JOURNAL OF POWER SOURCES
·
2019
·
IF 7.467
S.Z. Zhang,X.L. Wang,X.H. Xia,Z.J. Yao,Y.J. Xu,D.H. Wang,D. Xie,J.B. Wu,C.D. Gu,J.P. Tu
Interfacial issues have been the main obstacle to the development of solid-state batteries . In this work, we design a solid hybrid polymer electrolyte based on poly-(ethylene glycol) diacrylate and succinonitrile (PSSE) with a liquid state precursor. An intimate interface between PSSE and Li 4 Ti 5 O 12 @vertical graphene (LTO@VG) electrode with three-dimensional array structure is cleverly constructed by infiltrating fluid precursor of PSSE into vertical pores of LTO@VG followed by polymerization and solidification of PSSE. The quasi-solid-state LTO@VG//PSSE//Li and LiFePO 4 //PSSE//LTO@VG full cells exhibit superior electrochemical performance since the active materials are closely contacted by the conductive skeleton and ion-conductive electrolyte. The LTO@VG//PSSE//Li cells maintain 85.7% capacity retention after 400 cycles at 2 C and the LFP//PSSE//LTO@VG full cells still reach 99.0% capacity retention after 200 cycles at 0.5 C. This novel strategy for interface engineering paves the way for achieving high-performance solid-state batteries.
研究领域:
材料科学
·
电化学
·
能源存储
·
高分子化学
·
纳米材料
·
界面科学
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DOI
高影响因子
Materials Today Energy
·
2023
·
IF 9.3
Canhui Ling,Tuoya Naren,Xinsheng Liu,Jixu Yang,Pengfei Xiao,Weifeng Wei,Xiaobo Ji,Gui-Chao Kuang,Libao Chen
s The polymer electrolytes have become widely reported solid electrolytes in high-energy lithium metal batteries . However, this kind of electrolytes are limited by their tradeoff between ionic conductivity and mechanical strength . In addition, polymer electrolytes usually suffer from cracks or breakage due to the rigid structure. Therefore, these drawbacks have greatly influenced their practical applications in lithium metal batteries. Herein, we developed a novel self-healable polymer electrolyte (SHPE) by in-situ polymerizing the mixture of butyl acrylate and 2-ureido-4-pyrimidinone (UPy) with plastic crystal succinonitrile (SN) and lithium bis (trifuoromethanesulfonyl) imide (LiTFSI), which were premixed to behave as deep eutectic solvent (DES) to enhance the ionic conductivity . We found that SHPE displayed 0.46 mS/cm at 30 °C and its electrochemical window was determined to be 4.7 V. While the low dose of UPy could provide quadruple hydrogen bond to endow the polymer electrolyte with good self-healing capability and increase the polymer mechanical strength. Therefore, the symmetrical Li/Li cell using this SHPE showed stable properties as long as 1400 h. The Li/LiFePO 4 cell revealed good capacity retention (93.8%, 140.6 mAh/g) after 300 cycles at 0.2C. This work may provide a promising strategy to develop high-performance polymer electrolytes for lithium metal batteries.
研究领域:
材料科学
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电化学
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能源存储
·
高分子化学
·
固态电解质
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DOI
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Batteries-Basel
·
2025
·Vol. 11
·期 9
·334
·
IF 4.8
Fei Zhou,Jinwei Tan,Feixiang Wang,Meiling Sun
All-solid-state lithium batteries (ASSLBs) employing Li-rich layered oxide (LLO) cathodes are regarded as promising next-generation energy storage systems owing to their outstanding energy density and intrinsic safety. Polymer-in-salt solid electrolytes (PISSEs) offer advantages such as high room-temperature ionic conductivity, enhanced Li anode interfacial compatibility, and low processing costs; however, their practical deployment is hindered by poor oxidative stability especially under high-voltage conditions. In this study, we report the rational design of a bilayer electrolyte architecture featuring an in situ solidified LiClO4-doped succinonitrile (LiClO4–SN) plastic–crystal interlayer between a Li1.2Mn0.6Ni0.2O2(LMNO) cathode and a poly (vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)-based PISSE. This PISSE/SN–LiClO4configuration exhibits a wide electrochemical stability window up to 4.7 V vs. Li+/Li and delivers a high ionic conductivity of 5.68 × 10−4S cm−1at 25 °C. The solidified LiClO4-SN layer serves as an effective physical barrier, shielding the PVDF-HFP matrix from direct interfacial contact with LMNO and thereby suppressing its oxidative decomposition at elevated potentials. As a result, the bilayer polymer-based cells with the LMNO cathode demonstrate an initial discharge capacity of ∼206 mAh g−1at 0.05 C and exhibit good cycling stability with 85.7% capacity retention after 100 cycles at 0.5 C under a high cut-off voltage of 4.6 V. This work not only provides a promising strategy to enhance the compatibility of PVDF-HFP-based electrolytes with high-voltage cathodes through the facile in situ solidification of plastic interlayers but also promotes the application of LMNO cathode material in high-energy ASSLBs.
