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Crystals · 2022 ·Vol. 12 ·期 9 ·1290 · IF 2.67

Non-Flammable Dual-Salt Deep Eutectic Electrolyte for High-Voltage Lithium Metal Battery

Wanbao Wu,Qing Li,Miaomiao Cao,Deping Li,Jingyu Lu,Mingyu Li,Jiaheng Zhang

The application of high voltage cathode electrode materials is an effective way to increase the energy density of batteries. However, the development and design of a stable electrolyte at high voltages needs to be further addressed. Herein, we developed a non-flammable dual-salt deep eutectic solvent (DES) as a safe electrolyte containing LiTFSI, LiDFOB, and succinonitrile in different molar ratios. This non-flammable DES provides high ionic conductivity (4.23 mS cm−1) at 25 °C, high Li+transference number (0.75), and wide electrochemical stability (>5.5 V). When using the designed DES electrolytes in high voltage LiCoO2||Li cells, superior electrochemical performance was achieved at cut-off voltages of 3.0–4.45 V and 3.0–4.6 V, even at a high current density of 2 C. This work offers an in-depth understanding of the critical role of dual-salts in DES and provides an approach to designing safe electrolytes for high voltage LiCoO2||Li cells.Keywords:non-flammable;high Li+transference number;deep eutectic solvent;high voltage LCO;lithium metal battery

研究领域: 材料科学 · 电化学
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Journal of Materials Chemistry A · 2025 · IF 9.5

Nonflammable single-solvent electrolyte towards highly stable Li-rich Mn-based cathode materials

Dongwei Zhou,Shihao Wang,Jiansen Wen,Jie Mei,Guiyang Gao,Saichao Li,Baisheng Sa,Jie Lin,Laisen Wang,Guoying Wei,Dong-Liang Peng,Qingshui Xie

Li-rich Mn-based cathode materials, single-solvent, nonflammable feature, high voltage stability, solvation structure

CAS / MDL: 156783-95-8
研究领域: 材料科学 · 电化学
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ACS Applied Materials & Interfaces · 2018 · IF 8.097

Binary Mixtures of Highly Concentrated Tetraglyme and Hydrofluoroether as a Stable and Nonflammable Electrolyte for Li–O2 Batteries

Qin Zhao,Yuhang Zhang,Guiru Sun,Lina Cong,Liqun Sun,Haiming Xie,Jia Liu

Developing a long-term stable electrolyte is one of the most enormous challenges for Li–O2 batteries. Equally, the high flammability of frequently used solvents seriously weakens the electrolyte safety in Li–O2 batteries, which inevitably restricts their commercial applications. Here, a binary mixture of highly concentrated tetraglyme electrolyte (HCG4) and 1,1,2,2-tetrafluoroethyl 2,2,3,3-tetrafluoropropyl ether (TTE) was used for a novel electrolyte (HCG4/TTE) in Li–O2 batteries, which exhibit good wettability, enhanced ionic conductivity, considerable nonflammability, and high electrochemical stability. Being a co-solvent, TTE can contribute to increasing ionic conductivity and to improving flame retardance of the as-prepared electrolyte. The cell with this novel electrolyte displays an enhanced cycling stability, resulting from the high electrochemical stability during cycling and the formation of electrochemically stable interfaces prevents parasitic reactions occurring on the Li anode. These results presented here demonstrate a novel electrolyte with a high electrochemical stability and considerable safety for Li–O2 batteries.

