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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

A flexible, ion-conducting solid electrolyte with vertically bicontinuous transfer channels toward high performance all-solid-state lithium batteries

Chong Liu,Junxiao Wang,Weijie Kou,Zhihao Yang,Pengfei Zhai,Yong Liu,Wenjia Wu,Jingtao Wang

All-solid-state lithium batteries, featuring high security and volume energy density, hold great potential as next-generation energy storage device. However, their development needs the fabrication of ionic conductive and structural stable solid electrolyte. Herein, Li 0.33 La 0.557 TiO 3 (LLTO) framework with interlocked porous structure is synthesized by sintering the gel permeated nylon. Then, poly(ethylene oxide) (PEO) is incorporated in the pores to produce PEO-LLTO framework solid electrolyte (PLLF electrolyte) with vertically bicontinuous phase. We demonstrate that LLTO framework fast transports Li + through the intrinsic vacancy; meanwhile the confined PEO with low crystallization displays fast Li + transfer ability, thus synergistically realizing efficient Li + conduction. This novel PLLF electrolyte exhibits a remarkable ionic conductivity of 2.04 × 10 −4 S cm −1 , which is ~72 times higher than that of traditional PEO-based electrolytes and superior to most reported solid electrolytes. Moreover, the interconnected networks endow PLLF electrolyte with excellent structural stability. Thus, the LiFePO 4 (LFP)/Li cell exhibits extraordinary cycling stability: the discharge capacity of 154.7 mAh g −1 at 1 C after 150 cycles with capacity decay of only 0.03% per cycle. Briefly, such a vertically bicontinuous phase structure maximizes the cooperation between the conduction function of ceramic framework and the stability of polymer, offering a promising approach for all-solid-state batteries.

研究领域: 材料科学 · 能源存储技术
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Journal of Materials Chemistry A · 2024 ·Vol. 12 ·期 10 ·5768-5777 · IF 10.7

Pentafluorobenzene boronic acid with strong Lewis acidity for the modification of PEO-based polymer electrolytes

Liwei Su,Yijuan Zhu,Xingyi Zhan,Kang Yu,Tianyu Guo,Ke Gu,Hao Wu,Lianbang Wang,Yuanhao Wang,Xiaoxiang Wang

The practical application of polyethylene oxide (PEO) based solid-state electrolytes is severely limited by their low room-temperature ion transport, narrow electrochemical window, and unstable Li/PEO interfaces. This work introduces pentafluorobenzene boronic acid (PFBBA), with –C6F5 and –B(OH)2 ligands, as an advanced additive to resolve these problems. At 30 °C, the electrolyte containing 1.0% PFBBA shows the best performance with an ionic conductivity of 3.09 × 10−5 S cm−1, an Li+ ion transference number of 0.342, and an electrochemical window up to 5.0 V (vs. Li/Li+). The Li//Li battery can stably deposit/peel Li for 1000 h without a short circuit. The reversible capacity of Li//LiFePO4 full batteries at 0.5C after 500 cycles is 124.8 mA h g−1. The modification mechanism is studied by experimental and computational methods. The electron-withdrawing –C6F5 endows B in PFBBA with stronger Lewis acidity and better affinity with F in LiTFSI by forming π–π coordination. The hydrogen bonding interaction between B–OH in PFBBA and –O– in PEO changes the crystallinity of PEO. These two aspects enhanced Li+ ion transport and widened the electrochemical stability window. More importantly, PFBBA participates in in situ forming a LiF/Li–B–O rich SEI layer on the Li anode surface, enhancing the SEI film's mechanical strength and Li+ ion flux.

CAS / MDL: 90076-65-6
研究领域: 材料科学 · 电化学 · 能源存储
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JOURNAL OF MATERIALS SCIENCE · 2025 ·Vol. 60 ·期 10 ·4929-4945 · IF 3.9

Electrospun PEO/PVDF blend solid polymer electrolytes with improved electrochemical performances for lithium metal batteries

