Cathode–Sulfide Solid Electrolyte Interfacial Instability: Challenges and Solutions

Brahmbhatt, Teerth; Yang, Guang; Self, Ethan C.; Nanda, Jagjit

doi:10.3389/fenrg.2020.570754

Cited by 17 publications

(19 citation statements)

References 72 publications

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“…Sang 85 When the sulfide electrolyte is in contact with oxide cathode materials, such as LiCoO 2 and nickel manganese cobalt (NMC), interfacial side reactions, large interfacial resistance, and elemental interdiffusion will lead to fast capacity degradation. 86 For example, it has been found that cobalt migrated from the LiCoO 2 cathode to the sulfide electrolyte after initial charging. 87 The main cause of the large interfacial resistance at the cathode/sulfide interface is the space charge layer, which arises from the Li-ion concentration difference between the oxide electrodes and the sulfide electrolyte.…”

Section: Sulfidesmentioning

confidence: 99%

“…When the sulfide electrolyte is in contact with oxide cathode materials, such as LiCoO 2 and nickel manganese cobalt (NMC), interfacial side reactions, large interfacial resistance, and elemental interdiffusion will lead to fast capacity degradation 86 . For example, it has been found that cobalt migrated from the LiCoO 2 cathode to the sulfide electrolyte after initial charging 87 .…”

Section: Ceramic Electrolytesmentioning

confidence: 99%

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Ionic conductivity and ion transport mechanisms of solid‐state lithium‐ion battery electrolytes: A review

Yang

2022

Energy Science & Engineering

207

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This review article deals with the ionic conductivity of solid-state electrolytes for lithium batteries. It has discussed the mechanisms of ion conduction in ceramics, polymers, and ceramic-polymer composite electrolytes. In ceramic electrolytes, ion transport is accomplished with mobile point defects in a crystal. Li + ions migrate mainly via the vacancy mechanism, interstitial mechanism, or interstitial-substitutional exchange mechanism. In solid polymer electrolytes, Li + ions are transported mainly via the segment motion, ion hopping (Grotthuss mechanism), or vehicle mechanism (mass diffusion). This study has also introduced various electrolyte materials including perovskite oxides, garnet oxides, sodium superionic conductors, phosphates, sulfides, halides, cross-linked polymers, block-copolymers, metal-organic frameworks, covalent organic frameworks, as well as ceramic-polymer composites. In addition, it has highlighted some strategies to improve the ionic conductivity of solid-state electrolytes, such as doping, defect engineering, microstructure tuning, and interface modification.

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Section: Sulfidesmentioning

confidence: 99%

Section: Ceramic Electrolytesmentioning

confidence: 99%

Ionic conductivity and ion transport mechanisms of solid‐state lithium‐ion battery electrolytes: A review

Yang

2022

Energy Science & Engineering

207

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“…[33][34][35][36] One key issue is the reactivity between the sulfides and both electrodes, which leads to an impedance rise associated with the formation of a mixed conducting interphase (MCI). [23,[37][38][39][40][41][42][43][44][45][46] The interface between the metal anode and the SE should be either thermodynamically stable or be passivated to be kinetically stable. Sulfide SEs are not thermodynamically stable at 0 V versus Li/Li + , forming either MCI or a (partially) kinetically stabilized solid electrolyte interphase (SEI).…”

Section: Introductionmentioning

confidence: 99%

Stable Anode‐Free All‐Solid‐State Lithium Battery through Tuned Metal Wetting on the Copper Current Collector

et al. 2022

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A stable anode‐free all‐solid‐state battery (AF‐ASSB) with sulfide‐based solid‐electrolyte (SE) (argyrodite Li6PS5Cl) is achieved by tuning wetting of lithium metal on “empty” copper current‐collector. Lithiophilic 1 µm Li2Te is synthesized by exposing the collector to tellurium vapor, followed by in situ Li activation during the first charge. The Li2Te significantly reduces the electrodeposition/electrodissolution overpotentials and improves Coulombic efficiency (CE). During continuous electrodeposition experiments using half‐cells (1 mA cm−2), the accumulated thickness of electrodeposited Li on Li2Te–Cu is more than 70 µm, which is the thickness of the Li foil counter‐electrode. Full AF‐ASSB with NMC811 cathode delivers an initial CE of 83% at 0.2C, with a cycling CE above 99%. Cryogenic focused ion beam (Cryo‐FIB) sectioning demonstrates uniform electrodeposited metal microstructure, with no signs of voids or dendrites at the collector‐SE interface. Electrodissolution is uniform and complete, with Li2Te remaining structurally stable and adherent. By contrast, an unmodified Cu current‐collector promotes inhomogeneous Li electrodeposition/electrodissolution, electrochemically inactive “dead metal,” dendrites that extend into SE, and thick non‐uniform solid electrolyte interphase (SEI) interspersed with pores. Density functional theory (DFT) and mesoscale calculations provide complementary insight regarding nucleation‐growth behavior. Unlike conventional liquid‐electrolyte metal batteries, the role of current collector/support lithiophilicity has not been explored for emerging AF‐ASSBs.

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“…While design and construction of solid-state composite cathodes have been dominant in SSB research (Figure a), it is necessary to critically evaluate the compatibility of this design approach with fast charging. At higher charging rates, chemo-mechanical challenges including interfacial delamination and particle cracking due to severe volume fluctuations of the active material need to be understood and addressed. − Therefore, the relative mechanical compliance of the active material and surrounding matrix of solid electrolyte must be considered under a range of volumetric strain conditions. This mechanical damage can potentially be mitigated by using single crystal cathode particles instead of polycrystalline materials .…”

Section: Challenges For Fast Charge Of Solid-state Batteriesmentioning

confidence: 99%

Challenges and Opportunities for Fast Charging of Solid-State Lithium Metal Batteries

et al. 2021

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In this Perspective, we assess the promise and challenges for solid-state batteries (SSBs) to operate under fast-charge conditions (e.g., <10 min charge). We present the limitations of state-of-the-art lithium-ion batteries (LIBs) and liquid-based lithium metal batteries in context, and highlight the distinct advantages offered by SSBs with respect to rate performance, thermal safety, and cell architecture. Despite the promising fast-charge attributes of SSBs, we must overcome fundamental challenges pertaining to electro-chemo-mechanics interaction, interface evolution, and transport-kinetics dichotomy to realize their implementation. We describe the mechanistic implications of critical features including plating-stripping crosstalk, metallic filament growth, cathode microstructure, and interphase formation on the fast-charge performance of SSBs. Toward achieving the eventual goal of fast-charge in SSBs, we highlight both intrinsic (e.g., interface design, transport properties) and extrinsic (e.g., temperature, pressure) design factors that can favorably modulate the mechanistic coupling and cross-correlations. Finally, a list of key research questions is identified that need to be answered to gain a deeper understanding of the fast-charge capabilities and requirements of SSBs.

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Cathode–Sulfide Solid Electrolyte Interfacial Instability: Challenges and Solutions

Cited by 17 publications

References 72 publications

Ionic conductivity and ion transport mechanisms of solid‐state lithium‐ion battery electrolytes: A review

Ionic conductivity and ion transport mechanisms of solid‐state lithium‐ion battery electrolytes: A review

Stable Anode‐Free All‐Solid‐State Lithium Battery through Tuned Metal Wetting on the Copper Current Collector

Challenges and Opportunities for Fast Charging of Solid-State Lithium Metal Batteries

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