Motif-Based Exploration of Halide Classes of Li5M10.5M20.5X8 Conductors Using the DFT Method : Toward High Li-Ion Conductivity and Improved Stability
The development of all-solid-state lithium-ion batteries (ASSLIBs) is highly dependent on solid-state electrolyte (SSEs) performance. However, current SSEs cannot satisfactorily meet the requirements for high interfacial stability and Li-ion conductivity, especially under high-voltage cycling conditions. To overcome the intractable problems, we theoretically develop the chemistry of structural units to build a series of MX6-unit mixed framework Li5M10.5M20.5X8 (total 184 halides) for use as SSEs and recommend six halide candidates that combine the (electro)chemical stability with a low Li-ion migration barrier. Among them, three Li5M10.5M20.5F8 compounds (M1 = Ca and Mg; M2 = Ti and Zr) exhibit expansive electrochemical windows with a high cathodic limit (6.3 V vs μLi) and three-dimensional Li diffusion associated with moderate Li-migration barriers. To discuss their stability and compatibility (and in turn as a reference for experiments), the energy above the convex hull, the electrochemical stability window, the predicted (electro)reaction products, and the calculated reaction energies of Li5M10.5M20.5X8 in combination with Li-metal and several cathodes are tabulated. We stress that the importance of the cation-mixed effect and specific moieties for the halide anion leads to a design principle for a halide class of Li-ion SSEs. We provide insight into selecting the optimal halide anion and cations and open a new avenue of broad compositional spaces for stable Li-ion SSEs.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2023 |
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| Erschienen: |
2023 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:15 |
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| Enthalten in: |
ACS applied materials & interfaces - 15(2023), 36 vom: 13. Sept., Seite 42481-42489 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Li, Zengzhu [VerfasserIn] |
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| Links: |
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| Themen: |
All-solid-state Li-ion batteries |
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| Anmerkungen: |
Date Revised 13.09.2023 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
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| doi: |
10.1021/acsami.3c06745 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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| PPN (Katalog-ID): |
NLM361490704 |
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| 245 | 1 | 0 | |a Motif-Based Exploration of Halide Classes of Li5M10.5M20.5X8 Conductors Using the DFT Method |b Toward High Li-Ion Conductivity and Improved Stability |
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| 500 | |a Date Revised 13.09.2023 | ||
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| 520 | |a The development of all-solid-state lithium-ion batteries (ASSLIBs) is highly dependent on solid-state electrolyte (SSEs) performance. However, current SSEs cannot satisfactorily meet the requirements for high interfacial stability and Li-ion conductivity, especially under high-voltage cycling conditions. To overcome the intractable problems, we theoretically develop the chemistry of structural units to build a series of MX6-unit mixed framework Li5M10.5M20.5X8 (total 184 halides) for use as SSEs and recommend six halide candidates that combine the (electro)chemical stability with a low Li-ion migration barrier. Among them, three Li5M10.5M20.5F8 compounds (M1 = Ca and Mg; M2 = Ti and Zr) exhibit expansive electrochemical windows with a high cathodic limit (6.3 V vs μLi) and three-dimensional Li diffusion associated with moderate Li-migration barriers. To discuss their stability and compatibility (and in turn as a reference for experiments), the energy above the convex hull, the electrochemical stability window, the predicted (electro)reaction products, and the calculated reaction energies of Li5M10.5M20.5X8 in combination with Li-metal and several cathodes are tabulated. We stress that the importance of the cation-mixed effect and specific moieties for the halide anion leads to a design principle for a halide class of Li-ion SSEs. We provide insight into selecting the optimal halide anion and cations and open a new avenue of broad compositional spaces for stable Li-ion SSEs | ||
| 650 | 4 | |a Journal Article | |
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| 650 | 4 | |a all-solid-state Li-ion batteries | |
| 650 | 4 | |a density functional theory | |
| 650 | 4 | |a electrochemical windows | |
| 650 | 4 | |a halide solid-state electrolytes | |
| 700 | 1 | |a Dong, Huafeng |e verfasserin |4 aut | |
| 700 | 1 | |a Zhang, Bingkai |e verfasserin |4 aut | |
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