Li10Ge(P1-xSbx)2S12 Lithium-Ion Conductors with Enhanced Atmospheric Stability

被引:163
作者
Liang, Jianwen [1 ]
Chen, Ning [2 ]
Li, Xiaona [1 ]
Li, Xia [1 ]
Adair, Keegan R. [1 ]
Li, Junjie [1 ]
Wang, Changhong [1 ]
Yu, Chuang [1 ]
Banis, Mohammad Norouzi [1 ]
Zhang, Li [3 ]
Zhao, Shangqian [3 ]
Lu, Shigang [3 ]
Huang, Huan [4 ]
Li, Ruying [1 ]
Huang, Yining [5 ]
Sun, Xueliang [1 ]
机构
[1] Univ Western Ontario, Dept Mech & Mat Engn, London, ON N6A 5B9, Canada
[2] Canadian Light Source, Saskatoon, SK S7N 2V3, Canada
[3] China Automot Battery Res Inst Co Ltd, Beijing 100088, Peoples R China
[4] Glabat Solid State Battery Inc, London, ON N6G 4X8, Canada
[5] Univ Western Ontario, Dept Chem, London, ON N6A 3K7, Canada
基金
加拿大自然科学与工程研究理事会; 加拿大创新基金会;
关键词
SOLID-STATE ELECTROLYTES; SUPERIONIC CONDUCTOR; NA3SBS4; GLASS;
D O I
10.1021/acs.chemmater.9b04764
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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.
引用
收藏
页码:2664 / 2672
页数:9
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