Anion Engineering for Stabilizing Li Interstitial Sites in Halide Solid Electrolytes for All-Solid-State Li Batteries

Park, Kern-Ho; Kim, Se Young; Jung, Mina; Lee, Su-Bin; Kim, Min-Jeong; Yang, In-Jun; Hwang, Ji-Hoon; Cho, Woosuk; Chen, Guoying; Kim, KyungSu; Yu, Jisang

doi:10.1021/acsami.3c13002

Cited by 5 publications

(1 citation statement)

References 43 publications

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“…or Li 2 ZrCl 6 have gained popularity as catholytes owing to their favorable mechanical properties and excellent electrochemical oxidation stability. − However, their ionic conductivity does not (yet) surpass that of sulfides. Efforts are being made to enhance conductivity by investigating new compositions and structures through theoretical and experimental approaches. , Recent success has been achieved through the discovery of a few amorphous halides such as LiTaCl 6 , where the exact mechanism of high ionic conductivity is debatable. , …”

Section: Introductionmentioning

confidence: 99%

Critical Role of Framework Flexibility and Disorder in Driving High Ionic Conductivity in LiNbOCl₄

Singh,

Wang,

Liu

et al. 2024

J. Am. Chem. Soc.

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Section: Introductionmentioning

confidence: 99%

Critical Role of Framework Flexibility and Disorder in Driving High Ionic Conductivity in LiNbOCl₄

Singh,

Wang,

Liu

et al. 2024

J. Am. Chem. Soc.

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Enhanced Interfacial Conduction in Low‐Cost NaAlCl₄ Composite Solid Electrolyte for Solid‐State Sodium Batteries

Ruoff,

Kmiec,

Manthiram

2024

Advanced Energy Materials

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All‐solid‐state sodium batteries offer the advantage of both sustainability and safety. Solid‐state electrolytes play a key role, and an oxygen‐incorporated NaAlCl4 composite electrolyte is presented with a high ambient‐temperature ionic conductivity of > 0.1 mS cm−1. The electrolyte synthesized with a mechanochemical reaction consists of in situ‐formed Al2O3 nanoparticles that provide enhanced conduction through an oxychloride phase at the interface. Magic angle spinning nuclear magnetic resonance spectroscopy confirms the formation of Al2O3 and the oxychloride phases at the interface and sheds insights into the origin of the enhanced ionic conductivity of the composite electrolyte. Additionally, simply adding Al2O3 nanoparticles to NaAlCl4 before mechanochemical synthesis is investigated, and a relationship between Al2O3 surface area and composite electrolyte ionic conductivity is identified. All‐solid‐state sodium batteries assembled with the composite electrolyte demonstrate a high specific capacity of 124 mA h g−1, clearly outperforming the baseline NaAlCl4 electrolyte. Furthermore, X‐ray photoelectron spectroscopy is utilized to understand the origin of capacity fade and obtain insights into electrolyte decomposition products. This work provides a deeper understanding of methods for boosting the ion transport in a low‐cost halide solid electrolyte for practical viability of all‐solid‐state sodium batteries.

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Interfacial Challenges of Halide‐Based All‐Solid‐State Batteries

Tan,

Beltran,

et al. 2024

Advanced Energy Materials

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As the demand for high energy density and battery safety grows, all‐solid‐state batteries (ASSBs) have garnered considerable attention as promising energy storage systems by removing flammable liquid electrolytes (LEs). Cutting‐edge sulfide inorganic solid electrolytes (ISEs) such as Li10GeP2S12 and Li6PS5Cl have shown high Li+ conductivity comparable to those of LEs. However, the narrow electrochemical stability windows of sulfide ISEs hinder the development of high‐energy density ASSBs with severe interfacial challenges. Recently, halide ISEs such as Li3YCl6 and Li3InCl6 are attracting increasing attention because of their high Li+ ion conductivity, excellent thermal stability, and high oxidative stability above 4 V. These properties are crucial to developing ASSBs with high energy density, and exceptional cycle and rate performances when employing high‐voltage cathode materials. Nevertheless, recent studies have identified severe interfacial challenges in ASSBs utilizing halide ISEs. Moreover, the safety of ASSBs is assumed to be better than conventional LE batteries but studies find the opposite conclusion when certain types of ISEs are employed, which can be attributed to products from side reactions at the interfaces. The objective here is to summarize the interfacial challenges associated with halide ISEs‐based ASSBs that will guide the development of high‐performance and safe ASSBs.

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Anion Engineering for Stabilizing Li Interstitial Sites in Halide Solid Electrolytes for All-Solid-State Li Batteries

Cited by 5 publications

References 43 publications

Critical Role of Framework Flexibility and Disorder in Driving High Ionic Conductivity in LiNbOCl₄

Critical Role of Framework Flexibility and Disorder in Driving High Ionic Conductivity in LiNbOCl₄

Enhanced Interfacial Conduction in Low‐Cost NaAlCl₄ Composite Solid Electrolyte for Solid‐State Sodium Batteries

Interfacial Challenges of Halide‐Based All‐Solid‐State Batteries

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Anion Engineering for Stabilizing Li Interstitial Sites in Halide Solid Electrolytes for All-Solid-State Li Batteries

Cited by 5 publications

References 43 publications

Critical Role of Framework Flexibility and Disorder in Driving High Ionic Conductivity in LiNbOCl4

Critical Role of Framework Flexibility and Disorder in Driving High Ionic Conductivity in LiNbOCl4

Enhanced Interfacial Conduction in Low‐Cost NaAlCl4 Composite Solid Electrolyte for Solid‐State Sodium Batteries

Interfacial Challenges of Halide‐Based All‐Solid‐State Batteries

Contact Info

Product

Resources

About

Critical Role of Framework Flexibility and Disorder in Driving High Ionic Conductivity in LiNbOCl₄

Critical Role of Framework Flexibility and Disorder in Driving High Ionic Conductivity in LiNbOCl₄

Enhanced Interfacial Conduction in Low‐Cost NaAlCl₄ Composite Solid Electrolyte for Solid‐State Sodium Batteries