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JOURNAL OF ALLOYS AND COMPOUNDS · 2025 · IF 6.3

Electrochemical performance enhancement mechanism of CTMS modulating on LLZTO/PEO composite solid electrolyte interface

Qian Liu,Jinghua Yin,Jialong Shen,Zhen Chen,Minghua Chen

With the rapid development of solid state battery technology, composite electrolytes, as a key material for enhancing battery performance, face poor interfacial compatibility issues between inorganic fillers and the polymer matrix , which becomes a bottleneck restricting the improvement of electrochemical properties of the electrolyte. To address the issues of low ionic transport efficiency and the growth of lithium dendrites , which are triggered by the poor interfacial compatibility, this paper introduces the silane coupling agent (3-chloropropyl) trimethoxysilane (CTMS) into the PEO-LLZTO composite solid electrolytes to bridge the inorganic filler and polymer matrix through an in-situ coupling reaction, thereby enhancing the performance of the composite electrolyte. Its ionic conductivity is 1.84 × 10 −3 S/cm at 60°C, and the stability to lithium anode is improved, with a polarization voltage of only 0.017 V and ultra-long lithium symmetrical battery constant current cycle exceeding 1670 h. The assembled full battery exhibited excellent rate performance and cycle stability at 60°C under 0.2 C, its specific capacity remains 138.52 mAh/g after 135 cycles. The mechanism of CTMS enhancing electrolyte properties was investigated by density functional theory (DFT). The adsorption energy , differential charge density, and ELF are calculated to analyze the interaction between the electrolyte components. DFT calculation results suggest that O-Si-O bonds are readily formed at the LLZTO/PEO interface upon the addition of CTMS. More importantly, CTMS modifies the charge distribution of the space charge layer at this interface, effectively facilitating the migration of lithium ions , thereby optimizing the ionic transport properties at the interface. Both experimental and DFT results indicate that CTMS forms a strong chemical bond between the inorganic and polymer segments , which creates a rapid transport channel for lithium ions and reduces the migration of the lithium salt anion group, thereby improving the electrochemical performance of the electrolyte.

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Energy Storage Materials · 2023 · IF 20.4

4.2V polymer all-solid-state lithium batteries enabled by high-concentration PEO solid electrolytes

Zhe Xiong,Zixing Wang,Wang Zhou,Qi Liu,Jian-Fang Wu,Te-Huan Liu,Chaohe Xu,Jilei Liu

Polyethylene oxide (PEO) solid electrolytes (SEs) are practicable in all-solid-state lithium batteries (ASSLBs) with high safety for driving electric vehicles. However, the low oxidative decomposition potential (below 4 V) of normal PEO SEs rules out high-voltage (≥4.2 V) cathodes in PEO-based ASSLBs with sacrificed energy densities . Herein, high-concentration PEO SEs (EO:Li + ≤ 6:1) possessing high oxidation potentials (>5 V vs. Li/Li + ) are designed based on concentrated-salt chemistry with oxidation potential surging incessantly with increasing the degree of coordinated EO. Thereby, double-layered SEs with PEO(EO:Li=4:1) on the cathode side and PEO(EO:Li=16:1) on the anode side are designed to resist oxidation and bate interfacial impedance. Coupled with 4.2 V-class LiCoO 2 and LiNi 0.6 Co 0.2 Mn 0.2 O 2 , the ASSLBs using SEs exhibit enhanced stable cycling performances when charged to 4.2 V and 4.4 V at 60 °C. As revealed by the Wagner-type model and Raman spectra , high-concentration PEO SE could suppress the interfacial degradation kinetics , the production of electronic conduction in the cathode electrolyte interphase (CEI) and the irreversible phase-change of LiCoO 2 to Co 3 O 4 . All these contribute to the improved electrochemical performance of PEO/LiCoO 2 system with high-volage, offering a potential pathway toward high-voltage stable polymer electrolytes for high-energy-density lithium batteries.

