Yi Duan,Xiaopeng Qi,Xiangtao Bai,Tianwei Yu,Yanlong Wu,Zenghua Chang,Jiantao Wang
Argyrodite Li 6-x PS 5-x Cl 1+x with high ionic conductivity and excellent mechanical performance is an attractive solid electrolyte candidate for all-solid-state lithium batteries (ASSLBs). Adjusting Cl content is an effective strategy to enhance the ionic conductivity, however its effect on the thermal stability remain uncovered. Herein, our study shows that the increase of Cl content in Li 6-x PS 5-x Cl 1+x significantly enhances the ionic conductivity and electrochemical properties but significantly reduces its thermal stability. We reveal that the thermal stability of Li 6-x PS 5-x Cl 1+x is heavily dependent on its Cl content and can be significantly enhanced by elemental doping. LiNi 0.6 Co 0.2 Mn 0.2 O 2 based ASSLBs using Cl-rich argyrodite with pure phase shows better cycle performance. Achievements from this study could serve as a guidance for optimizing and applicating argyrodite solid electrolytes towards high-performance and safe ASSLBs.
Graphical Bi−F dual-doped Li 5.5 PS 4.5 Cl 1.5 electrolyte is synthesized and exhibits significant compatibility for bare lithium metal, directs uniform Li + deposition/stripping by forming a Li−Bi alloy, and forms a robust LiF phase to inhibit the growth of lithium dendrites. In addition, the formation of BiS 4 ⁵ − unit and LiBiS 2 phase gives it a high air/moisture resistance. Chlorine-rich lithium argyrodite is considered as a promising superionic conductor electrolyte, but its practical application is limited due to poor air stability and instability toward lithium metal. In this work, BiF 3 is proposed as a multi-functional dopant for electrolyte modification, and the effects on the ionic conductivity, air stability, critical current density, and electrolyte/Li metal interfacial stability are studied. The results show that the doped electrolyte Li 5.54 P 0.98 Bi 0.02 S 4.5 Cl 1.44 F 0.06 (LPBiSClF 0.06 ) still maintains a relatively high ionic conductivity of 5.37 mS cm −1 . Additionally, the formation of BiS 4 5− unit and LiBiS 2 phase provides high air/moisture resistibility. Meanwhile, the critical current density of the Li/LPBiSClF 0.06 /Li cell is increased two-fold (2.1 mA cm −2 ). The in-situ formation of LiF and Li−Bi alloy at the lithium metal/electrolyte interface plays a key role in achieving high performance. As a result, the assembled LCO@LNO/LPBiSClF 0.06 /Li battery retains 78.4 % of its capacity after 100 cycles at 0.2C.
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