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PEO–LiTFSI
CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

A highly ion-conductive three-dimensional LLZAO-PEO/LiTFSI solid electrolyte for high-performance solid-state batteries

Dan Cai,Donghuang Wang,Yongjie Chen,Shengzhao Zhang,Xiuli Wang,Xinhui Xia,Jiangping Tu

Composite solid electrolytes have recently attracted widespread attention due to their acceptable lithium-ion (Li-ion) conductivity and suitable flexibility. However, isolated ceramic particles in composite electrolyte cannot provide continuous fast Li-ion transport channels. And the non-uniformity caused by particle agglomeration usually leads to a decrease in the performance of the composite electrolyte. Here, we design a “polymer in ceramic” composite electrolyte that combines three-dimensional Li 6.4 La 3 Zr 2 Al 0.2 O 12 (3D LLZAO) framework with polyethylene oxide (PEO)/LiTFSI (T-LAPL) via a template and solution method. In addition to the significantly enhanced Li-ion conductivity (2.51 × 10 −4 S cm −1 at room temperature) and the high Li-ion transference number (t Li+  = 0.53), the T-LAPL composite electrolyte also exhibits improved thermal and electrochemical stability. Both symmetrical Li/T-LAPL/Li cells and LiFePO 4 /T-LAPL/Li cells display excellent electrochemical performance. The repeated lithium stripping/plating process at 0.1 mA cm −2 can keep stable for 400 h without short circuit at room temperature. The assembled LiFePO 4 cell shows an initial discharge capacity of 165.9 mAh g −1 at 0.2C and the capacity can remain 80% after 100 cycles. This high-performance composite electrolyte reveals a promising opportunity for the next-generation lithium batteries with high energy density and high safety.

研究领域: 材料科学 · 电化学 · 能源存储
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Journal of Materials Chemistry A · 2026 · IF 9.2

Acetonitrile-driven structural change of Li3InCl6 enables amorphization of PEO-LiTFSI for enhanced room-temperature performance

Weiye Ma,Lun Zhang,Guanghan Zhu,Hongrui Kang,Haiyang Yuan,Yongyi Long,Zhiyi Pan,Zhiqiang Liu,Xiaojing Liu,Jin Liang,Yuxin Liang,Zhenduo Cui,Shengli Zhu,Ying Zhao,Zhonghui Gao

Poly(ethylene oxide) (PEO)-based electrolytes are promising for all-solid-state batteries but are typically limited to elevated temperatures due to PEO crystallinity and strong Li⁺–EO coordination. Here, we report a homogeneous PEO–LiTFSI electrolyte incorporating optimized Li3InCl6 that suppresses PEO crystallization, weakens Li⁺–TFSI⁻ coordination, and enhances Li-ion transport after acetonitrile solvent removal. This effect originates from the structural collapse of Li3InCl6 in acetonitrile, which exposes In3⁺ sites that preferentially adsorb TFSI⁻ anions, thereby disrupting the regular arrangement of PEO chains and inducing amorphization. In contrast to other oxide-based inorganic fillers, our results also found that the interface between PEO and Li3InCl6 enables efficient Li-ion transport. The resulting electrolyte achieves a high room-temperature ionic conductivity of 1.13×10⁻4 S cm-1 and excellent cycling stability with a LiNi0.8Co0.1Mn0.1O2 cathode, retaining 74 % capacity after 100 cycles at 0.3 C and 25 oC. To confirm the generality of this strategy and mechanism, we extended it to InCl3 and GaCl3 fillers, which similarly promoted amorphization in PEO–LiTFSI electrolytes. This work provides a general strategy to design amorphous polymer electrolytes for high-voltage solid-state batteries operating at room temperature.