Gao Shanshan,Wang Wenshuo,Xing Haoran,Pan Pengju,Bao Yongzhong

Solid polymer electrolytes (SPEs) are routinely regarded as potential candidates to replace conventional lithium-ion liquid electrolytes due to their high safety and energy density. Poly(ethylene oxide)/poly(vinylidene fluoride)/lithium bis(trifluoromethanesulfonyl)imide (PVDF/PEO/LiTFSi) SPEs were prepared by a one-step electrospinning process and utilized in lithium metal batteries in this study. The electrospinning process enhanced the compatibility between PEO and PVDF, and induced the α to β -phase crystalline transition of PVDF. Consequently, the continuity of the conductive phase, the solubility and the migration ability of lithium ions within the polymer matrix were improved. Compared to PEO/PVDF/LiTFSi SPE prepared by a solution casting method, the electrospun SPE exhibited superior electrochemical performances at the same composition, achieving a lithium-ion transference number of 0.64 at room temperature and 0.60 at 60 °C. The assembled LiFePO 4 /SPE/Li cell shows a stable capacity of 112 mAh g −1 with a retaining capacity of 105 mAh g −1 after 400 cycles at the current density of 1 C at 60 °C, and the Coulombic efficiency is 100%. Graphical abstract

CAS / MDL: 68-12-2 872-50-4
研究领域: 材料科学 · 能源存储
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS · 2020 ·Vol. 31 ·期 3 ·2708-2719 · IF 2.22

Nano-SiO2@PMMA-doped composite polymer PVDF-HFP/PMMA/PEO electrolyte for lithium metal batteries

Li Jian,Hu Rong,Zhou Hongming,Tao Shengdong,Wang Ya

Polymer electrolytes have attracted widespread attention owing to their low cost and excellent processability. However, polymer electrolytes have yet been widely applied in commercial batteries due to their own drawbacks, such as weak mechanical properties and lower ionic conductivity. In this paper, poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) was blended with polyethylene oxide (PEO) and polymethyl methacrylate (PMMA) to build a novel polymer matrix, and SiO 2 @PMMA was doped into blended polymer matrix to form a composite polymer electrolyte named CPE-(SiO 2 @PMMA). The CPE-(SiO 2 @PMMA) performs superior electrochemical performance, such as a favorable electrochemical stability window (4.7 V vs Li/Li + ), decent ionic conductivity (8.54 × 10 –5  S cm −1 at 60 ℃), and excellent interface stability. The lithium metal battery LiNi 0.8 Co 0.1 Mn 0.1 O 2 /CPE/Li was fabricated to build a high specific energy system, which performs excellent cycling and C-rate performance compared to others polymer electrolytes. Capacity retention of LiNi 0.8 Co 0.1 Mn 0.1 O 2 /Li cell with CPE-(SiO 2 @PMMA) achieves 81.6% after 100 cycles, while CPE was broken with 100 cycles unfinished. All of the above favorable properties proved that PVDF-HFP/PMMA/PEO polymer matrix with SiO 2 @PMMA doped is a promising electrolyte candidate for flexible lithium metal batteries.

研究领域: 材料科学 · 能源技术
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TALANTA · 2019 · IF 4.916

Development of amphiphile 4-armed PEO-based Ti4+ complex for highly selective enrichment of phosphopeptides

Yu-Lin Huang,Jian Wang,Ying-Hua Jiang,Peng-Yuan Yang,Guo-Wei Wang,Feng Liu

Protein phosphorylation is a reversible and important post-translational modification. Identification of phosphopeptides without enrichment is difficult for the low-abundance of phosphopeptides in real complex biological samples. Therefore, the effective and selective concentration of phosphopeptides prior to proteomic identification by mass spectrometer is necessary. In this study, we synthesized a novel titanium-based immobilized metal ion affinity chromatography material for highly selective enrichment of phosphopeptides. To improve material hydrophilia to the maximum extent, titanium ions were immobilized on the 4-armed Poly(ethylene oxide)(4μ-PEO-Ti 4+ ), a totally soluble polymer with large molecular weight (20000 g/mol). The 4μ-PEO-Ti 4+ was used to enrich phosphopeptides from tryptic digests of standard proteins and real complex biological samples, followed by MALDI-TOF MS analysis. In enrichment of phosphopeptides from 4 pmol β-casein, the 4μ-PEO-Ti 4+ performed the best property with starting material of 99–132 μg, loading buffer of 50% ACN/5% TFA (v/v), elution buffer of 10% NH 3 ·H 2 O (v/v) and elution time of 30 min. The 4μ-PEO-Ti 4+ has a superior detection sensitivity as low as 2 fmol for phosphopeptides. The high selectivity of 4μ-PEO-Ti 4+ allows a deep enrichment of phosphopeptides of β-casein from a mixture with BSA of 1000-fold abundant. The 4μ-PEO-Ti 4+ shows great stability and endurability and can be recycled up to at least 5 times. In addition, 4μ-PEO-Ti 4+ could detect 10 and 15 phosphopeptides from non-fat milk and nonenzymatic human saliva, respectively. In total, 4μ-PEO-Ti 4+ is a novel excellent material which shows great sensitive and selective enrichment of low-abundance phosphopeptides in real complex biological samples.