研究领域:
储能与转换
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材料科学
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电化学
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高分子科学
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锂离子电池
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DOI
高影响因子
Advanced Energy Materials
·
2023
·Vol. 13
·期 16
·2204036
·
IF 27.8
Su Wang,Qifang Sun,Qing Zhang,Chen Li,Chaoran Xu,Yue Ma,Xixi Shi,Hongzhou Zhang,Dawei Song,Lianqi Zhang
The low ionic conductivity and short service life of solid polymer electrolytes (SPEs) limit the application of ambient-temperature polymer lithium metal batteries, which is perhaps a result of the inherent restricted segment movement of the polymer at room temperature. Herein, an ambient-temperature dual-layer solid polymer electrolyte is developed and the related working mechanisms are innovatively investigated. In the strategy, poly(propylene carbonate) (PPC)/succinonitrile (SN) contacts with the cathode while polyethylene oxide (PEO)/Li 7 La 3 Zr 2 O 12 is adopted near the anode. Molecular dynamics simulations demonstrate the formation of solvated sheath-like structure [SN···Li + ], which demonstrates strong interaction with polymers (PPC···[SN···Li + ]/PEO···[SN···Li + ]). Further density functional theory calculations show that these structures, allow rapid transport of Li ions through polymer segments. These results are confirmed with Fourier transform infrared spectroscopy and nuclear magnetic resonance. Therefore, the Li-ion transport mechanism for ambient-temperature SPEs can be reasonably revealed. Remarkably, the binding energy between PPC and SN is stronger than that of PEO, which helps avoid the parasitic reaction between SN and Li. A low overpotential of 55 mV is exhibited for Li/Li symmetrical cells after 1000 h. Notably, a capacity retention of 86.3% is maintained for LiNi 0.6 Co 0.2 Mn 0.2 O 2 /Li cell at 25 °C, implying good application potential in ambient-temperature high voltage lithium metal batteries.
研究领域:
材料科学
·
电化学
·
储能技术
·
高分子物理
·
电池技术
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Guang Chen,Shun-Ran Peng,Ying Du,Wei Liu,Zhe Wang,Zong-Bin Lu,Fan Gao,Wei-Qiang Huang,Long-Hai Wang,Chun-Yan Hong,Ze Zhang,Ye-Zi You
Solid polymer electrolytes (SPEs) play a crucial role in solid-state lithium metal batteries (LMBs), offering smooth interfacial contact with the electrodes. Among these, polyethylene glycol (PEG)-based polymers are particularly effective at dissociating lithium salts and generating mobile Li+ ions. However, the strong binding between Li+ and PEG, coupled with slow polymer segmental motion, significantly limits the Li+ transport. Achieving rapid Li+ transport by modulating the Li+-PEG interaction is crucial but remains challenging for developing high-performance polymer electrolytes. Here, we introduce trimethylamine oxide (TMAO), a biologically derived osmotic agent, into a solid polymer electrolyte to reshape the Li+-PEG interaction for promoting Li+ transport. TMAO can effectively coordinate with Li+ through its highly negatively charged oxygen atom and reverse the PEG’s polarization induced by Li+, thereby weakening the Li+-polymer binding. This process significantly enhances the ionic conductivity (1.07 mS cm–1, 25 °C) and improves the cycling stability of lithium metal batteries with LiNi0.6Co0.2Mn0.2O2 cathodes (96% capacity retention over 300 cycles). This work provides a perspective for promoting Li+ transport in SPEs, advancing the performance of solid-state batteries.