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IONICS · 2022 ·Vol. 28 ·期 12 ·5341-5350 · IF 2.961

Boosting the mechanical strength and electrochemical performance of PEO/LiTFSI polymeric solid electrolyte via nylon nanofibers

Wang Lei,Yan Jiawei,Shen Wenzhuo,Zhong Min,Zhang Jiali,Guo Shouwu

Poly(ethylene oxide) (PEO)-based polymeric solid electrolytes (PSEs) hold great promise for all-solid-state lithium batteries, but the intrinsic low mechanical strength of PEO limits their practical application and scale production. Herein, PSEs consisting of PEO and lithium bis(trifluoromethanesulfonyl)-imide (LiTFSI) supported on poly(hexamethylene adipamide) (nylon) nanofiber matrix (nylon@PEO/LiTFSI PSEs) are designed and prepared in situ on the Al, Cu foils, and the LiFePO 4 electrodes through coaxially electrospinning at 45 °C. The nylon@PEO/LiTFSI PSEs show nonporous morphology due to in situ melting of the PEO/LiTFSI shell. The mechanical strength of the nylon@PEO/LiTFSI PSE can reach to 3.32 and 2.44 MPa at 25 and 60 °C, respectively, which is stronger than that of the pure PEO membrane or the PSEs prepared via conventional solution casting. The nylon@PEO/LiTFSI PSEs also show tight interfacial contact with LiFePO 4 electrode, resulting in small charge transfer resistance of 376 Ω, and thus afford the LiFePO 4 half coin cells with long charge/discharge cycling stability.

研究领域: 材料科学 · 电化学
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ELECTROCHIMICA ACTA · 2026 · IF 5.8

Oxygen-vacancy-rich nanosized CeO2 for enhancing ionic transport and cycling stability in PEO-LiTFSI composite solid electrolytes

Jun Seo,Mohammad Nasir,Taeho Moon,Hee Jung Park

Low ionic conductivity and low Li⁺ transference numbers limit the practical application of polyethylene oxide (PEO)-based polymer solid electrolytes, arising from PEO semi-crystallinity and poor lithium salt dissociation at ambient conditions. Here, we systematically investigate the size-dependent role of CeO 2 fillers by incorporating nanosized (∼5 nm) and submicron particles into PEO-LiTFSI electrolytes. The nanosized CeO 2 , enriched with surface oxygen vacancies and high specific surface area, simultaneously suppresses PEO crystallinity and provides abundant Lewis acid sites that immobilize TFSI⁻ via Lewis acid-base interactions, increasing the mobile Li + carrier concentration. As a result, the nanosized CeO 2 -based composite electrolyte exhibits an ionic conductivity of 5.95 × 10 –5  S/cm at room temperature (2.4 × higher than pristine PEO) and a Li⁺ transference number of 0.30, nearly fourfold higher than the filler-free system (0.08). In addition, it delivers a widened electrochemical stability window of ∼4.9 V, a high critical current density of 0.8 mA/cm², and stable Li||Li symmetric cycling over 600 h, substantially outperforming both the submicron CeO 2 -based composite and the filler-free electrolytes. Download: Download high-res image (522KB) Download: Download full-size image

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ChemistryOpen · 2020 ·Vol. 9 ·期 6 ·713-718 · IF 2.37

PEO-LITFSI-SiO2-SN System Promotes the Application of Polymer Electrolytes in All-Solid-State Lithium-ion Batteries

Wang Lyu,Guoqiang He,Ting Liu

All-solid-state polymer lithium-ion batteries are ideal choice for the next generation of rechargeable lithium-ion batteries due to their high energy, safety and flexibility. Among all polymer electrolytes, PEO-based polymer electrolytes have attracted extensive attention because they can dissolve various lithium salts. However, the ionic conductivity of pure PEO-based polymer electrolytes is limited due to high crystallinity and poor segment motion. An inorganic filler SiO 2 nanospheres and a plasticizer Succinonitrile (SN) are introduced into the PEO matrix to improve the crystallization of PEO, promote the formation of amorphous region, and thus improve the movement of PEO chain segment. Herein, a PEO 18 −LiTFSI−5 %SiO 2 −5 %SN composite solid polymer electrolyte (CSPE) was prepared by solution-casting. The high ionic conductivity of the electrolyte was demonstrated at 60 °C up to 3.3×10 −4 S cm −1 . Meanwhile, the electrochemical performance of LiFePO 4 /CSPE/Li all-solid-state battery was tested, with discharge capacity of 157.5 mAh g −1 at 0.5 C, and capacity retention rate of 99 % after 100 cycles at 60 °C. This system provides a feasible strategy for the development of efficient all-solid-state lithium-ion batteries. Graphical All-solid-state polymer lithium-ion batteries are ideal choice for the next generation of rechargeable lithium-ion batteries due to their high energy, safety and flexibility. The ionic conductivity of pure PEO-based polymer electrolytes are limited by high crystallinity and poor segment motion. In this work, an inorganic filler and a plasticizer have been introduced into the PEO matrix to improve the crystallization and promote the formation of amorphous region, and thus improve the movement of PEO chain segments. This work provides a feasible strategy for the development of all-solid-state lithium-ion battery.

