ADVANCED FUNCTIONAL MATERIALS
·
2020
·Vol. 30
·期 22
·1909392
·
IF 16.836
Jiliang Qiu,Xinyu Liu,Rusong Chen,Qinghao Li,Yi Wang,Penghao Chen,Luyu Gan,Sang-Jun Lee,Dennis Nordlund,Yijin Liu,Xiqian Yu,Xuedong Bai,Hong Li,Liquan Chen
Poly(ethylene oxide) (PEO)-based solid electrolytes are expected to be exploited in solid-state batteries with high safety. Its narrow electrochemical window, however, limits the potential for high voltage and high energy density applications. Herein the electrochemical oxidation behavior of PEO and the failure mechanisms of LiCoO 2 -PEO solid-state batteries are studied. It is found that although for pure PEO it starts to oxidize at a voltage of above 3.9 V versus Li/Li + , the decomposition products have appropriate Li + conductivity that unexpectedly form a relatively stable cathode electrolyte interphase (CEI) layer at the PEO and electrode interface. The performance degradation of the LiCoO 2 -PEO battery originates from the strong oxidizing ability of LiCoO 2 after delithiation at high voltages, which accelerates the decomposition of PEO and drives the self-oxygen-release of LiCoO 2 , leading to the unceasing growth of CEI and the destruction of the LiCoO 2 surface. When LiCoO 2 is well coated or a stable cathode LiMn 0.7 Fe 0.3 PO 4 is used, a substantially improved electrochemical performance can be achieved, with 88.6% capacity retention after 50 cycles for Li 1.4 Al 0.4 Ti 1.6 (PO 4 ) 3 coated LiCoO 2 and 90.3% capacity retention after 100 cycles for LiMn 0.7 Fe 0.3 PO 4 . The results suggest that, when paired with stable cathodes, the PEO-based solid polymer electrolytes could be compatible with high voltage operation.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
Journal of Materials Chemistry A
·
2026
·
IF 9.2
Yaning Liu,Da Yang,Rui Xu,Yijue Wang,Liuyi Hu,Tianqi Yang,Min Fan,Meiqing Feng,Jianping Xu,Zhen Xiao,Ruyi Fang,Jun Zhang,Xinhui Xia,Hui Huang,Xiayin Yao,Wenkui Zhang,Yang Xia
The advancement of all-solid-state lithium metal batteries (ASSLMBs) with high energy density is significantly constrained by the inherent drawbacks of solid polymer electrolytes (SPEs), such as low room-temperature ionic conductivity, inadequate mechanical strength to prevent lithium dendrite growth, and unstable interfaces between electrodes and electrolytes.To overcome these limitations, this study introduces a synergistic modification strategy for poly(ethylene oxide) (PEO)-based SPEs by incorporating calcium fluoride (CaF2), aiming to concurrently improve bulk electrolyte properties and interfacial stability. The introduction of CaF2 effectively inhibited the crystallization of PEO by steric hindrance and Lewis acid, which made the ionic conductivity of the electrolyte reach 8.49 × 10-5 S cm-1 at 40°C (70% higher than that of the original electrolyte) and the lithium-ion migration number increased to 0.34.The composite electrolyte also demonstrates improved mechanical robustness (yield strength of 1.61 MPa) and electrochemical stability window (with decomposition voltage elevated to 5.01 V), enabling a critical current density of 0.8 mA cm-2 . Theoretical and experimental investigations reveal that CaF2 promotes the formation of a hybrid solid electrolyte interphase (SEI) enriched with LiF and Ca-Li alloys, which guides uniform lithium deposition. As a result, Li symmetric cells achieve stable cycling over 1600 hours, and LiFePO4||Li full cells retain 98.1% of their initial capacity after 300 cycles at 0.5 C. This work offers a scalable pathway for designing dendrite-suppressing SPEs through dual optimization of bulk and interfacial characteristics.
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DOI
高影响因子
Journal of Materials Chemistry A
·
2026
·
IF 9.2
Qiuying Xu,Zunxiang Hu,Yaning Shangguan,Lina Liu,Rongmin Lu,Lijuan Zhang,Xuehui Shangguan,Lijun Gao,Mengmeng Liu,Haixin Zhang,Huanqi Yao,Qinglei Wang,Faqiang Li
Polyethylene oxide (PEO) is widely used in solid electrolytes because of its excellent interface compatibility and film-forming ability. However, its low room-temperature ionic conductivity and narrow electrochemical window limit its commercial application. Herein, these issues can be effectively addressed via a carbonate-tuned strategy based on different cyclic carbonate side chains such as vinylene carbonate (VC) and vinylethylene carbonate (VEC). By shielding lithium salt electrostatic interactions through ion–dipole interactions, the highly polar carbonyl group of VEC preferentially induces the decomposition of DFOB−, forming a composite SEI film rich in LiF and thus inhibiting the continuous decomposition of PEO. It is noted that PEVEC SPE exhibits superior electrochemical performance due to flexible chain segment movement and uniform charge regulation. The optimized SPE presents a high ionic conductivity of 3.87 × 10−5 S cm−1 at 25 °C and a broad electrochemical window of 4.9 V. Besides, the Li/Li symmetric cell displays excellent cycle stability over 2500 hours. Notably, the Li/LFP cell shows enhanced long-term stability (capacity retention is 93.73% after 1000 cycles at 25 °C). More importantly, the 4.4 V Li/LCO battery displays a capacity retention rate of 84.4% after 120 cycles at 25 °C. Meanwhile, this well-engineered electrolyte enables outstanding safety performance in pouch cells even under harsh deformation and sectioning conditions. This carbonate-tuned strategy opens new avenues for designing PEO-based solid electrolytes towards high-performance lithium metal batteries.
