Journal
CHEMISTRY OF MATERIALS
Volume 32, Issue 6, Pages 2664-2672Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.9b04764
Keywords
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Funding
- Natural Sciences and Engineering Research Council of Canada (NSERC)
- GLABAT Solid-State Battery Inc.
- China Automotive Battery Research Institute Co. Ltd.
- Canada Research Chair Program (CRC)
- Canada Foundation for Innovation (CFI)
- Ontario Research Fund
- Canada Light Source at the University of Saskatchewan (CLS)
- Canada MITACS fellow
- University of Western Ontario
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Sulfide solid electrolytes have recently attracted significant interest for use in all-solid-state lithium batteries (ASSLBs) due to their high ionic conductivity. However, one of the main challenges associated with the commercialization of sulfide-based electrolytes is their instability toward air/moisture, which leads to complex processing requirements. Herein, we develop a strategy to not only increase ionic conductivity but also obtain high air stability of the Li10Ge(P1-xSbx)(2)S-12 electrolyte system with soft acid Sb substitution. Theoretical calculations predict the Sb substitution in (Ge,P)S-4 tetrahedral sites, which is further confirmed by the X-ray diffraction Rietveld refinement and synchrotron X-ray absorption fine structure analysis. Opened channels and increased unit cell volume are achieved with an appropriate amount of Sb substitution, leading to an ultrahigh ionic conductivity of 17.3 +/- 0.9 mS cm(-1). The softer acidity of Sb compared to that of P also ensures strong covalent bonding with S in Li10Ge(P1-xSbx)(2)S-12, which improves the air stability of the electrolyte. Moreover, the air-exposed samples exhibit high ionic conductivities of 12.1-15.7 mS cm(-1). Bulk-type ASSLBs assembled with either pristine or air-exposed Li10Ge(P1-xSbx)(2)S-12 exhibit high initial Coulombic efficiencies of 92.8 and 91.0%, respectively, with excellent cycling performances of over 110 cycles. The observed variations in the structural parameters and bond strengths provide an effective approach toward designing more ionically conductive and stable solid-state electrolytes.
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