研究领域: 储能 · 电化学 · 材料科学 · 电池技术
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Energy & Environmental Materials · 2022 ·Vol. 6 ·期 4 ·e12568 · IF 13.443

A Self-Healing and Nonflammable Cross-Linked Network Polymer Electrolyte with the Combination of Hydrogen Bonds and Dynamic Disulfide Bonds for Lithium Metal Batteries

Kai Chen,Yuxue Sun,Xiaorong Zhang,Jun Liu,Haiming Xie

The self-healing solid polymer electrolytes (SHSPEs) can spontaneously eliminate mechanical damages or micro-cracks generated during the assembly or operation of lithium-ion batteries (LIBs), significantly improving cycling performance and extending service life of LIBs. Here, we report a novel cross-linked network SHSPE (PDDP) containing hydrogen bonds and dynamic disulfide bonds with excellent self-healing properties and non-flammability. The combination of hydrogen bonding between urea groups and the metathesis reaction of dynamic disulfide bonds endows PDDP with rapid self-healing capacity at 28 °C without external stimulation. Furthermore, the addition of 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (EMIMTFSI) improves the ionic conductivity (1.13 × 10 −4 S cm −1 at 28 °C) and non-flammability of PDDP. The assembled Li/PDDP/LiFePO 4 cell exhibits excellent cycling performance with a discharge capacity of 137 mA h g −1 after 300 cycles at 0.2 C. More importantly, the self-healed PDDP can recover almost the same ionic conductivity and cycling performance as the original PDDP.

研究领域: 材料科学 · 高分子化学 · 电化学 · 能源存储 · 功能材料
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

An improved N–N dimethylacetamide-based non-flammable molecular crowding electrolyte using NaOTf for cobalt-based prussian blue//hard carbon aqueous solution battery

Shuaishuai Li,Xudun Shen,Bowang Zhao,Longnian Tang,Yechen Qian,Wenyao Li,Shijie Li

Aqueous sodium-ion batteries (ASIBs) are promising for large-scale electrical energy storage (LSEES) applications due to their cost and safety advantages. However, the low voltage stabilization window of water (∼1.23 V) and the lack of cathode with high specific capacity and long cycle life have limited their development. Cobalt-based Prussian blue analogues (NaCoPBAs) have the advantage of high theoretical specific capacity but short cycle life. Recently, the molecular crowding electrolyte (MCE) strategy has been proposed to improve the electrolyte voltage stability window (ESW) of electrolytes, in this work, we report an improved xMC (x: ratio, MC: molecular crowding agent) electrolyte that uses N–N dimethylacetamide (DMAC) as the molecular crowding agent and NaOTf as the advanced salt with an ESW of 2.65 V and excellent nonflammability. The side reactions of the NaCoPBA//Hard Carbon (HC) full-cell active material are improved with the aid of the electrolyte. Capacity retention of 75 % after 600 cycles with excellent cycling stability. These results demonstrate that this advanced MCE strategy can be utilized for practical applications designed for safety, high specific capacity and long cycle (ASIB).

研究领域: 储能技术 · 电化学 · 材料科学 · 电池技术 · 化学工程
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ADVANCED MATERIALS · 2021 ·Vol. 33 ·期 42 ·2102134 · IF 30.849

Lithium Fluoride in Electrolyte for Stable and Safe Lithium-Metal Batteries

Yi-Hong Tan,Gong-Xun Lu,Jian-Hui Zheng,Fei Zhou,Mei Chen,Tao Ma,Lei-Lei Lu,Yong-Hui Song,Yong Guan,Junxiong Wang,Zheng Liang,Wen-Shan Xu,Yuegang Zhang,Xinyong Tao,Hong-Bin Yao

Electrolyte engineering via fluorinated additives is promising to improve cycling stability and safety of high-energy Li-metal batteries. Here, an electrolyte is reported in a porous lithium fluoride (LiF) strategy to enable efficient carbonate electrolyte engineering for stable and safe Li-metal batteries. Unlike traditionally engineered electrolytes, the prepared electrolyte in the porous LiF nanobox exhibits nonflammability and high electrochemical performance owing to strong interactions between the electrolyte solvent molecules and numerous exposed active LiF (111) crystal planes. Via cryogenic transmission electron microscopy and X-ray photoelectron spectroscopy depth analysis, it is revealed that the electrolyte in active porous LiF nanobox involves the formation of a high-fluorine-content (>30%) solid electrolyte interphase layer, which enables very stable Li-metal anode cycling over one thousand cycles under high current density (4 mA cm −2 ). More importantly, employing the porous LiF nanobox engineered electrolyte, a Li || LiNi 0.8 Co 0.1 Mn 0.1 O 2 pouch cell is achieved with a specific energy of 380 Wh kg −1 for stable cycling over 80 cycles, representing the excellent performance of the Li-metal pouch cell using practical carbonate electrolyte. This study provides a new electrolyte engineering strategy for stable and safe Li-metal batteries.