研究领域: 蛋白质组学 · 生物化学 · 分析化学
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Energy Storage Materials · 2020 · IF 16.28

Polycation ionic liquid tailored PEO-based solid polymer electrolytes for high temperature lithium metal batteries

Jiewen Tan,Xin Ao,Alvin Dai,Yifei Yuan,Hao Zhuo,Hao Lu,Libin Zhuang,Yuxuan Ke,Chenliang Su,Xinwen Peng,Bingbing Tian,Jun Lu

Poly(ethylene oxide) (PEO)-based polymer electrolytes are promising candidates for solid-state electrolytes in safer, next generation lithium metal batteries. Despite their benefits however, PEO-based electrolyte exhibits highly crystalline ethylene oxide chains that provide poor ionic conductivity and, thus severely limit its practical application. Here, we report the use of hydroxypropyl trimethylammonium bis(trifluoromethane) sulfonimide chitosan salt (HACC-TFSI), which is an amorphous poly(ionic liquid) based biomass chitosan derivative, as a modifier for PEO-based solid polymer electrolytes (SPEs) to address these deficiencies. Hybrid SPEs with HACC-TFSI display enlarged amorphous regions with enhanced ionic conductivity. Interactions between quaternary ammonium cations and TFSI − anions in hybrid SPEs are also found to promote dissociation between Li + and TFSI − , which further increases ionic mobility. Moreover, the electrochemical stability, mechanical strength, and thermal stability of hybrid SPEs are collectively superior to blank SPEs without HACC-TFSI. LiFePO 4 /SPEs/Li full-cells assembled using 10wt% HACC-TFSI in PEO (10%HACC-TFSI/SPEs) electrolyte provide a capacity of 161.3 mAh g −1 and operate with excellent cycle performances at 0.2 C and 60 °C. Even when the temperature is increased to 150 °C, LiFePO 4 /SPEs/Li cells with 10%HACC-TFSI/SPEs still display remarkable cycle performance with 73% capacity retention after 100 cycles at 1 C rate.

研究领域: 材料科学 · 电化学
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Journal of Energy Storage · 2026 · IF 10.7

Hierarchically porous copper-based metal–organic framework for high-performance PEO-based solid-state electrolytes

Yinzuo Wu,Hua Zhu,Ziyue Fu,Qinlong Zhou,Pengliang Zhang,Qiang Shangguan,Haibang Zhang,Hedong Jiang,Pingchun Guo,Yanxiang Wang,Shijin Yu

The inherent low ionic conductivity and lithium dendrite growth challenges of poly(ethylene oxide) (PEO)-based solid-state electrolytes pose significant barriers to their utilization in safe, high-energy-density lithium metal batteries. To overcome these challenges, this study designed a novel composite solid electrolyte by introducing a HKUST-1 metal-organic framework (HP-Cu-MOF) with a hierarchical microporous/mesoporous structure into a PEO matrix. The unique dual-pore structure of HP-Cu-MOF enables synergistic regulation: its micropores effectively confine TFSI − anions, significantly increasing the Li + transference number t Li + to 0.40 at 60 °C (vs. 0.11 for pure PEO), while the interconnected mesopores construct continuous ion transport channels, achieving a high ionic conductivity of 7.83 × 10 −4  S cm −1 at 60 °C. Simultaneously, the regular octahedral rigid framework of HP-Cu-MOF enhances the mechanical strength of the electrolyte, with Young's modulus increasing to 2.17 GPa (vs. 1.09 GPa for pure PEO). This enables a high critical current density of 1.7 mA cm −2 and excellent cycling stability, with Li symmetric cells stably operating for over 1800 h at 0.2 mA cm −2 . Furthermore, the electrolyte exhibits a broad electrochemical stability window of 5.1 V, enabling compatibility with high-voltage cathodes. The assembled LFP full cell delivers an initial discharge specific capacity of 151.2 mAh g −1 at 0.5C with excellent capacity retention. This work demonstrates that hierarchically porous MOFs offer an efficient electrolyte design strategy for developing next-generation lithium metal batteries integrating high energy density, long cycle life, and enhanced safety.