研究领域: 材料科学 · 能源存储
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ELECTROCHIMICA ACTA · 2016 · IF 4.803

A new composite solid electrolyte PEO/Li10GeP2S12/SN for all-solid-state lithium battery

Bo Chen,Zhen Huang,Xiaotian Chen,Yanran Zhao,Qiang Xu,Peng Long,Shaojie Chen,Xiaoxiong Xu

A new solid polymer electrolyte (SPE) PEO-LiTFSI-1%LGPS-10%SN is successfully prepared via a convenient method with low cost. The effect of SN on the ionic conductivity of PEO-based electrolyte is systematically investigated. It presents a maximum conductivity of 9.10   ×   10 −5   S·cm −1 at 25   °C, and a 15-fold ion conductivity enhancement in PEO-LiTFSI. It exhibits wide electrochemical window (0–5.5   V) and excellent compatibility with metallic Li. The LiFePO 4 /Li batteries exhibit a good cycling and rate performance under 40   °C, whose maximum discharge specific capacity at 0.1 C is 160.6   mAh·g −1 , and 94.7% can be retained after 60 cycles. At 0.5C, the maximum discharge specific capacity is 138.4   mAh·g −1 , and capacity retention close to 90% even after 100 cycles. The reasons of activation process are discussed. This new SPE with outstanding electrochemical performance is a promising solid electrolyte candidate for applications in all-solid-state lithium battery.

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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2021 · IF 4.464

Study of solid polyurethane electrolytes synthesized from HDI and PEO of different molecular weight

Qian Zhang,Yuhao Wen,Kang Liu,Nailiang Liu,Yaping Du,Chunjie Ma,Liang Zhou,Yongri Liang,Yongcheng Jin

The development of solid polymer electrolyte (SPE) is important for the fabrication of safe and high performance lithium ion battery of the next generation. A series of polyurethanes (PUs) based SPEs synthesized from hexamethylene diisocyanate (HDI) and poly(ethylene glycol)s (PEGs) of varying molecular weight ( MW  = 300 ~ 1500 corresponding to PU03 ~ PU15) via one-step approach are investigated for the conductivity of lithium ion and other electrochemical properties. These synthetic PUs exhibit semi-crystalline structures when the MW of PEG is higher than 300, and turn into amorphous after the addition of LiClO 4 . The ionic conductivity decreases with the increasing concentration of LiClO 4 . The highest lithium ion conductivity was found to be 3.42 × 10 −5 S/cm for PU15 with 10 wt% LiClO 4 at 50 °C. However, its lithium ion transference number is low by 0.15. All of the PU-based SPEs containing 10 wt% LiClO 4 are electrochemically stable up to 4.2 ~ 4.5 V versus Li + /Li, and show very good cycling stability in charge/discharge experiments. In the assembled battery with LiFePO 4 as the cathode, PU15 displays higher performances than PU03, indicating good correlation to the molecular weight of PEG.

研究领域: 材料科学 · 电化学 · 电池技术
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Scientific Reports · 2025 ·Vol. 15 ·期 1 ·1-11 · IF 3.9

Tuning of dynamic solvation structures via click chemistry for PEO-based solid polymer electrolytes

Li Ruiyang,Yang Xueying,Chen Qichen,Huang Boyang,Zhao Siyu,Zhang Peng,Lin Jie,Zhao Jinbao

