Revealing the role of the cathode–electrolyte interface on solid-state batteries

Zahiri, Beniamin; Patra, Arghya; Kiggins, Chadd; Yong, Adrian Xiao Bin; Ertekin, Elif; Cook, John B.; Braun, Paul V.

doi:10.1038/s41563-021-01016-0

Cited by 144 publications

(102 citation statements)

References 51 publications

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“…(The ionic conductivity of these materials are reported separately [19] ). Further annealing at T>543 K resulted in the lower ion conductivity tetragonal phase of NPS.…”

Section: Methods and Samplesmentioning

confidence: 99%

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Good Solid‐State Electrolytes Have Low, Glass‐Like Thermal Conductivity

Cheng

Chen

et al. 2021

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Lithium-ion batteries (LIBs) are widely used for electrical energy storage. The kinetics of charge transport, intercalation, and chemical reactions [1,2] in LIBs are strongly dependent on temperature. These processes, in turn, control cell round-trip efficiency and cycle life. For example, side reactions that irreversibly consume Li ions, for example, electrolyte decomposition, are accelerated at high temperatures. Furthermore, exposure of a battery to elevated temperatures, while beneficial for fast charging, leads to significant safety risks due to the potential for electrolyte decomposition, oxygen release by cathode materials, and if heat cannot be removed at an appropriate rate, thermal runaway. Greater understanding of the thermal properties of battery materials will facilitate advances in the engineering design and thermal management of LIBs is needed to improve safety and performance.The thermal properties of materials used in liquid-electrolyte-based batteries were summarized by Kantharaj et al. at both the device and material levels. [2] An additional level of complexity is created by the fact that the thermal conductivity of cathodes and anodes are known to depend on the state of charge, for example, the thermal conductivities of LiCoO 2 and graphite depend on Li composition. [3] From the cell assembly perspective, interfaces play a significant role in heat transfer. [4] For example, Lubner et al. characterized thermal resistances in a pouch-cell and showed that the thermal resistance of the separator-electrode interfaces accounts for up to 65% of the total thermal resistance within the cell. [4] Solid-state batteries (SSBs) are under intense investigation as safer, more robust, and higher energy-density alternatives to liquid-electrolyte-based LIBs. Similar to their liquidelectrolyte-based counterparts, SSBs also require thermal management strategies for dissipation of heat, especially in large, high-energy cell stacks. [2,5,6] If lithium metal is used as the SSB anode, which is highly attractive due to lithium's low reduction potential (−3.04 V vs standard-hydrogen-electrode) and high specific capacity (3860 mAh g −1 ), [7] temperature control becomes particularly important, as control of internal temperature distributions enhances the homogeneity of Li deposition and suppresses the formation of dendrites. [6] In Thermal management in Li-ion batteries is critical for their safety, reliability, and performance. Understanding the thermal conductivity of the battery materials is crucial for controlling the temperature and temperature distribution in batteries. This work provides systemic quantitative measurements of the thermal conductivity of three important classes of solid electrolytes (SEs) over the temperature range 150 < T < 350 K. Studies include the oxides

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“…(The ionic conductivity of these materials are reported separately [19] ). Further annealing at T>543 K resulted in the lower ion conductivity tetragonal phase of NPS.…”

Section: Methods and Samplesmentioning

confidence: 99%

“…Milling times of 1-4 h were studied and a 2-h milling period was selected. The final highly conductive phase (cubic-NPS) was achieved after 2 h of annealing at 543 K under Ar (The ionic conductivity of these materials were reported separately [19] ). Further annealing at T > 543 K resulted in the lower ion conductivity tetragonal phase of NPS.…”

Section: Samplesmentioning

confidence: 99%

Good Solid‐State Electrolytes Have Low, Glass‐Like Thermal Conductivity

Cheng

Chen

et al. 2021

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“…The batteries with (104)oriented NCM thin film exhibited higher interface resistances than those of (001)-exhibited NCM thin film, suggesting the importance of the crystallographic presentation of SEs and CAMs on interfacial diffusion kinetics. To further prove the effect in larger format SSBs concepts, Zahiri et al prepared a series of highly crystallographically oriented, crystalline, thick, and dense alkali ion TM oxide cathodes contacted with various SEs to comprehensively study the role that crystallography and interface morphology plays in the performance of SSBs [81]. As expected, a direct effect of interfacial crystallography on SSBs performance is shown by the linear correlation between interfacial ion transport and capacity fade.…”

Section: Microscopic Scalesmentioning

confidence: 98%

“…Structural inhomogeneities inside the composite cathode ranging from nanometer to micrometer scales can often dominate the ionic conductivity [37]. The prime example is the influence of interface crystallographic orientation between SEs and CAMs [78,80,81]. In composite cathodes, CAM and SE often possess different crystal structures, which usually causes the mismatch of interfaces, further seriously blocking the transportation of Li + at the interface, especially for CAMs with high specific surface area.…”

Section: Microscopic Scalesmentioning

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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“…19–22 The SPEs can have flexible contact with the positive and negative electrodes, but their high crystallinity at room temperature leads to low ionic conductivity. 23–25 Due to the Lewis acid–base effect between fillers and polymers, the fillers not only reduce the crystallinity and increase the ionic conductivity, but also improve the mechanical properties and safety properties. 26,27 Therefore, CSEs are one of the most promising solid electrolytes.…”

Section: Introductionmentioning

confidence: 99%

Hydrogen bonding enhanced SiO₂/PEO composite electrolytes for solid-state lithium batteries

et al. 2022

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Revealing the role of the cathode–electrolyte interface on solid-state batteries

Cited by 144 publications

References 51 publications

Good Solid‐State Electrolytes Have Low, Glass‐Like Thermal Conductivity

Good Solid‐State Electrolytes Have Low, Glass‐Like Thermal Conductivity

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

Hydrogen bonding enhanced SiO₂/PEO composite electrolytes for solid-state lithium batteries

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Revealing the role of the cathode–electrolyte interface on solid-state batteries

Cited by 144 publications

References 51 publications

Good Solid‐State Electrolytes Have Low, Glass‐Like Thermal Conductivity

Good Solid‐State Electrolytes Have Low, Glass‐Like Thermal Conductivity

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

Hydrogen bonding enhanced SiO2/PEO composite electrolytes for solid-state lithium batteries

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Hydrogen bonding enhanced SiO₂/PEO composite electrolytes for solid-state lithium batteries