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DOI
高影响因子
Nanoscience and Nanotechnology Letters
·
2019
·Vol. 11
·期 3
·361-369
·
IF 0
Zhu Yinghua,Cao Jiang,Li Baohua,Wang Yanjie,Liang Linfu,Chen Hong
Polymer electrolyte is an effective way to solve stability and security issues in lithium (Li) metal anode caused by nonuniform lithium deposition and unstable solid electrolyte interphase (SEI). However, it still remains a challenge to obtain an electrolyte that combines high ionic
conductivity and mechanical properties. Herein, we used nano-SiO2 grafted with reactive groups as crosslinkers to cooperate with PEO to construct a composite polymer network. And this polymer network was further interpenetrated with PVDF-HFP to build a Semi-IPN gel composite polymer
electrolyte (Semi-IPN-GCPE) by simple UV curing. The polymer electrolyte exhibited high ionic conductivity (2.71 × 10–3 S cm–1 at room temperature), wide electrochemical stable window (∼5 V vs. Li/Li+), considerable tensile strength (7.04
MPa), breaking strain (248.1%), good thermal stability up to 330 °C and excellent stability with lithium metal anode. The assembled Li/Semi-IPN-GCPE/LiFePO4 cell delivered specific capacities of 103 mAh g–1 at 10 C and presented above 90% capacity reten- tion
after 300 cycles at 1 C. Our work provides a facile approach to preparing dendrite-suppressing polymer electrolytes with potential applicability in next-generation Li metal batteries.
研究领域:
材料科学
·
储能技术
·
聚合物化学
·
电化学
·
锂离子电池
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DOI
Journal of Physical Chemistry C
·
2023
·
IF 3.7
Huihui Gan,Jiajun Sun,Ye Xia,Pengyuan Qiu,Liang Li,Wen Zhu
A composite solid polymer electrolyte (CSPE) is the best candidate in all-solid-state lithium metal batteries because of its flexibility, high safety, wide electrochemical stability, relatively high ionic conductivity, and excellent compatibility with the lithium metal. In this work, the garnet-type Li6.75La3Zr1.75Ta0.25O12 (LLZTO) is introduced into a poly(ethylene oxide) (PEO)/poly(vinylidene fluoride–hexafluoropropylene) (PVDF–HFP)-based CSPE (PEO/PVDF–HFP/LLZTO CSPE). The PEO/PVDF–HFP/LLZTO CSPE possesses a high lithium-ion transference number of 0.47, a high ionic conductivity of 2.65 × 10–4 S cm–1, a wide electrochemical window of 5.55 V vs Li+/Li, and effective inhibition of lithium dendrite growth for 1000 h with a current density of 0.10 mA cm–2. Furthermore, the Li//LiFePO4 cell assembled with the PEO/PVDF–HFP/LLZTO CSPE delivers superior rate capability and good cycling stability. Therefore, the PEO/PVDF–HFP/LLZTO CSPE is a very promising candidate for high-performance all-solid-state lithium metal batteries.
研究领域:
材料科学
·
电化学
·
储能技术
·
高分子科学
·
锂电池
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DOI
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2023
·Vol. 25
·期 27
·18297-18309
·
IF 3.3
Lifa Zhang,Liang Fu,Weisi Qin,Yaolong He,Hong Liu,Hongjiu Hu
Pre-stretching as a method for directing polymer crystallization offers a promising solution for addressing the limitations of solid polymer electrolytes in flexible batteries at ambient temperatures. In this study, we have investigated the ionic conductivity, mechanical behaviour, and microstructural and thermal properties of polyethylene oxide (PEO)-based polymer electrolytes with varying pre-strain levels. The results indicate that thermal stretching-induced pre-deformation can significantly increase the through-plane ionic conductivity, in-plane strength, stiffness of solid electrolytes, and cell-specific capacity. However, modulus and hardness decrease for pre-stretched films in the thickness direction. Notably, applying 50–80% pre-strain to the PEO matrix composites through thermal stretching may be preferred for improving the electrochemical cycling performance, as it can increase through-plane ionic conductivity by at least 1.6 times while maintaining compressive stiffness at 80% compared to their unstretched counterparts, while the in-plane strength and stiffness can be boosted by 120–140%. Besides, adding nanoceramics contributes to lithiated PEO exhibiting a higher enhancement coefficient than the pristine sample. This positive effect is because the pre-strain and nano-inorganic filler decrease crystallinity and increase the free volume size of pre-stretched PEO-based electrolytes.