The Li + -transport mechanisms in both solid polymer electrolytes (SPEs) and liquid electrolytes (LEs) are fundamentally governed by solvation dynamics, requiring an optimal balance between continuous coordination and moderate binding strength. Poly(ethylene oxide) (PEO) is a classic SPE matrix that leverages its –CH 2 –CH 2 –O– (EO) segments to provide continuous oxygen coordination for Li + transport via amorphous regions. While continuous EO segments facilitate the intra-chain Li + -transport, their strong multidentate solvation of Li + through a chelate effect – each Li + chelates with 4–6 ethylene oxide (EO) units – significantly hinders the inter-chain Li + mobility. This effect creates rigid solvation cages that both immobilize Li + and resist modification by alternative moieties (e.g. carbonate or nitrile groups), resulting in poor room-temperature ionic conductivity ( σ ) and low Li + transference number ( t Li+ ). To address these challenges, we developed a series of precise Li + -transport models (LTMs) through click chemistry, strategically combining acrylate-PEG and acrylonitrile to engineer balanced interactions between multidentate (EO) and monodentate (C = O, C ≡ N) coordination sites. This design achieved synergistic enhancement of both inter- and intra-chain transport pathways, demonstrated by significantly improved performance with σ  = 6.40 × 10 − 5 S/cm and t Li+ = 0.44 at 25 °C. This approach permits tailored control of dynamic solvation structures, offering new opportunities to enhance Li + transport in PEO-based solid polymer electrolytes.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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Batteries-Basel · 2022 ·Vol. 8 ·期 10 ·141 · IF 5.938

Agglomeration-Free and Air-Inert Garnet for Upgrading PEO/Garnet Composite Solid State Electrolyte

Jun Cheng,Hongqiang Zhang,Deping Li,Yuanyuan Li,Zhen Zeng,Fengjun Ji,Youri Wei,Xiao Xu,Qing Sun,Shang Wang,Jingyu Lu,Lijie Ci

Due to the intrinsically high ionic conductivity and good interfacial stability towards lithium, garnet-type solid electrolytes are usually introduced into polymer electrolytes as fillers to prepare polymer/garnet composite electrolytes, which can improve the ionic conductivity and enhance the mechanical strength to suppress Li dendrites. However, the surface Li2CO3and/or LiOH passive layers which form when garnet is exposed to the air greatly reduce the enhancement effect of garnet on the composite electrolyte. Furthermore, compared with micro-size particles, nano-size garnet fillers exhibit a better effect on enhancing the performance of composite solid electrolytes. Nevertheless, inferior organic/inorganic interphase compatibility and high specific surface energy of nanofillers inevitably cause agglomeration, which severely hinders the effect of nanoparticles for promoting composite solid electrolytes. Herein, a cost-effective amphipathic 3-Aminopropyltriethoxysilane coupling agent is introduced to modify garnet fillers, which effectively expands the air stability of garnet and greatly improves the dispersion of garnet fillers in the polymer matrix. The well-dispersed garnet filler/polymer interface is intimate through the bridging effect of the silane coupling agent, resulting in boosted ionic conductivity (0.72 × 10−4S/cm at room temperature) of the composite electrolyte, enhanced stability against lithium dendrites (critical current density > 0.5 mA/cm2), and prolonged cycling life of LFP/Li full cells.

研究领域: 材料科学 · 电化学
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IONICS · 2018 ·Vol. 24 ·期 12 ·3805-3813 · IF 2.347

Effect of liquid crystal ionomer intercalated montmorillonite nanocomposites on PEO/PLA solid polymer electrolytes

Zhang Nan,Zhang Ai-ling,Liu Qi-fang,Zhang Meng,Li Qiu,Li Fang-fang

A series of solid polymer electrolytes (SPEs) based on poly (ethylene oxide)/polylactic acid (PEO/PLA) with liquid crystal ionomer (LCI) intercalated montmorillonite (MMT) nanocomposites (LCI-MMT) has been prepared by solution blending method. The effects of LCI-MMT on the structural, crystallization, thermal, and ionic conductivity properties of solid polymer electrolytes have been analyzed. It is demonstrated that the incorporation of LCI-MMT into the blend suppressed the crystallinity of PEO and increased the crystallinity of PLA. The maximum ionic conductivity is found to be in the range of 1.05 × 10 −5  S/cm for 0.5 wt% LCI-MMT, which is higher than that of the LCI-MMT-free polymer electrolyte (5.36 × 10 −6  S/cm) at room temperature.

