Lithium solid-state batteries: State-of-the-art and challenges for materials, interfaces and processing

Boaretto, Nicola; Garbayo, Íñigo; Valiyaveettil-SobhanRaj, Sona; Quintela, Amaia; Li, Chunmei; Casas‐Cabanas, Montse; Aguesse, Frédéric

doi:10.1016/j.jpowsour.2021.229919

Cited by 103 publications

(89 citation statements)

References 460 publications

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“…The nanoparticles interact with the PEO chains, resulting in a decrease in the crystallinity of the PEO chains. And Al 2 O 3 as a high-stability and easily prepared passive filler can improve the conductivity and the mechanical strength of SPEs [32]. Molecular dynamics (MD) simulation is a powerful tool that can obtain insights into transport phenomena at the molecular level [33].…”

Section: Introductionmentioning

confidence: 99%

Lithium ion transport in solid polymer electrolyte filled with alumina nanoparticles

Wang

Fan

et al. 2022

Energy Adv.

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Section: Introductionmentioning

confidence: 99%

Lithium ion transport in solid polymer electrolyte filled with alumina nanoparticles

Wang

Fan

et al. 2022

Energy Adv.

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“…The chief idea in the ASSB concept is to combine Li-metal anode with a solid-state electrolyte (SSE) to increase the energy density while keeping optimal safety. Yet the actual performance of ASSBs is generally much lower than expected due to high interfacial resistance between the SSE and electrode materials, especially at high states of charge. − Such interfacial resistance arises from generalized decomposition reactions taking place during battery cycling, as revealed by first-principles thermodynamics. − In addition, the ionic conductivities of SSEs are at least an order of magnitude lower than that of typical nonaqueous liquid electrolytes. As a consequence of such sluggish ionic diffusion, large polarizations are induced and high working temperatures are required to mitigate the problem. − Progress in ASSB research therefore requires developing new SSEs with better ionic conductivities capable of forming stable Li/SSE interfaces.…”

Section: Introductionmentioning

confidence: 99%

Molecular-Level Insight into the Interfacial Reactivity and Ionic Conductivity of a Li-Argyrodite Li₆PS₅Cl Solid Electrolyte at Bare and Coated Li-Metal Anodes

Golov

Carrasco

2021

ACS Appl. Mater. Interfaces

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Sulfide glasses, with high room-temperature Li-ion conductivities, are a promising class of solid-state electrolytes for all-solid-state batteries. Yet, when in contact with Li metal, our current understanding of important interfacial phenomena such as electrolyte reduction and Li-ion transport is still quite limited, especially at the atomic scale. Here, using first-principles molecular dynamics simulations, we tackle these open questions head-on and examine key interfacial properties of Li-argyrodite Li6PS5Cl electrolyte at bare and coated Li-metal anodes. Specifically, we investigate the role of the interfacial composition and morphology in a number of Li-metal surfaces, including surfaces coated with thin films of Li2Sn5, MoS2, LiF, and Li3P. Our materials models are designed to gain insights into the early stages of interface formation and structural evolution. In addition, by employing a novel topological analysis of procrystal electron density distribution as applied to interfacial solid-state ionics, we thoroughly assess Li-ion conductivity through the investigated interfaces. Our results provide evidence of progressive breaking of P–S bonds in PS4 3– groups and eventual P–P recombination of intermediate species as the main reaction mechanisms of Li6PS5Cl reduction by Li metal. We also predict Li2Sn5 as the most suitable coating to partially prevent the electrolyte degradation while keeping a relatively low interfacial resistance. These findings shed light on the interface chemistry of sulfide-based electrolytes in contact with Li metal and pave the way for rationalizing further computational and experimental studies in the field.

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“…Solid-state batteries are heralded as a complimentary technology to the incumbent liquid-electrolyte-based energy storage devices, with potential applications ranging from avionics to electric automobiles. − Sodium-ion solid-state batteries are of particular interest given the potentially reduced material costs relative to lithium-based energy storage. , The processing of solid-state batteries has been identified as one of the most important obstacles standing between the laboratory and the market. − …”

Section: Introductionmentioning

confidence: 99%

Design and Sintering of All-Solid-State Composite Cathodes with Tunable Mixed Conduction Properties via the Cold Sintering Process

Grady

Fan

Ndayishimiye

et al. 2021

ACS Appl. Mater. Interfaces

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Electrodes for solid-state batteries require the conduction of both ions and electrons for extraction of the energy from the active material. In this study, we apply cold sintering to a model composite cathode system to study how low-temperature densification enables a degree of control over the mixed conducting properties of such systems. The model system contains the NASICON-structured Na3V2(PO4)3 (NVP) active material, NASICON-structured solid electrolyte (Na3Zr2Si2PO12, NZSP), and electron-conducting carbon nanofiber (CNF). Pellets of varying weight fractions of components were cold-sintered to greater than 90% of the theoretical density at 350–375 °C, a 360 MPa uniaxial pressure, and with a 3 h dwell time using sodium hydroxide as the transient sintering aid. The bulk conductivity of the diphasic composites was measured with impedance spectroscopy; the total conductivities of the composites are increased from 3.8 × 10–8 S·cm–1 (pure NVP) to 5.81 × 10–6 S·cm–1 (60 wt % NZSP) and 1.31 × 10–5 S·cm–1 (5 wt % CNF). Complimentary direct current polarization experiments demonstrate a rational modulation in transference number (τ) of the composites; τ of pure NVP = 0.966, 60 wt % NZSP = 0.995, and 5 wt % CNF = 0.116. Finally, all three materials are combined into triphasic composites to serve as solid-state cathodes in a half-cell configuration with a liquid electrolyte. Electrochemical activity of the active material is maintained, and the capacity/energy density is comparable to prior work.

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Lithium solid-state batteries: State-of-the-art and challenges for materials, interfaces and processing

Cited by 103 publications

References 460 publications

Lithium ion transport in solid polymer electrolyte filled with alumina nanoparticles

Lithium ion transport in solid polymer electrolyte filled with alumina nanoparticles

Molecular-Level Insight into the Interfacial Reactivity and Ionic Conductivity of a Li-Argyrodite Li₆PS₅Cl Solid Electrolyte at Bare and Coated Li-Metal Anodes

Design and Sintering of All-Solid-State Composite Cathodes with Tunable Mixed Conduction Properties via the Cold Sintering Process

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Lithium solid-state batteries: State-of-the-art and challenges for materials, interfaces and processing

Cited by 103 publications

References 460 publications

Lithium ion transport in solid polymer electrolyte filled with alumina nanoparticles

Lithium ion transport in solid polymer electrolyte filled with alumina nanoparticles

Molecular-Level Insight into the Interfacial Reactivity and Ionic Conductivity of a Li-Argyrodite Li6PS5Cl Solid Electrolyte at Bare and Coated Li-Metal Anodes

Design and Sintering of All-Solid-State Composite Cathodes with Tunable Mixed Conduction Properties via the Cold Sintering Process

Contact Info

Product

Resources

About

Molecular-Level Insight into the Interfacial Reactivity and Ionic Conductivity of a Li-Argyrodite Li₆PS₅Cl Solid Electrolyte at Bare and Coated Li-Metal Anodes