研究领域:
材料科学
·
聚合物物理
·
储能技术
·
电化学
·
固体离子学
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DOI
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2024
·Vol. 26
·期 10
·8125-8140
·
IF 2.9
Qinghua Yang,Detao Kong,Liang Fu,Yaolong He,Hongjiu Hu
Polyethylene oxide (PEO)-based solid polymer electrolytes (SPEs) have good ionic conductivity and flexibility, and is a key component of all-solid-state lithium batteries (ASSLBs). Therefore, the mechanical integrity of PEO-based SPEs during cell operation needs to be urgently evaluated. Here, we conducted a series of tensile and shear adhesion performance tests on PEO16–LiTFSI electrolyte and LiFePO4 electrode adhesion samples at various temperatures and quenching rates. Based on the interface performance data and the elastic–viscoplastic material model of the PEO–LiTFSI electrolyte, a comprehensive electrochemical–mechanical model was established to analyze the stress in the cell and evaluate the mechanical integrity of the PEO16–LiTFSI electrolyte and SPE/cathode interface. The experimental results show that the adhesion strength of the SPE and cathode decreases significantly with increasing operating temperature and quenching rate. The simulation study indicates that the mechanical properties of the SPE can be fully utilized to a certain extent by increasing the quenching rate. In addition, appropriately increasing the operating temperature helps maintain the mechanical integrity of the SPE during cell operation. However, increasing the quenching rate and operating temperature will reduce the interface bonding properties between the SPE and the cathode, resulting in an increased probability of mechanical failure at the SPE/cathode interface. To suppress this negative effect, a design scheme to maintain the structural integrity of the PEO-based polymer electrolyte is proposed by using the C-rate and the SPE thickness as control parameters, which can assist in engineering design and safe operation of Li/PEO16–LiTFSI/LiFePO4 for ASSLBs.
研究领域:
材料科学
·
电化学
·
固态电池
·
机械工程
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Qingqing Zhou,Chuyang Li,Bin Wang,Wenwei Ding,Junjie Lu,Bifu Sheng,Wei Li,Wenjuan Zhu,Qian Ni,Xiang Han
Polyethylene oxide (PEO)-based solid-state batteries have attracted extensive attention due to their scalable processing, flexible and soft interface contact, and excellent compatibility with lithium metal. The low ionic conductivity at room temperature, caused by the strong interaction between PEO chains and lithium ions , however, limits its practical application. Herein, taking the PEO-PAN dual-matrix polymer electrolyte as an example, a weak coordinated solvation structure is enabled by fluoroethylene carbonate (FEC) as a co-solvent during electrolyte preparation. The tiny residual FEC is demonstrated to weaken the interaction between lithium ions and PEO chains while competitively dissociating lithium salts with the residual solvent and anions. In addition, the incorporation of FEC enhances the dispersion of LATP nanoparticle fillers, which reduces the crystallinity of PEO. Furthermore, the anion-derived LiF-rich solid-electrolyte interphase significantly suppresses the formation of lithium dendrites. Consequently, the prepared PEO-PAN-LATP-LiTFSI-5 % FEC (PPLLF) composite solid polymer exhibits an ambient ionic conductivity of ∼ 1 × 10 −4 S cm −1 and enables stable cycling for over 450 h in a Li||Li symmetrical battery at room temperature. The assembled Li|PPLLF|LFP full battery delivers a specific capacity of 137.6 mAh/g after 300 cycles at 0.2C, further demonstrating the effectiveness of the solvation manipulation strategy.
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF POLYMER RESEARCH
·
2012
·Vol. 19
·期 11
·1-7
·
IF 1.733
Yu Wei-Na,Liu Shou-Xin,Wang Hong-Mei,Tian Rong
Temperature-responsive P(NIPAM- co -HMAM)- b -PEO- b -P(NIPAM- co -HMAM) triblock copolymers were synthesized by an atomic transfer radical polymerization (ATRP) method without freeze–pump–thaw cycles. The composition, structure, and molecular weight of the synthesized block copolymer were characterized by 1 H NMR and GPC. The phase transitions induced by temperature for different copolymers in dilute aqueous solutions have been studied using transmittance measurements, laser particle size measurements, viscosity analysis, and surface tension measurement, which showed that the HMAM content and the PEO (or PEG) chain length in the synthesized triblock copolymer affects the copolymer’s lower critical solution temperature (LCST). The micellization behavior of each temperature-responsive triblock copolymer was investigated by fluorescence probe measurements and transmission electron microscopy (TEM), which showed that the triblock copolymers form stable micelles above the LCST. The introduction of the HMAM component and the formation of micelles represent the first steps in the development of an injectable gel that forms in situ through chemical and physical crosslinking.