研究领域: 材料科学 · 电化学 · 储能 · 电池技术
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

High-Voltage and Intrinsically Safe Sodium Metal Batteries Enabled by Nonflammable Fluorinated Phosphate Electrolytes

Hui Li,Hui Chen,Xiaohui Shen,Xingwei Liu,Yongjin Fang,Faping Zhong,Xinping Ai,Hanxi Yang,Yuliang Cao

Sodium metal is a promising anode for high-energy-density sodium rechargeable batteries (RSBs). However, the low Coulombic efficiency (CE) of the Na plating/stripping process and the problem of safety hinder their practical application. Herein, we report a facile strategy for employing the fluorinated phosphate solvents to realize highly reversible Na plating/stripping and improve the safety performance. The fluorinated phosphate molecules reduce the polarity of the solvent and lower the coordination number to Na+, which makes it possible to form the anion-induced ion–solvent-coordinated (AI-ISC) structures with high reduction tolerance. Moreover, the fluorination treatment enhances the oxidation resistance of the phosphate solvent, enabling compatibility with the high-voltage Na3V2(PO4)2F3 (NVPF) cathode. As expected, the Na@Al//NVPF full cell with the as-prepared 0.9 M NaFSI/tris(2,2,2-trifluoroethyl) phosphate (TFEP) demonstrates a capacity retention of 83.4% after 200 cycles with an average CE of 99.6%. This work opens a new avenue for designing high-energy-density RSBs with improved safety performance.

CAS / MDL: 78-40-0 67605-68-9
研究领域: 材料科学 · 电化学 · 能量存储
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ACS Applied Materials & Interfaces · 2025 · IF 8.2

Quasi-Solid Electrolytes with Flexible Branches and Rigid Skeletons for High-Temperature Li Metal Batteries

Lanhua Ma,Jiwei Zhao,Mengjie Li,Hai Su,Yong Li,Yuansheng Liu,Hang Liu,Ewa Zygadło-Monikowska,Yunhua Xu

Quasi-solid electrolytes are poised to revolutionize the next generation of high-energy-density lithium metal batteries. However, they face considerable challenges in operating at high temperatures due to severe side reactions, particularly with high-voltage cathodes. Here, we fabricated a nonflammable quasi-solid electrolyte (QSE) using an in situ copolymerization method. This electrolyte features a copolymer host with both flexible branches and a rigid skeleton, along with fire-retardant fluorine- and phosphorus-based plasticizers. The flexible branches reduce crystallinity and facilitate lithium-ion migration, while the rigid skeleton provides excellent high-temperature stability. The optimized fluorine–phosphorus mixed plasticizer provides effective sequestration of highly reactive oxygen/hydroxide radicals, along with a wide electrochemical window (up to 4.7 V vs Li+/Li), thereby ensuring excellent interface stability and safety characteristics. Consequently, the resulting quasi-solid electrolyte demonstrates remarkable physicochemical and electrochemical properties, enabling highly reversible lithium plating-stripping processes and good compatibility with cathodes. Using the nonflammable QSE, a high capacity retention of 82.3% is achieved for LiFePO4 after 1000 cycles at a high current density of 5 C and 80 °C. The good compatibility with high-voltage cathodes was demonstrated by the stable cycling of LiCoO2 over 400 cycles at a high cutoff voltage of 4.5 V and an elevated temperature of 60 °C.

CAS / MDL: 78-67-1
研究领域: 材料科学 · 电化学 · 储能技术 · 锂离子电池 · 高分子化学
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