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PubMed
高影响因子
TRIBOLOGY INTERNATIONAL
·
2025
·
IF 6.9
Hongyu Liang,Qilin Yang,Shijing Zou,Cheng Yang,Jiahui Li,Xu Fang,Hanlin Zheng,Yongfeng Bu
Deep eutectic solvents (DES) based on hydrogen bonding are a key class of liquid superlubricious materials, with the typical binary DES composed of choline chloride and ethylene glycol. However, the limitations of conventional binary designs and their hydrogen bond acceptors/donors have hindered the development of advanced and sustainable superlubricious materials. This study introduces a novel ternary DES comprising the organic ligands 2-pyrrolidinone (PD) and succinonitrile (SN) combined with lithium bis(trifluoromethanesulfonyl)imide (LiTFSI). Compared to the base lubricant (LP 1:3 ) with a single ligand (PD), the optimized system with two ligands (LPS 1:3:3 ) demonstrates superlubricity, achieving an ultralow coefficient of friction (∼0.007) and high load-bearing capacity (469 MPa). Competitive coordination between PD, SN, and Li + reduces viscosity and enhances the asymmetric contact probability of size-expanded liquid clusters, forming ultra-low shear sliding interfaces. Additionally, replacing water molecules with organic molecules in the Li + solvation shell improves resistance to various humidity levels. This study highlights the role of size-distribution-expanded clusters and adsorbed films in intensifying the ligand competition-induced asymmetric contact effect, providing fresh insights into the design of next-generation multivariate DES superlubricious materials.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yuxue Sun,Man Wang,Xiaorong Zhang,Haiming Xie,Jun Liu
Gel polymer electrolytes (GPEs) combine polymer matrix with plasticizer to enhance safety and ionic conductivity . However, the use of nitrile-based plasticizers in lithium metal batteries (LMBs) is constrained by their poor interfacial stability with lithium metal. Here, we propose a novel nitrile plasticizer , cyclopentane-1,1-dicarbonitrile (CPDCN), which employs a triangular coordination mechanism with Li + through its dual cyano groups . This configuration minimizes free cyano group accumulation at the lithium metal anode (LMA) interface, effectively suppressing parasitic reactions. Furthermore, the fully substituted α-position structure of CPDCN eliminates the reaction of α‑hydrogen (α-H) with lithium metal. The resulting GPE (denoted as PCNE), fabricated from poly(vinylidene fluoride- co -hexafluoropropylene) (PVDF-HFP) and CPDCN, demonstrates exceptional compatibility with LMA, enabling stable lithium plating/stripping for over 550 h in Li|PCNE_50|Li symmetric cells without additives. The LiFePO 4 |PCNE_50|Li cell delivers an initial discharge capacity of 156.4 mAh g −1 at 0.2C and retains 80% capacity after 750 cycles. Meanwhile, high-voltage LMBs using LiNi 0.6 Co 0.2 Mn 0.2 O 2 (NCM622) cathode achieve 95.9% capacity retention after 200 cycles at 0.1C. This work presents a practical molecular structural design for nitrile-based electrolytes with improved lithium metal compatibility.