研究领域:
高分子化学
·
生物材料
·
药物递送系统
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DOI
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2024
·Vol. 141
·期 44
·e56156
·
IF 2.7
Hao Sun,Qinghua Yang,Detao Kong,Yanrui Li,Yaolong He,NengHui Zhang,Hongjiu Hu
Polyethylene oxide (PEO)-based solid polymer electrolytes are regarded as promising electrolyte materials because of their safety and flexibility. However, low ionic conductivity at ambient temperature and poor mechanical properties have been a hindrance to its development. In this work, we thermally compressed the PEO-based electrolytes and explored the ionic conductivity, mechanical performance, free volume, and thermal properties of the electrolyte under different thermal pre-compressing strains (TPC-strains). The results show that TPC-strain can significantly improve the ionic conductivity, in-plane strength, stiffness, and cell specific capacity as well as the mechanical integrity of solid polymer electrolytes within the battery environment. However, it also results in a reduction in the modulus and stiffness of the SPEs in the through-plane. In particular, applying a TPC-strain of 10%–20% to the SPEs by thermal compressing may be a suitable option, which can increase the ionic conductivity of the through-plane to a factor of 3.4 compared with the uncompressed electrolyte, and increase the in-plane strength by up to 141%, resulting in better mechanical integrity during charging/discharging processes. At the same time, the compression modulus can be maintained at 80% or higher.
研究领域:
材料科学
·
电化学
·
高分子物理
·
能源存储
·
固态离子学
✓ 已验证
DOI
高影响因子
Coatings
·
2018
·Vol. 8
·期 2
·68
·
IF 2.35
Jia Li,Boxiang Wang,Jie Lin,Dehong Cheng,Yanhua Lu
Multifunctional mulberry silk fabrics with excellent temperature- and pH-sensitivity, antibacterial properties and permeability are successfully prepared by surface modification with PNIPAAm/chitosan/poly(ethylene oxide) nanofibers. The nanofibers deposited on the surface of mulberry silk fabric are produced by the electrospinning technique. The surface properties of mulberry silk fabrics were changed by coating process and glutaraldehyde vapor cross-linking technology. The PNIPAAm/chitosan/PEO nanofibers have good apparent morphology and uniform fiber diameter. The contact angle of modified mulberry silk obviously increases with the increasing temperature. The bacterial reduction rates of modification of mulberry silk againstE. coliandS. aureusall reach above 80%. Permeability test results show that it can largely improve the poor permeability of coated fabric by intelligent nanofiber modification technology. The air permeability of temperature- and pH-sensitivity mulberry silk fabric modified with PNIPAAm/chitosan/PEO nanofibers, which has reached about 5.1 × 102L/m2/s, is higher than that of the silk fabric coated with PNIPAAm/chitosan/PEO solution that reached 1.5 × 102L/m2/s. The nanofibers coated with mulberry silk fabrics show outstanding temperature- and pH-sensitivity, antibacterial properties and permeability, and may be a potential application in medical care, intelligent materials and textiles.Keywords:chitosan;poly(N-isopropyl acrylamide);mulberry silk;electrospinning;antibacterial activity;thermosensitive behavior
研究领域:
材料科学
·
纺织工程
·
生物医学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Youlan Zou,Zhuoran Ao,Zhehao Zhang,Nantao Chen,Haiyan Zou,Yiyang Lv,Yuxing Huang
All-solid-state lithium metal batteries (ASSLMBs) are expected to provide a next-generation solution for energy storage. However, intrinsic low ionic conductivity of PEO-based electrolyte causes inferior capacity seriously hinders their widespread commercial application. Here, a new kind of solid electrolyte is explored by incorporation of PEO with metal–organic framework ZIF-67 to enhance the ionic conductivity to 1 × 10 -4 S cm −1 at room temperature. Lewis acid-base interaction that forms between Co element and TFSI - promotes the dissociation of lithium salt and enhances Li + transport. Moreover, N H bonds of ZIF-67 combine with the lone pair of electrons of O on the PEO segment to form hydrogen bonds (N H…O), reducing the strong interaction between Li + and PEO. The cathode with 6 mg cm −2 of LiFePO 4 loading delivers a high capacity of 129.7 mAhg -1 at 0.1C. Furthermore, the assembled batteries delivered a capacity of 147 mAhg -1 at room temperature after 300 cycles.
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DOI
高影响因子
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