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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2026 · IF 9.6

PEO-based electrolyte with coordination-entropy-increase strategy for all-solid-state lithium metal batteries

Ziwei Lu,Huicai Wang,Jinping Yu,Yonghui Wang,Jingyi Wu

Multi-cation doping weakens the Li O coordination. • Increased coordination entropy lowers the energy barrier for Li + migration in PEO-based electrolytes. • The new class of PEO-based electrolyte achieves 0.103 mS cm −1 ionic conductivity at room temperature. • The LiFePO 4 /Li full cell delivers stable cycling at 30 °C and 0.1 C. Polyethylene oxide (PEO)-based solid-state polymer electrolytes (SPEs) are promising key materials for all-solid-state lithium metal batteries because of their good processability and compatibility with Li metal. However, their practical deployment is limited by the low Li + conductivity, which mainly originates from the high migration energy barrier induced by strong Li–polymer coordination. Here, this work proposes a coordination-entropy-increase driven all-solid-state electrolyte, PEO-LiTFSI-MgCl 2 -AlCl 3 -ZrCl 4 (SPE-MAZ). The introduction of multi-cations induces diverse coordination structures on PEO chains, creating Li + sites with varied binding strengths and distinct energy barriers. These features narrow the energy differences between adjacent sites, facilitate Li + mobility, and achieve enhanced ionic conduction. SPE-MAZ delivers an ionic conductivity of 0.103 mS cm −1 at room temperature (RT, 30 °C). The assembled Li/SPE-MAZ/Li symmetric cells maintain stable operation for over 1700 h at 60 °C. The LiFePO 4 /SPE-MAZ/Li full cells achieve a specific capacity of 115.1 mAh g −1 at 60 °C and 5 C, with 80% capacity retention preserved after 100 cycles at RT and 0.1 C. This coordination-entropy-increase strategy leads to the realization of SPEs featuring both high conductivity and good stability, offering a novel perspective for SPEs design. Introducing multiple cations (Mg 2+ , Al 3+ , and Zr 4+ ) induces diverse coordination structures on PEO chains, creating Li + sites with distinct binding strengths, which lowers the Li + migration energy barrier and boosts ionic conductivity, thus enabling stable cycling of LFP/Li full cells. Download: Download high-res image (138KB) Download: Download full-size image

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ACS Applied Materials & Interfaces · 2025 · IF 8.2

Tea Polyphenol-Derived Zinc-Rich Complexes for Enhanced Interfacial Dynamics in PEO-Based Gel Electrolytes

Tianyu Zou,Bingchun Jiang,Qian Qu,Bozhong Cao,Jingyu Xu,Shubing Zhen,Jincheng Zhang,Lei Ling,Yusheng Lu,Tong Zhang

The aqueous zinc-ion battery (AZIB) is regarded as one of the most promising energy storage solutions. However, its widespread adoption is hindered by challenges such as zinc dendrite formation and undesirable side reactions, primarily caused by excess free water molecules and ions. This study introduces an ethylene oxide (PEO)-based gel electrolyte designed to address these limitations. By incorporating a zinc-rich ionic conductor (TP-Zn) that establishes a cross-linked hydrogen bond network, we successfully reduce the crystallinity of the PEO matrix and enhance the ionic conductivity and mechanical strength of the electrolyte. The resulting PGPS@TP-Zn gel electrolyte exhibits a remarkable tensile deformation of up to 1785%. The incorporation of TP-Zn significantly alleviates interfacial challenges between the electrolyte and electrode, leading to a more uniform zinc ion flux distribution. This, in turn, improves ion transport kinetics, resulting in a high ionic conductivity of 1.32 × 10–3 S cm–1 and a zinc ion transference number of 0.86. Furthermore, the Zn||Zn symmetrical cell shows exceptional stability when using PGPS@TP-Zn, with a cycle life exceeding 3000 h at a current density of 1 mA cm–2 and a capacity of 1 mAh cm–2. In addition, the Zn||PGPS@TP-Zn||α-MnO2 full cell maintains a capacity retention of 76.9% even after 1000 cycles at a current of 2 A g–1. Remarkably, the assembled pouch cell functions normally even when bent to a maximum angle of 180 degrees. This study highlights the significant practical advantages of the PGPS@TP-Zn gel electrolyte design for advanced AZIB applications.