研究领域: 材料科学 · 电化学 · 储能技术 · 高分子科学 · 锂离子电池
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ACS Omega · 2026 ·Vol. 11 ·期 34 ·50883-50891 · IF 5.2

Li3InCl6 as an Active Filler Improves Interfacial Stability of PEO-LiTFSI Composite Solid Polymer Electrolytes for All-Solid-State Lithium Metal Batteries

Kang Hongrui,Ma Weiye,Hofmann Jan P.,Gao Zhonghui

Composite solid polymer electrolytes (CSPEs) with inorganic fillers are of great interest for advanced all-solid-state lithium–metal batteries (ASSLMBs), enabling high energy density and enhanced safety. Despite increasing interest, the effects of different inorganic fillers on the interface between CSPEs and the lithium metal anode (LMA) remain not fully understood. Herein, we systematically study the contact behavior between the LMA and CSPEs containing PEO, LiTFSI, as well as oxide- (Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 ), sulfide- (Li 6 PS 5 Cl), and halide-based (Li 3 InCl 6 ) fillers by evaporating lithium metal stepwise onto CSPE thin films under ultrahigh vacuum conditions, followed by in-system X-ray photoelectron spectroscopy (XPS) analysis. XPS results demonstrate that halide-based fillers can facilitate the formation of electron-rich Li–O and Li–S species at the interfaces, acting as a passivation layer, which can prevent further decomposition of the CSPE and thus improve interfacial stability. In contrast, the incorporation of oxide- and sulfide-based fillers does not promote the interfacial reactions. Impedance spectroscopy as a function of resting time also shows that the incorporation of a halide-based filler reduces the CSPE/LMA interfacial impedance, which is beneficial for increasing the critical current density for lithium dendrite formation. The incorporation of active inorganic fillers to induce protective interphases offers a novel strategy for interfacial engineering of ASSLMBs.

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Journal of Energy Storage · 2024 · IF 8.9

Ga/Ta co-doped LLZO enhanced voltage tolerance and lithium dendrite resistance of composite solid electrolytes

Pengfei Pang,Yiran Bai,Hu Wang,Jiangchao Chen,Furong Zhang,Zhuoyan Yi,Yunyun Zhao,Kunpeng Jiang,Guisheng Zhu,Huarui Xu

The all-solid-state lithium batteries (ASSLBs) are widely acknowledged as the most promising candidate for energy storage devices due to their excellent safety features and high energy density. However, ASSLBs face significant challenges in terms of low ionic conductivity and the formation of lithium dendrites. Excitingly, composite solid-state electrolytes offer promising solutions to critical challenges. Here, we report a PEO-LiTFSI/LGLZTO organic-inorganic composite solid-state electrolytes (O-ICSEs). A high-performance Li 6.4 Ga 0.10 La 3 Zr 11.7 Ta 0.30 O 12 particles, co-doped with Ga and Ta, was incorporated into matrices of poly (ethylene oxide) (PEO) and lithium bis(trifluoro-methylsulfonyl)imide (LiTFSI) to establish a continuous pathway for the transportation of Li + . Additionally, the synergistic effect of Ga and Ta enhances the Li + transport capability within the LGLZTO particles. PEO-LiTFSI/LGLZTO O-ICSEs, which have fast ion transport channels, exhibit exceptional ionic conductivity (4.35 × 10 −4  S cm −1 at 60 °C) and possess a wide and stable electro- chemical window (5.5 V). The Li||PL(Ga 0.10 Ta 0.30 ) 25 ||Li cell demonstrates an outstanding cycle life exceeding 1000 h at a current density of 0.2 mAh cm −2 . The prominent electrochemical performance of PL(Ga 0.10 Ta 0.30 ) 25 O-ICSEs can primarily be attributed to their excellent electrode/electrolyte interfacial compatibility and effective suppression of Li dendrite growth. The proposed PL(Ga 0.10 Ta 0.30 ) 25 O-ICSEs offer a promising solution for designing highly efficient ASSLBs.

