JOURNAL OF APPLIED POLYMER SCIENCE
·
2026
·
IF 3.1
Haihua Wang,Haonan Wang,Kewei Shu,Chaoxian Chen,Qing Liu,Rui Cao,Jiaheng Li,Xing Yang,Zhuyu Li
Owing to its high lithium-ion conductivity, the cubic garnet-phase material Li 7 La 3 Zr 2 O 12 (LLZO) is a widely adopted key component in the fabrication of composite solid-state electrolytes (CSSEs). Nevertheless, the advancement of all-solid-state lithium batteries (ASSLBs) is still hindered by two major challenges: the high intrinsic crystallinity of poly(ethylene oxide) (PEO) and poor interfacial stability. Herein, cubic garnet Li 6.3 La 2.7 Ba 0.3 ZrNbO 12 (LLBZNO) featuring Ba and Nb co-doping was first prepared by a conventional solid-state method. Following this, the material was dispersed within a PEO matrix to construct composite solid-state electrolytes. Adding LLBZNO served to decrease PEO's crystallinity while enhancing its mechanical flexibility and bolstering its interfacial compatibility with lithium metal. The optimized membrane demonstrated superior properties, including a high Li + transference number of 0.75 (at 60°C) and an extended electrochemical stability window of up to 5.1 V (vs. Li/Li + ) under the present testing conditions. It also showed an excellent ability to suppress dendrites, facilitating stable cycling at 0.1 mA cm −2 for 1500 h without short-circuiting. Furthermore, the LFP/LLBZNO–PEO/Li battery delivered a high discharge capacity of 101.6 mA h g −1 after 300 cycles at 1°C with nearly 99% coulombic efficiency. These findings highlight that LLBZNO-PEO composite solid electrolytes possess superior ionic transport, electrochemical stability, and mechanical robustness, providing a viable pathway toward the advancement of next-generation high-performance ASSLBs.
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DOI
高影响因子
ENERGY & FUELS
·
2026
·Vol. 40
·期 35
·19765-19777
·
IF 6
Yang Zhitao,Liu Yulei,Fu Xiuwen,Xu Weiheng,Liu Jinpeng
Poly(ethylene oxide) (PEO)-based solid polymer electrolytes
are
promising for solid-state lithium metal batteries because of their
favorable flexibility, processability, and lithium-salt solvation
capability. However, their practical application is still limited
by insufficient ion transport, a low lithium-ion transference number,
and poor lithium-metal interfacial stability. Herein, dual-lithium-salt-regulated
composite polymer electrolytes (DSCPEs) were constructed by incorporating
a LiTFSI/LiDFOB dual-salt system into a PEO–LLZTO composite
polymer electrolyte matrix to achieve a balance between ion transport
capability and lithium-metal interfacial stability. The optimized
DSCPE-2 (LiTFSI:LiDFOB = 3:2) delivers an ionic conductivity of 6.63
× 10 –4 S cm –1 , a lithium-ion
transference number of 0.69, and an electrochemical stability window
of up to 5.1 V. In addition, the Li|DSCPE-2|Li symmetric cell operates
stably for over 2000 h at 60 ° C under 0.1 mA cm –2 , with a critical current density of 1.05 mA cm –2 , indicating its enhanced compatibility with lithium metal. When
assembled with a LiFePO 4 cathode, the Li|DSCPE-2|LFP full
cell delivers an initial discharge capacity of 136.54 mAh g –1 and retains 123.41 mAh g –1 after 300 cycles at
0.5 C and 60 ° C, corresponding to a capacity retention of 90.38%.
Furthermore, the cell maintains a reversible capacity of approximately
115 mAh g –1 even at 5 C. This work provides an effective
strategy for regulating ion transport behavior and lithium–metal
interfacial stability in PEO-based composite polymer electrolytes.