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ELECTROCHEMISTRY COMMUNICATIONS · 2025 · IF 4.2

Influence of lithium salt anions on the interfacial properties of PEO-based solid-state electrolytes

Yi-Min Wei,An Qiu,Jingchao Wang,Yu Gu,Jian-Feng Li

The use of poly(ethylene oxide) (PEO)-based solid-state electrolytes have shown potential to improve both the energy density and safety performance of lithium-metal batteries. However, these electrolytes often form unstable interfaces with lithium metal anodes, compromising the durability and sustained performance of solid-state lithium-metal batteries. In this study, three lithium salts, lithium (fluorosulfonyl) (trifluoromethanesulfonyl)imide (LiFTFSI), lithium bis(fluorosulfonyl)imide (LiFSI), and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), were each mixed in equimolar ratios with tetraethylene glycol dimethyl ether (G4) and introduced as a conductivity enhancer in PEO-based solid-state electrolytes. The effects of the lithium salt anions on the electrolyte properties were systematically investigated. Among the three, the fluorosulfonyl group was found to enhance ionic conductivity, while the trifluoromethanesulfonyl group improved thermal stability. Notably, the synergistic interaction between these two groups in LiFTFSI led to the formation of a stable solid-electrolyte interphase (SEI), characterized by a higher content of inorganic species and reduced organic components. As a result, LiFTFSI/G4-based solid-state electrolytes enabled stable cycling for 200 cycles at a 0.5C rate in LiFePO 4 -based solid-state lithium-metal batteries, achieving a capacity retention of 91 %. This study provides valuable insights into the optimization of high-efficiency solid-state lithium-metal batteries by elucidating the distinct roles of lithium salt anions.

CAS / MDL: 68441-17-8
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Journal of Mechanical Science and Technology · 2024 ·Vol. 38 ·期 11 ·6169-6179 · IF 1.5

Rapid prediction of electrohydrodynamically printed polyethylene oxide (PEO) fiber width by using response surface methodology

Zhang Bing,Kachar Maryem,Xiao Huapan,Liu Wei,Sui Fanping,Meng Lingchao,Lin Liwei,Ding Jianning

Electrohydrodynamic (EHD) printing of polyethylene oxide (PEO) based composites has attracted extensive interests to fabricate micro/nanoscale fibrous structures in the fields of flexible electronics, tissue engineering, and biosensors. As the PEO fiber width varies remarkably with different processing parameters, it is still difficult to obtain an optimal processing condition before the EHD process. In this study, response surface methodology (RSM) was employed to establish a mathematical model and predict the EHD-printed fiber width. The PEO fibers were electrohydrodynamically printed to obtain the original input data for the modeling. Typical processing parameters including feeding rate, stage moving speed, working voltage, and nozzle-to-collector distance were selected to establish the regression model for the prediction of EHD-printed fiber width. Analysis of variance indicates that the feeding rate has the most significant effect on the fiber width. Theoretical analysis and simulation of the electric field intensity demonstrated the validity of the prediction model. Furthermore, the prediction model has also been verified by EHD printing experiments. This study provides a feasible approach to conveniently predict PEO fiber width without conducting EHD processes, which may promote the rapid design and fabrication of tiny structures with desired feature sizes.

研究领域: 材料科学 · 增材制造 · 纳米加工 · 生物医学工程 · 柔性电子
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2025 · IF 3.9

Electrospun PEO-Based Composite Polymer Electrolyte with MOF Modified LLZTO for Solid-State Lithium Batteries

Yuchen Cong,Jing Li,Haiping Su,Yazhuo Shang,Honglai Liu

Solid polymer electrolytes have emerged as one of the most promising solid electrolytes due to their excellent flexibility and interfacial contact. However, their practical applications are hindered by low ionic conductivity and Li dendrite growth. Herein, metal–organic framework (ZIF-67) modified Li6.4La3Zr1.4Ta0.6O12 (LLZTO) were used as nanofillers (LZ) for PEO-based composite solid polymer electrolytes (CSPE). The electrospinning method was applied to promote the uniform dispersion of LZ particles in the film that helps to construct continuous Li+ transport channels. In addition, the ZIF-67 interact with both ether oxygen in PEO and anion in Li salt and can release more free lithium ions, thereby significantly enhancing the ionic conductivity (1.39 × 10–4 S cm–1, RT) and the Li+ transference number (0.62). The Li/Li symmetric cell continuously cycled without short-circuiting for a long duration over 2000 h, proving the high interface stability of Li-solid electrolyte. The Li/CSPE-LZ/LiFePO4 full cell delivered an initial discharge capacity of 154.3 mA h g–1 at 1 C, with a capacity retention rate of 95.4% after 220 cycles, demonstrating the feasibility of this CSPE for high performance all-solid-state lithium metal batteries.

研究领域: 材料科学 · 电化学 · 能源存储 · 高分子化学 · 固态离子学
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