研究领域: 材料科学 · 电化学 · 能源存储
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Journal of Materials Chemistry A · 2020 ·Vol. 8 ·期 44 ·23344-23353 · IF 11.301

Thin laminar composite solid electrolyte with high ionic conductivity and mechanical strength towards advanced all-solid-state lithium–sulfur battery

Pengfei Zhai,Na Peng,Zeyu Sun,Wenjia Wu,Weijie Kou,Guoshi Cui,Kang Zhao,Jingtao Wang

The development of thin solid-state electrolyte with high ionic conductivity and mechanical strength is of great importance for the high-performance all-solid-state lithium–sulfur battery. However, the state-of-the-art solid polymer electrolyte suffers from poor ionic conductivity and a high thickness but inferior mechanical strength. Herein, a thin laminar composite solid electrolyte (LCSE), namely Vr/PEO-LCSE, is fabricated by filtrating vermiculite nanosheets, followed by intercalation of PEO–LiTFSI into the interlayer through a swelling and filtration method. The continuous interlayer channels with improved PEO chain motility and LiTFSI dissociation afford Vr/PEO-LCSE a highly enhanced ionic conductivity of 1.22 × 10−5 S cm−1 at 25 °C. Together with the low thickness (10 μm), Vr/PEO-LCSE achieves an ultralow area-specific resistance of 66 Ω cm2 at 30 °C, about 50 times lower than pure PEO. Meanwhile, the typical brick-and-mortar architecture combined with the strong rigidity of vermiculite nanosheet imparts Vr/PEO-LCSE an excellent compressive strength of 131 MPa, 550% higher than that of pure PEO. As a result, the rate performance of the assembled Li–S battery is significantly improved. The Li|Vr/PEO-LCSE|S cell achieves low capacity fading as current density increases from 0.05C to 0.20C, and the discharge capacity recovers to 1100 mA h g−1 when the current density switches back to 0.05C.

研究领域: 材料科学 · 电化学 · 电池技术
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Li+ affinity ultra-thin solid polymer electrolyte for advanced all-solid-state lithium-ion battery

Shuohan Wang,Jian Li,Tengfei Li,Weiguo Huang,Lihua Wang,Shengdong Tao

The chasing for all-solid-state lithium-ion batteries (ASSLIBs) is based on the need for safer and higher energy density batteries. In this regard, solid polymer electrolytes (SPEs) are well-renowned for their processability and electrochemical stability, yet slimmer and more flexible SPE with higher ionic conductivity is still desired. Herein, an ultrathin (35 µm), rigidity-enhancing co-blending SPEs design using electrospinning was proposed, blending bio-polyamide with a N -substituted pyrrolidone ring (IBD) with polyethylene oxide/lithium bis(trifluoromethanesulfonyl)imide (PEO/LiTFSI). IBD is confirmed to possess the dominant Li + affinity. Then IBD with flexible chain segments of PEO, triggers a concerted ion-transport mechanism synergistically, in which IBD is responsible for the processes of enhanced ion-pair dissociation resulting in dynamic association between the mobile cations and the long-chain molecules that constitute the SPE. Meanwhile, it could broaden the ion transport channel in some extent. The ionic conductivity of the SPE is up to 4.26 × 10 −4  S cm −1 at 50 ℃. Furthermore, the high strength modulus, low crystallinity, and ultra-thin characteristic of IBD-PEO/LiTFSI power-assisted the ASSLIBs of LiFePO 4 //Li to achieve extraordinary cycle performance (80.5 % capacity retention after 580 cycles at C/2 rate) and the average coulomb efficiency exceeds 99.5 % at 50 ℃. Moreover, it has the ability to withstand folding and bending conditions.

CAS / MDL: 123-31-9 7664-38-2
研究领域: 材料科学 · 电化学 · 电池技术
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