研究领域:
电化学
·
能源材料
·
高分子科学
·
锂离子电池
·
电池技术
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Shiyu Cao,Zhenyu Fu,Bokang Liu,Yawen Wu,Qiang Shen,Fei Chen
Succinonitrile (SN)-based plastic crystal electrolytes (PCEs) show great potential for solid-state batteries, but their practical application is limited by poor interfacial stability with lithium metal anodes. To address this critical challenge, an asymmetric bilayer composite electrolyte was designed, which consists of a porous PVDF-SN-LiTFSI-LiDFOB (PSTD) catholyte ensuring fast Li + transport, and a dense PVDF-LLZO-LiTFSI (PLT) anolyte serving as a robust protective layer. Notably, the PLT anolyte acts not only as a physical barrier against Li dendrites but also as a chemical buffer that facilitates the in-situ formation of a robust, tailored SEI from migrant additives, synergistically suppressing harmful side reactions. The resulting bilayer electrolyte exhibits a high ionic conductivity of 3.1 × 10 −4 S cm −1 at 30 °C and a wide electrochemical window of 4.85 V. As a result, the LFP/Li cells demonstrate excellent long-term cycling stability, delivering a high discharge capacity of 144.8 mAh g −1 and a retention rate of 95.9 % after 500 cycles at 1 C and 30 °C.
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高影响因子
CHINESE JOURNAL OF POLYMER SCIENCE
·
2026
·
IF 4
Chen Shuai-Jun,Huang Biao,Song Li-Xin,Wang Zha,Du Ping-Fan,Xiong Jie,Zhu Hai-Lin,Guo Yu-Hai
Solid polymer electrolytes (SPEs) are considered promising candidates for all-solid-state lithium metal batteries because of their easy preparation and good compatibility with lithium metal. However, their applications are restricted by their low ionic conductivity and poor mechanical properties. In this study, a composite solid polymer electrolyte composed of poly(ethylene oxide) (PEO), poly(vinylidene fluoride- co -hexafluoropropylene) (PVDF-HFP), plasticizer succinonitrile (SN), and polytetrafluoroethylene (PTFE) fibrous porous membranes was prepared. The PTFE fibrous membrane significantly enhanced the mechanical strength of the electrolyte as a supporting framework. SN reduced the crystalline regions of PEO and facilitated rapid lithium-ion transport. PVDF-HFP promoted lithium salt dissolution and improved the electrochemical stability of the electrolyte. Accordingly, the optimized PTFE/PEO/PVDF-HFP/SN polymer electrolyte exhibited a tensile strength of 3.31 MPa at 352% elongation and demonstrated an ionic conductivity of 7.6×10 −4 S·cm −1 at 60 °C. Lithium symmetric cells maintained stable cycling for over 2500 h at 0.15 mA·cm −2 , and Li//LiFePO 4 full cells showed a high capacity retention of 91.6% after 300 cycles at 0.5 C, with coulombic efficiency consistently exceeding 99.9% throughout cycling.
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高影响因子
ACS Nano
·
2026
·Vol. 20
·期 32
·22475-22484
·
IF 17.3
Yao Zhengyin,Ma Jiucheng,Yan Sanjing,Yu Shun,Röding Magnus,Liu Hanwei,Yang Chunzhen,Jiao Xuechen,Sun Dongbai,Zhang Peng
Highly concentrated electrolytes often exhibit a counterintuitive
combination of reduced bulk ionic conductivity and markedly improved
cycling stability in metal batteries, yet the structural origin of
this long-standing trade-off remains poorly understood. Here, using
the lithium bis(trifluoromethanesulfonyl)imide (LiTFSI)-succinonitrile
(SN) deep-eutectic electrolyte as a model system, we establish a direct
structure–property framework that reconciles transport kinetics
with electrochemical durability across different concentration regimes.
By integrating synchrotron small- and wide-angle X-ray scattering
with vibrational spectroscopy, electrochemical characterization, and
machine-learning-assisted mesoscale reconstruction, we resolve how
ionic organization evolves from locally mobile, weakly correlated
environments to salt-rich, structurally constrained networks. We show
that the highest ionic conductivity at intermediate concentration
arises from optimally connected mesoscale pathways that facilitate
fast ion transport, whereas higher salt concentration induces a TFSI – -dominated solvation framework with partial salt ordering
that suppresses bulk transport but stabilizes long-term cycling and
Coulombic efficiency. These findings suggest that the electrochemical
behavior of concentrated electrolytes is closely associated with concentration-induced
ionic organization, structural heterogeneity, and interphase stabilization
rather than conductivity alone. The results provide a structural perspective
for understanding the apparent performance paradox of salt-rich electrolytes
and offer general insights for the design of next-generation battery
electrolytes.
