Understanding interface stability in solid-state batteries

Xiao, Yihan; Wang, Yan; Bo, Shou‐Hang; Kim, Jae Chul; Miara, Lincoln J.; Ceder, Gerbrand

doi:10.1038/s41578-019-0157-5

Cited by 735 publications

(683 citation statements)

References 248 publications

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“…For the topic of SEs, major parts of alkali ionic conductor include organic, inorganic, and composite polymer electrolyte have been introduced in detail; [ 5–7 ] for alkali metal anodes, many challenges like safety, especially alkali metal dendrites, have been deeply explored; [ 8,9 ] for the interface issues, the problems and solutions of anodic and cathodic interfaces have been investigated systematically. [ 10–12 ] From these works, the application prospect of ASSBs has been restricted by some critical problems: 1) large resistance caused by poor contact and space charge layer generated in the interface inside the ASSBs; 2) the cell failure due to alkali metal dendrite growth; 3) poor interface stability between electrode and solid electrolyte (SE), which leads to inferior cycle performance of ASSBs. [ 1,13–16 ] Thus, the interface dominates the performance of ASSBs.…”

Section: Introductionmentioning

confidence: 99%

Advanced Characterization Techniques for Interface in All‐Solid‐State Batteries

Gao

et al. 2020

Small Methods

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The interface is a critical factor of electrochemical performance for all‐solid‐state batteries (ASSBs). Comprehending the composition, structure, morphology, and their evolution in the interface during charge/discharge cycling is greatly important for the development and practical application of ASSBs. The characterization techniques are very crucial and powerful for investigating the interface properties of ASSBs. This review briefly describes how the interface is generated in ASSBs, and then emphatically summarizes some important advanced techniques used to characterize the interface in ASSBs. The principle, advantage, and application of the techniques in the interface investigation are systematically discussed. This review provides fundamental insights and perspectives for developing the characterization techniques to deeply understand the interfacial behaviors of ASSBs, which is valuable for accelerating the commercialization of ASSBs used in electronic devices, electric vehicles, and large‐scale energy storage.

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Section: Introductionmentioning

confidence: 99%

Advanced Characterization Techniques for Interface in All‐Solid‐State Batteries

Gao

et al. 2020

Small Methods

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“…[1] Despite the successful implementation of LIBs in portable electronics, proliferation of Li + -based energy storage SEs results in decomposition of the SE at both the anode and cathode surfaces. [13][14][15][16][17][18] While progress has been made in the implementation of low voltage cathodes, the reductive instability of LGPS at lithium anodes remains a considerable issue. Previous investigations of the LGPS/Li 0 interface have identified Li 2 S, Li 3 P, Li-Ge alloys, and other PS and SS containing species as some of the most common reductive decomposition products formed during lithium plating.…”

Section: Introductionmentioning

confidence: 99%

Direct Observation of Interfacial Mechanical Failure in Thiophosphate Solid Electrolytes with Operando X‐Ray Tomography

Madsen

Bassett

et al. 2020

Adv Materials Inter

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at larger scales (electric vehicle or gridscale energy storage) has been hampered by insufficient energy densities, prohibitive material costs, and safety concerns. [2] While significant progress has been made in the development of high energy density battery materials, the implementation of these materials in practical systems without sacrificing cell longevity or safety remains a pressing scientific challenge. One of the best studied approaches to improve the energy density of LIBs is to replace existing graphitic anodes (372 mA h g −1 capacity) with metallic lithium (3860 mA h g −1 capacity). [3] Unfortunately, uneven lithium plating and stripping in conventional organic liquid electrolytes promotes the growth of lithium dendrites, accelerating the formation of internal short-circuits. Additionally, the low thermal stability of electrolyte solvents (often mixtures of cyclic and linear carbonates) incurs exothermic decomposition of the electrolyte in the event of cell failure, often resulting in catastrophic thermal runaway. [4-6] While many approaches have been explored to address these issues, one of the most promising options is the elimination of the liquid electrolyte in favor of a solid electrolyte. [7] Transitioning from conventional liquid electrolytes to Li +conducting solid electrolytes (SEs) presents two primary advantages. The high mechanical rigidity of inorganic SEs may act to suppress the formation of dendrites at lithium anodes, reducing the possibility of internal short circuits. [8] Additionally, the negligible flammability of most SEs dramatically lowers the risk of uncontrolled thermal runaway in the event of cell failure. [9,10] These potential benefits motivate the search for materials with sufficiently high ionic conductivities to serve as replacements for their liquid counterparts. Among the known SE formulations, the thiophosphate class of superionic conductors exhibit exceptionally fast lithium transport at room temperature. [11] Specifically, Li 10 GeP 2 S 12 (LGPS) demonstrates an ionic conductivity of ≈10 mS cm −1 , comparable to conductivities achievable in conventional liquid electrolytes. [12] Despite the favorable ionic conductivity of LGPS, its poor chemical and electrochemical stabilities remain key challenges for practical application. The narrow window of electrochemical stability of LGPS and many other thiophosphate