研究领域: 材料科学 · 高分子科学 · 电化学 · 纳米复合材料
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ELECTROCHIMICA ACTA · 2017 · IF 4.798

A promising TPU/PEO blend polymer electrolyte for all-solid-state lithium ion batteries

Can Tao,Ming-Hao Gao,Bo-Hao Yin,Bin Li,Yi-Ping Huang,Gewen Xu,Jun-Jie Bao

Solid polymer electrolyte (SPE) membranes composed of thermoplastic polyurethane (TPU), poly(ethylene oxide) (PEO) and lithium bis(trifluoromethane sulfonimide) (LiTFSI) are prepared and investigated in this work. The results show that addition of TPU to the blend polymer results in loss of the crystallinity of PEO and improve the dissolution of lithium salts into the SPE matrix. TPU can also improve the mechanical stability and the electrochemical properties. Among the TPU/PEO blend electrolytes, the TPU/PEO   =   1:3 based electrolyte presents an ionic conductivity of 5.3   ×   10 −4   S   cm −1 with electrochemical stability above 5   V (vs. Li + /Li) at 60   °C. The LiFePO 4 /SPE/Li coin cell based on SPE (TPU/PEO   =   1:3) is assembled and shows the attractive discharge capacity (140 and 154   mAh   g −1 at 0.2C under 60 and 80   °C, 112 and 127   mAh   g −1 at 1C under 60 and 80   °C) and outstanding cycling stability (close to 96% and 94% after 100th cycles at 1C under 60 and 80   °C), respectively. These results demonstrated that the TPU/PEO blend polymer electrolyte should be a promising electrolyte for all-solid-state lithium ion batteries.

CAS / MDL: 90076-65-6 68-12-2
研究领域: 材料科学 · 电化学 · 能源存储
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Journal of Materials Chemistry A · 2021 ·Vol. 9 ·期 43 ·24661-24669 · IF 12.732

Porous polyamine/PEO composite solid electrolyte for high performance solid-state lithium metal batteries

Chenghan Li,Shi Zhou,Lijie Dai,Xuanyi Zhou,Biao Zhang,Liwen Chen,Tao Zeng,Yating Liu,Yongfu Tang,Jie Jiang,Jianyu Huang

Solid polymer electrolytes (SPEs) have attracted much attention due to their better safety and flexibility. However, the low ionic conductivity and narrow electrochemical window impede their applications in PEO-based solid-state batteries. Here we report the synthesis of a new SPE comprising PEO with 1 wt% fluoromethyl modified polyamine (PAN-FMP) as a filler that has high ionic conductivity and a wide electrochemical window. The LiFePO4 (LFP)/SPE/Li cell delivers an initial capacity of 124 mA h g−1 at 1C with a capacity retention of 83% after 1000 cycles. Moreover, the electrochemical stability window of the SPE has been widened up to 4.8 V, which makes it compatible with high voltage cathodes such as LiNi0.8Co0.1Mn0.1O2 (NMC811). The enhanced ionic conductivity of the SPE originates from the PAN-FMP filler rich in –CF3 groups that interact with ether oxygen on the PEO segment and make ether oxygen form loose ion pairs with Li+ ions, thus inhibiting the rearrangement and crystallization of PEO and enhancing Li+ ion transport of the SPE. The long cycle life of the full cell is attributed to the formation of a LiF-rich-solid electrolyte interface (SEI) layer due to PAN-FMP promoting the defluorination of TFSI−. The LiF SEI layer enables uniform lithium metal deposition, and prevents the growth of lithium dendrites. The low-cost, simple preparation method and superior electrochemical performance of the SPE with an organic PAN-FMP filler thus provide a new strategy to enable high voltage and high energy density polymer based solid-state batteries.

