Lithium Ytterbium-Based Halide Solid Electrolytes for High Voltage All-Solid-State Batteries
All-solid-state Li-ion batteries that utilize nonflammable solid electrolytes are considered potential candidates for sustainable energy storage systems. Although sulfide solid electrolytes have been widely explored, their lack of electrochemical stability above 2.7 V requires the application of pro...
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| Published in | ACS materials letters Vol. 3; no. 7; pp. 930 - 938 |
|---|---|
| Main Authors | , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
American Chemical Society
05.07.2021
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| Online Access | Get full text |
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| Abstract | All-solid-state Li-ion batteries that utilize nonflammable solid electrolytes are considered potential candidates for sustainable energy storage systems. Although sulfide solid electrolytes have been widely explored, their lack of electrochemical stability above 2.7 V requires the application of protective coating layer on 4 V-class cathode materials, whereas the superior oxidative stability of chloride solid electrolytes enables their direct use with such high voltage cathodes. Here, we report a metastable trigonal phase of Li3YbCl6 with an ionic conductivity of 1.0 × 10–4 S·cm–1 and mixed-metal halide solid electrolytes, Li3–x Yb1–x Zr x Cl6, with conductivities up to 1.1 mS·cm–1 at room temperature. Combined neutron, single-crystal, and powder X-ray diffraction methods reveal that Zr-substitution for Yb in Li3YbCl6 triggers a trigonal-to-orthorhombic phase transition and forms new, lower energy pathways for Li-ion migration. All-solid-state cell cycling with uncoated >4 V-class cathodes is enabled by the high electrochemical oxidation stability of the mixed-metal halide solid electrolyte. |
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| AbstractList | All-solid-state Li-ion batteries that utilize nonflammable solid electrolytes are considered potential candidates for sustainable energy storage systems. Although sulfide solid electrolytes have been widely explored, their lack of electrochemical stability above 2.7 V requires the application of protective coating layer on 4 V-class cathode materials, whereas the superior oxidative stability of chloride solid electrolytes enables their direct use with such high voltage cathodes. Here, we report a metastable trigonal phase of Li3YbCl6 with an ionic conductivity of 1.0 × 10–4 S·cm–1 and mixed-metal halide solid electrolytes, Li3–x Yb1–x Zr x Cl6, with conductivities up to 1.1 mS·cm–1 at room temperature. Combined neutron, single-crystal, and powder X-ray diffraction methods reveal that Zr-substitution for Yb in Li3YbCl6 triggers a trigonal-to-orthorhombic phase transition and forms new, lower energy pathways for Li-ion migration. All-solid-state cell cycling with uncoated >4 V-class cathodes is enabled by the high electrochemical oxidation stability of the mixed-metal halide solid electrolyte. |
| Author | Assoud, Abdeljalil Nazar, Linda F Kim, Se Young Zhou, Laidong Liu, Jue Kaup, Kavish Park, Kern-Ho Wu, Xiaohan |
| AuthorAffiliation | Department of Chemistry and the Waterloo Institute for Nanotechnology Neutron Scattering Division |
| AuthorAffiliation_xml | – name: Department of Chemistry and the Waterloo Institute for Nanotechnology – name: Neutron Scattering Division |
| Author_xml | – sequence: 1 givenname: Se Young orcidid: 0000-0001-9188-868X surname: Kim fullname: Kim, Se Young organization: Department of Chemistry and the Waterloo Institute for Nanotechnology – sequence: 2 givenname: Kavish orcidid: 0000-0001-6201-2582 surname: Kaup fullname: Kaup, Kavish organization: Department of Chemistry and the Waterloo Institute for Nanotechnology – sequence: 3 givenname: Kern-Ho surname: Park fullname: Park, Kern-Ho organization: Department of Chemistry and the Waterloo Institute for Nanotechnology – sequence: 4 givenname: Abdeljalil surname: Assoud fullname: Assoud, Abdeljalil organization: Department of Chemistry and the Waterloo Institute for Nanotechnology – sequence: 5 givenname: Laidong orcidid: 0000-0002-8556-3296 surname: Zhou fullname: Zhou, Laidong organization: Department of Chemistry and the Waterloo Institute for Nanotechnology – sequence: 6 givenname: Jue orcidid: 0000-0002-4453-910X surname: Liu fullname: Liu, Jue organization: Neutron Scattering Division – sequence: 7 givenname: Xiaohan surname: Wu fullname: Wu, Xiaohan – sequence: 8 givenname: Linda F orcidid: 0000-0002-3314-8197 surname: Nazar fullname: Nazar, Linda F email: lfnazar@uwaterloo.ca organization: Department of Chemistry and the Waterloo Institute for Nanotechnology |
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