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高影响因子
Nature Communications
·
2026
·
IF 18.1
Xu Xu,Chen Jian,Yang Zhuo,Zhou Zhiming,Zhang Xiaosa,Zeng Xinhui,Wan Yun,Chen Xiaomin,Kuang Wenxi,Shi Xiaoyan,Zhang Lingling,Zhou Xunzhu,Chou Shulei,Li Lin
Acetonitrile-based electrolytes have garnered significant attention for sodium-ion batteries due to their high ionic conductivity and favorable oxidation resistance. However, their practical implementation is hindered by an unsatisfactory anti-reduction ability, leading to poor compatibility with hard carbon anode and, consequently, rapid capacity degradation. Herein, we employ a widely used commercial carbonate ester solvent (ethyl methyl carbonate) to modulate the ion-dipole interactions in fluorine-free acetonitrile-based electrolytes. The relatively weak solvation ability of ethyl methyl carbonate facilitates more anions to participate the inner solvation sheath, thereby promoting the formation of robust electrode-electrolyte interface at a wide temperature range. This stabilized interface effectively suppresses continuous electrolyte decomposition, significantly improving the compatibility between fluorine-free acetonitrile-based electrolytes and hard carbon anodes. As a result, the optimized electrolyte enables stable operation of hard carbon ||Prussian blue full cells over a wide temperature range (25-100 °C), demonstrating a capacity retention of 62.5% after 600 cycles at 55 °C and 1.0 C. It is worth noting that Ampere-hour-level hard carbon ||Prussian blue pouch cells deliver consistent electrochemical performance at both 25 °C and 55 °C. This study elucidates the mechanistic role of cosolvent engineering in enhancing the reductive stability of fluorine-free acetonitrile-based electrolytes and provides a viable electrolyte design strategy for their practical implementation in sodium-ion batteries.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Yuan Liang,Junhao Chen,Zhantao Wu,Chenran Tang,Jiapeng Liu,Dengjie Chen,Jing Yu
The designed rigid-flexible GPEs decouple mechanical robustness and ion transport. • This GPE achieves a skeleton modulus of 125 MPa, thereby suppressing dendrites. • The designed electrolyte regulates Na + solvation to form an inorganic-rich SEI. • This GPE enables fast-charging cells under high voltage and wide temperatures. Gel polymer electrolytes for next-generation sodium-metal batteries (SMBs) are limited by a trade-off between mechanical robustness and ionic conductivity, which hampers fast-charging and wide-temperature applications. Herein, we address this challenge via an innovative rigid-flexible coupled polymer network, specifically synthesized by copolymerizing flexible butyl acrylate (BA) monomers with rigid triallyl isocyanurate (TAIC) crosslinkers. The rigid TAIC framework imparts exceptional mechanical integrity and electrochemical stability, while the polymerized BA matrix effectively confines solvents, enabling efficient ion-transport pathways. Moreover, the polymer network regulates the Na + solvation environment, thereby inducing a stable, inorganic-rich solid electrolyte interphase. The rationally designed electrolyte (pBAT-1/8) achieves an ultrahigh Young's modulus of 40 MPa (125 MPa of the pBAT-1/8 skeleton) to effectively suppress dendrites, while maintaining high ionic conductivities (0.33, 1.58, and 2.11 mS cm −1 at −10, 30, and 70 °C, respectively) and a high Na + transference number (0.51). Consequently, Na|pBAT-1/8|Na demonstrates stable cycling over 1500 h at 0.1 mA cm −2 . Remarkably, Na|pBAT-1/8|Na 3 V 2 (PO 4 ) 3 cells deliver exceptional capacity of 92.7 mAh g −1 at 5C after 2600 cycles and operate reliably under harsh conditions, including high cathode mass loading (10.3 mg cm −2 ), high cut-off voltage (4.5 V), and broad operating temperature range (−10 to 70 °C). This work offers a transformative strategy to decouple mechanical and transport properties for practical high-energy-density SMBs. Download: Download high-res image (130KB) Download: Download full-size image
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高影响因子
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