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“…However, almost all thiophosphate electrolytes are stable only in a narrow voltage window and likely decompose if combined with the Li metal anode, as stated by thermodynamics (Richards et al, 2016 ; Zhu et al, 2016 ). Their decomposition products often include metallic phases that induce the continuous growth of a decomposition layer (Xiao et al, 2020 ). Indeed, continuous formation of Li 2 S, Li 3 P, and Li 15 Ge 4 alloy (or Ge metal) is observed at the interface between Li 10 GeP 2 S 12 and Li metal (Wenzel et al, 2016 ).…”

Section: Introductionmentioning

confidence: 99%

“…Indeed, continuous formation of Li 2 S, Li 3 P, and Li 15 Ge 4 alloy (or Ge metal) is observed at the interface between Li 10 GeP 2 S 12 and Li metal (Wenzel et al, 2016 ). Alternatively, the solid electrolyte-Li metal anode interface can be kinetically stabilized if the decomposition reaction leads to electronically insulating phases (Xiao et al, 2020 ). For Li 7 P 3 S 11 , decomposed Li 2 S and Li 3 P intrinsically passivate the Li 7 P 3 S 11 -Li metal interface with a self-limited thickness, affording sustained electrolyte function at the expense of cell polarization (Wenzel et al, 2016 , 2018 ).…”

Section: Introductionmentioning

confidence: 99%

“…Here, we investigate the electrochemical properties of antiperovskite lithium oxychloride with the nominal target composition Li 3 OCl as a passivation material to protect the solid electrolyte-Li metal interface. This material consists of no reduceable cations other than Li, making it electrochemically stable against Li metal (Xiao et al, 2020 ). Computational predictions and experimental evidence show that Li 3 OCl indeed forms stable interfaces against Li (Lü et al, 2016 ; Richards et al, 2016 ).…”

Section: Introductionmentioning

confidence: 99%

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Lithium and Chlorine-Rich Preparation of Mechanochemically Activated Antiperovskite Composites for Solid-State Batteries

et al. 2020

Self Cite

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Assembling all-solid-state batteries presents a unique challenge due to chemical and electrochemical complexities of interfaces between a solid electrolyte and electrodes. While the interface stability is dictated by thermodynamics, making use of passivation materials often delays interfacial degradation and extends the cycle life of all-solid cells. In this work, we investigated antiperovskite lithium oxychloride, Li 3 OCl, as a promising passivation material that can engineer the properties of solid electrolyte-Li metal interfaces. Our experiment to obtain stoichiometric Li 3 OCl focuses on how the starting ratios of lithium and chlorine and mechanochemical activation affect the phase stability. For substantial LiCl excess conditions, the antiperovskite phase was found to form by simple melt-quenching and subsequent high-energy ball-milling. Li 3 OCl prepared with 100% excess LiCl exhibits ionic conductivity of 3.2 × 10 −5 S cm −1 at room temperature, as well as cathodic stability against Li metal upon the extended number of cycling. With a conductivity comparable to other passivation layers, and stable interface properties, our Li 3 OCl/LiCl composite has the potential to stably passivate the solid-solid interfaces in all-solid-state batteries.

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Understanding interface stability in solid-state batteries

Cited by 735 publications

References 248 publications

Advanced Characterization Techniques for Interface in All‐Solid‐State Batteries

Advanced Characterization Techniques for Interface in All‐Solid‐State Batteries

Direct Observation of Interfacial Mechanical Failure in Thiophosphate Solid Electrolytes with Operando X‐Ray Tomography

Lithium and Chlorine-Rich Preparation of Mechanochemically Activated Antiperovskite Composites for Solid-State Batteries

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