideration of all three provides for a more comprehensive understanding of the specific factors that could impede the scale up to production. Much of the recent activity in solidstate battery research has been aimed at mitigating the various interfacial instabilities that currently prevent the fabrication of a low cost, high performance device. With such a wide breadth of options, it can be difficult for researchers to identify the most promising or scalable pathways forward. As such, we aim to empower researchers to make more informed decisions by providing them with insights into how their materials choices are likely to impact the manufacturing scalability of different interfacial mitigation alternatives. In doing so, we hope that generalizable lessons about scalability can be extracted and applied to subsequent challenges in solid-state battery development, thereby accelerating their scale up to manufacturing.

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A surfactant-assisted strategy to tailor Li-ion charge transfer interfacial resistance for scalable all-solid-state Li batteries

Abstract: An economical and simple technique to mitigate the solid electrolyte–lithium metal anode interfacial charge transfer resistance.

Cited by 53 publications

References 41 publications

Microstructural and Electrochemical Properties of Alkaline Earth Metal-Doped Li Garnet-Type Solid Electrolytes Prepared by Solid-State Sintering and Spark Plasma Sintering Methods

Microstructural and Electrochemical Properties of Alkaline Earth Metal-Doped Li Garnet-Type Solid Electrolytes Prepared by Solid-State Sintering and Spark Plasma Sintering Methods

Building Lithiophilic Ion‐Conduction Highways on Garnet‐Type Solid‐State Li⁺ Conductors

Manufacturing scalability implications of materials choice in inorganic solid-state batteries

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A surfactant-assisted strategy to tailor Li-ion charge transfer interfacial resistance for scalable all-solid-state Li batteries

Abstract: An economical and simple technique to mitigate the solid electrolyte–lithium metal anode interfacial charge transfer resistance.

Cited by 53 publications

References 41 publications

Microstructural and Electrochemical Properties of Alkaline Earth Metal-Doped Li Garnet-Type Solid Electrolytes Prepared by Solid-State Sintering and Spark Plasma Sintering Methods

Microstructural and Electrochemical Properties of Alkaline Earth Metal-Doped Li Garnet-Type Solid Electrolytes Prepared by Solid-State Sintering and Spark Plasma Sintering Methods

Building Lithiophilic Ion‐Conduction Highways on Garnet‐Type Solid‐State Li+ Conductors

Manufacturing scalability implications of materials choice in inorganic solid-state batteries

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Building Lithiophilic Ion‐Conduction Highways on Garnet‐Type Solid‐State Li⁺ Conductors