研究领域: 材料科学 · 电化学 · 能源存储
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Micro & Nano Letters · 2018 ·Vol. 13 ·期 12 ·1688-1692 · IF 0.841

Centrifugally spun ultrafine starch/PEO fibres as release formulation for poorly water-soluble drugs

Xianglong Li,Yishen Lu,Teng Hou,Jing Zhou,Bin Yang

In this work, the authors prepared drug-loaded ultrafine starch/polyethylene oxide (PEO) fibres through centrifugal spinning, which use the poorly water-soluble drugs ibuprofen (ibu) and ketoprofen (ket) as model drugs. The obtained fibres were treated by acetic acid/glutaraldehyde solution (1/1, v/v) for 12 h at 40°C, in order to remove residual sodium hydroxide in fibres and improve the water stability. The morphology, chemical structures, and mechanical properties of obtained fibres were investigated. In-vitro drug release tests revealed that more than 75% of loaded drugs could be released from fibrous membranes without initial burst release (>80% in the first 2 h). The ibu-loaded fibrous membranes showed a sustained release period as long as 24 h, while the ket-loaded fibrous membranes could release more than 48 h. These fibre-based delivery systems are therefore proposed to be good candidate drug formulations, especially for improving solubility and bioavailability of poorly water-soluble drugs.

研究领域: 药剂学 · 材料科学
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Bifunctional MOF Doped PEO Composite Electrolyte for Long-Life Cycle Solid Lithium Ion Battery

Guolong Lu,Hongjin Wei,Chuanqi Shen,Feng Zhou,Min Zhang,Yihuang Chen,Huile Jin,Jun Li,Guang Chen,Jichang Wang,Shun Wang

A highly stable composite electrolyte was developed in this research to address the performance decline over time in a solid lithium ion battery (SLIB). It involved the synthesis of bifunctional MOF material (MOF-2) from two different functionalized UiO-66 materials containing carboxyl groups and amine groups, respectively, and the subsequent blending of PEO (polyethylene oxide) with the MOF-2 to form the novel composite solid electrolyte (PEO-MOF-2). The composite electrolytes showed higher ionic conductivity (5.20 × 10–4 S/cm) than that of pristine PEO. The LiFePO4||Li cells constructed with PEO-MOF-2 exhibited 98.45% capacity retention with 149.92 mA h/g after 100 cycles operation at 1.0 C, which was higher than those cells prepared with pristine PEO electrolyte or with PEO-based electrolytes that were only doped by aminated MOF or carboxylated MOF. Furthermore, our experiments showed that there was about a 40% increase in the potential window (from 3.5 to 5.0 V) and 80% increase in the lithium ion transfer number (from 0.20 to 0.36 at 60 °C) as a result of replacing pristine PEO electrolyte with PEO-MOF-2.

研究领域: 材料科学 · 电化学
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2023 · IF 8.2

Electrospun nanofiber membranes for rapid liver hemostasis via N-alkylated chitosan doped chitosan/PEO

Tao Liu,Shuhan Liu,Yihan Shi,Zhuoran Zhang,Sheng Ding,Kexin Hou,Wen Zhang,Xin Meng,Fan Li

The ideal hemostatic agents should be able to stop bleeding quickly and avoid secondary bleeding caused by adhesion with blood clots during dressing change. Herein, a hydrophobic electrospun nanofiber membrane was prepared for achieving hemostasis , rationally targeting both attributes, via doping N -alkylated chitosan ( N -CS) grafted with octadecyl into chitosan/polyethylene oxide (PEO). In vitro and in vivo coagulation tests showed that CPNs doped with small amounts of N -CS (CPN31) could significantly shorten hemostasis time and promote the formation of more stable and stronger blood clots. In particular, the whole blood clotting time of CPN31 (58.8 ± 2.2 s) was significantly lower than that of chitosan/PEO (CPN0) nanofiber membrane (67 ± 3.5 s) and the medical sterile gauze (86.7 ± 0.6 s). Furthermore, due to the hemophobic nature of CPNs, blood wetting of the dressing was severely limited and blood can coagulated at the site of liver injury in rats, thus reducing blood loss and allowing rapid removal of the dressing without triggering secondary hemorrhage. The CPN31 exhibited excellent hemostasis properties, easy to remove, blood compatibility, biocompatibility and promoting fibroblast proliferation properties. This hydrophobic CPNs is a promising biological adhesive for hemorrhage control.

研究领域: 生物医学工程 · 材料科学 · 医学
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