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高影响因子
IONICS
·
2025
·
IF 2.6
Xiong Zhen-Yu,Wang Guan-Hua,Wang Hong-Yu,Li Peng-Yuan,Sun Yang,Ma Yu-Han,Guo Tao,Shi Fa-Nian,Zhang Yu-Hang
Polyethylene oxide (PEO) is regarded as the most promising candidate for the next generation solid polymer lithium metal batteries (LMBs). However, it suffers from low mechanical strength and limited electrochemical stability window (ESW), which restricts its application in high energy density LMBs. In this work, polycaprolactone (PCL) is chosen as the main matrix to fabricate a blending polymer-based electrolyte with PEO, which shows an improved electrochemical performance with a high lithium ion transference number of 0.65. The improvement can be attributed to the competition between ester and ether groups of different polymer chains, which can both interact with lithium ions to release more free cations. Moreover, the high-voltage resistance of PCL can broaden the electrochemical stability window to 4.8 V of PCL/PEO solid electrolyte to match LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) cathode, and its high-temperature resistance ensure a satisfying dimensional stability for the assembled NCM811||Li cell to operate at 55 ℃, with a high initial specific capacity of 210 mAh/g and a retention of 95% within 100 cycles. Compared to other blending systems, the PCL/PEO blend exhibits superior compatibility, mechanical properties, and electrochemical stability, offering a promising strategy for the commercialization of high-voltage, safe, and high-energy-density solid-state lithium metal batteries operable at elevated temperatures.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Longfei Han,Junling Wang,Xiaowei Mu,Tao Wu,Can Liao,Na Wu,Weiyi Xing,Lei Song,Yongchun Kan,Yuan Hu
Poly (ethylene oxide) (PEO) polymer electrolyte , attracts great attention owing to its excellent flexibility, good processability and high safety compared with liquid electrolytes . However, its low ionic conductivity and weak ability to suppress the lithium dendrite severely restrict the further progress of PEO . Herein, we prepare a high ionic conductivity solid polymer electrolyte for all-solid-state lithium batteries by mixing PEO and magnetically aligned functionalized sepiolite (KFSEP) nanowires. The ionic conductivity of PEO/LiTFSI/10%⊥KFSEP solid polymer electrolyte is 2.0 × 10 −5 S cm −1 at 20 °C (The ionic conductivity of PEO/LiTFSI solid polymer electrolyte is 4.0 × 10 −7 S cm −1 at 20 °C). The experiments and simulation analysis indicate that the aligned nanowires provide a fast-moving channel for lithium ions . The capacity of Li/PEO/LiTFSI/10%⊥KFSEP/LFP cell is 130 mAh g −1 at 1.0 C under 60 °C after 450cycles. Furthermore, Li/PEO/LiTFSI/10%⊥KFSEP/LFP cell shows 150 mAh g −1 at 0.2 C under 25 °C. The Li/PEO/LiTFSI/10%⊥KFSEP/Li cell can work normally more than 600 h, indicating the high stability and lithium dendrite suppressing function of PEO/LiTFSI/10%⊥KFSEP. Overall, a high performance solid polymer electrolyte with higher safety is constructed by incorporating magnetically aligned sepiolite nanowires into PEO.
研究领域:
材料科学
·
电化学
·
能源存储
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DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Yubing Guo,Ming Zhang,Zhen Ge,Zixuan Fang,Ziqiang Xu,Jintian Wu,Mengqiang Wu
Polyethylene oxide (PEO)-based solid polymer electrolytes exhibit promising commercial prospects due to their superior processability and scalability. However, limited ion transport and unstable electrode/electrolyte interface restrict their practical application. Herein, the paraelectric strontium titanate (STO) is introduced into PEO-based electrolytes to solve those problems. The electrostatic force originating from polarized STO weakens the coordination between EO and Li + and releases more free Li + , thus promoting ion transport inside the electrolyte. Numerous STOs form a new reverse electric field that inhibits lithium dendrites' vertical growth at the anode interface. Polarized STO triggers the generation of LiF, Li 2 O, and Li 3 N-riched solid electrolyte interphase (SEI), contributing to interfacial stability and Li + mobility. Consequently, polarized STO-modified PEO-based solid electrolyte has an outstanding ion conductivity of 0.61 mS cm −1 with a superior lithium stability of 5.29 V. Li/Li symmetric battery with STO-modified electrolyte undergoes >1200 h at 0.2 mA cm −2 . A large capacity retention of 85.3% after 850 cycles at 1 C is achieved for LFP/Li battery and be cycled 600 times even against a high-loading cathode (LFP:6 mg cm −2 ). This study provides a novel strategy to prepare composite-modified solid-state electrolytes that can be utilized in lithium metal batteries.
研究领域:
材料科学
·
电化学
·
能源存储
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DOI
高影响因子
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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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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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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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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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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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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高影响因子
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