Three types of inorganic electrolytes [Li 10 GeP 2 S 12 (LGPS), 75Li 2 S·24P 2 S 5 ·1P 2 O 5 (LPOS), Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 (LAGP)] with different particle sizes and electrochemical properties are selected as active fillers incorporated into poly(ethylene oxide) (PEO) matrix to fabricate hybrid solid electrolytes. The optimum composition of each filler is found in consideration of ionic conductivity. Their electrochemical characteristics are investigated. The optimal conductivities are 1.60 × 10 −5 , 1.18 × 10 −5 , and 2.12 × 10 −5 S cm −1 at room temperature for PEO-1%LGPS, PEO-1%LPOS, and PEO-20%LAGP, respectively. The electrochemical stability windows of these hybrid solid electrolytes are all above 5 V (vs. Li + /Li). The results show that these fillers have positive effects on the ionic conductivity, lithium ion transference number, and electrochemical stability. The relationship between the type of filler and electrochemical properties has been investigated. All-solid-state cells LiFePO 4 /Li are fabricated and present fascinating electrochemical performance with high capacity retention and good cycling stability. This work provides promising electrolytes prepared by a simple method.
Composite polymer-ceramic electrolytes have shown considerable potential for high-energy-density Li-metal batteries as they combine the benefits of both polymers and ceramics. However, low ionic conductivity and poor contact with electrodes limit their practical usage. In this study, a highly conductive and stable composite electrolyte with a high ceramic loading is developed for high-energy-density Li-metal batteries. The electrolyte, produced through in situ polymerization and composed of a polymer called poly-1,3-dioxolane in a poly(vinylidene fluoride)/ceramic matrix, exhibits excellent room-temperature ionic conductivity of 1.2 mS cm −1 and high stability with Li metal over 1500 h. When tested in a Li|electrolyte|LiFePO 4 battery, the electrolyte delivers excellent cycling performance and rate capability at room temperature, with a discharge capacity of 137 mAh g −1 over 500 cycles at 1 C. Furthermore, the electrolyte not only exhibits a high Li + transference number of 0.76 but also significantly lowers contact resistance (from 157.8 to 2.1 Ω) relative to electrodes. When used in a battery with a high-voltage LiNi 0.8 Mn 0.1 Co 0.1 O 2 cathode, a discharge capacity of 140 mAh g −1 is achieved. These results show the potential of composite polymer-ceramic electrolytes in room-temperature solid-state Li-metal batteries and provide a strategy for designing highly conductive polymer-in-ceramic electrolytes with electrode-compatible interfaces.
Xunzhi Miao,Jianhe Hong,Shuo Huang,Liye Ding,Fang Wang,Min Liu,Quanquan Zhang,Hongyun Jin
All-solid-state lithium batteries (ASSLBs) are highly promising as next-generation energy storage devices owing to their potential for great safety and high energy density. This work demonstrates that composite solid polymer electrolyte with vertically-aligned card-house structure can simultaneously improve the high rate and long-term cycling performance of ASSLBs. The vertical alignment of laponite nanosheets creates fast and uniform Li + ion transport channels at the nanosheets/polymer interphase, resulting in high ionic conductivity of 8.9 × 10 −4 S cm −1 and Li + transference number of 0.32 at 60 °C, as well as uniformly distributed solid electrolyte interphase. Such electrolyte is characterized by high mechanical strength, low flammability, excellent structural stability and stable ion transport channels. In addition, the ASSLB cell with the electrolyte and LiFePO 4 cathode delivers a high discharge specific capacity of 124.8 mAh g −1 , which accounts for 85.6% of its initial capacity after 500 cycles at 1C. The reasonable design through structural control strategy by interconnecting the vertically-aligned nanosheets open a way to fabricate high performance composite solid polymer electrolytes.