JOURNAL OF POWER SOURCES
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2019
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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
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电化学
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能源存储
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高分子化学
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纳米材料
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界面科学
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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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JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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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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CHINESE JOURNAL OF POLYMER SCIENCE
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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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ACS Nano
·
2026
·Vol. 20
·期 32
·22475-22484
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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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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
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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
ACS Applied Energy Materials
·
2026
·
IF 5.5
Lu Kun-Rong,Li Dong-Yang,Wang Hong-Yu,Han Yue-Xi,Shi Fa-Nian,Wang Peng-Fei,Zhang Yu-Hang
Polyethylene oxide (PEO)-based polymer electrolytes hold promise for application in solid-state lithium metal batteries. However, the high crystallinity of PEO poses a significant challenge to ion transport, particularly limiting its room-temperature performance. Poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP), a semi-crystalline polymer with rigid fluorocarbon chains, can provide robust mechanical support to the electrolyte system. Herein, a quasi-solid electrolyte (QSE) was fabricated by using PEO and PVDF-HFP, in which succinonitrile (SN) was introduced as a plasticizer to enhance the electrochemical properties at room temperature. Innovatively, 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (TTE) was employed as a shield layer to prevent direct contact between the Li anode and the prepared SN-modified PEO/PVDF-HFP-QSE, thus forming a stable anode/electrolyte interface. The obtained TTE-P 8 P 2 S(12%)-QSE exhibits high room-temperature electrochemical properties, with an ionic conductivity of 4.02 × 10 –4 S cm –1 , a lithium-ion transport number of 0.47, and a wide electrochemical window of 5.4 V vs. Li + /Li. By interfacial modification, TTE-P 8 P 2 S(12%)-QSE can enable long-term cycling of LiCoO 2 cathodes and Li anodes, with an initial discharge capacity of 126.9 mAh g –1 , and achieve an average capacity of 142.8 mAh g –1 within 100 cycles at room temperature. Characterizations reveal that the incorporation of TTE preserves the structural integrity of the lithium electrodes, promotes efficient utilization of active lithium ions, and tailors the composition and structure of the solid-electrolyte interphase (SEI) on the lithium metal anode, thereby substantially enhancing interfacial stability. This work provides a feasible strategy for building high-energy-density lithium metal batteries for room-temperature applications.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Jiacheng Yan,Yuxin Chen,Tuoya Naren,Zhongshen Wang,Antai Zhu,Shaozheng Huang,Bowei Ju,Gui-Chao Kuang,Libao Chen
Deep eutectic solvent (DES) electrolyte, due to its low volatility, flame retardancy and environmental friendliness, has become one of the next-generation electrolytes for lithium metal batteries (LMBs). However, DES has poor compatibility with lithium metal and there is still a risk of leakage, which limits the use of DES in LMBs. The introduction of polymers into the electrolyte is an effective strategy to solve the leakage problem and improve the compatibility of the interface. Here, we report a polymer formed from nitrogen-rich monomers that polymerize in-situ in the flame-retardant DES (1 mol/L LiTFSI in succinonitrile) to form a gel electrolyte (D-TAEA). D-TAEA maintains high ionic conductivity (0.52 mS cm −1 at 30 °C) while effectively inhibiting electrolyte leakage and optimizing interface stability. Benefiting from the synergistic effect of polyurea and tertiary amine groups, D-TAEA exhibits a wide electrochemical window (5.0 V vs Li/Li + ), high Li + migration number (0.69) and excellent cycle performance. Due to the stable SEI formed by D-TAEA and Li electrode, Li/Li symmetrical battery can stably cycle for 800 h, moreover, the capacity retention rate of LiFePO 4 full battery remains at 92.6 % after 300 cycles at 0.1C. Therefore, this three-dimensional cross-linking network provides a new path for the traditional DES system.
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Journal of Energy Chemistry
·
2025
·
IF 14.9
Yufeng Ren,Junhong Guo,Suli Chen,Tianxi Liu
Solid polymer electrolytes (SPEs) are considered one of the most promising materials for all-solid-state lithium metal batteries (ASSLMBs) due to their facile processability. However, developing SPEs with both high ionic conductivity and interfacial stability remains a challenge. Here, a donor-acceptor (D-A) like solid plasticizer, tris(pentafluorophenyl)borane (TPFPB), containing electron-rich F atoms and electron-deficient B sites, was introduced to regulate the ion transport behavior and interfacial chemistry of polyethylene oxide (PEO)-based SPEs. Owing to the multiple ion-dipole interactions (F‧‧‧Li + ‧‧‧TFSI − and B‧‧‧TFSI − ‧‧‧Li + ) between the TPFPB molecule and Li salts, a multimodal electrolyte environment featuring more free Li + and trapped TFSI − anions was generated, which cooperates with the reduced crystallinity of PEO, significantly facilitating the rapid migration of Li + . More importantly, TPFPB tends to be preferentially reduced to form a stable inorganic-rich solid electrolyte interphase on the Li-metal anode, ensuring uniform Li plating/stripping behavior. Thus, the TPFPB-modulated SPEs system achieves a high Li + conductivity of 0.74 mS cm −1 and effectively suppresses dendrite growth, which enables a long-cycle dendrite-free Li/Li symmetric cell for over 5000 h, and remarkable electrochemical performance has been further validated in operational ASSLMBs. The findings in this work would inspire efforts to develop high-performance SPEs for all-solid-state alkali-metal batteries.
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Crystals
·
2022
·Vol. 12
·期 9
·1290
·
IF 2.67
Wanbao Wu,Qing Li,Miaomiao Cao,Deping Li,Jingyu Lu,Mingyu Li,Jiaheng Zhang
The application of high voltage cathode electrode materials is an effective way to increase the energy density of batteries. However, the development and design of a stable electrolyte at high voltages needs to be further addressed. Herein, we developed a non-flammable dual-salt deep eutectic solvent (DES) as a safe electrolyte containing LiTFSI, LiDFOB, and succinonitrile in different molar ratios. This non-flammable DES provides high ionic conductivity (4.23 mS cm−1) at 25 °C, high Li+transference number (0.75), and wide electrochemical stability (>5.5 V). When using the designed DES electrolytes in high voltage LiCoO2||Li cells, superior electrochemical performance was achieved at cut-off voltages of 3.0–4.45 V and 3.0–4.6 V, even at a high current density of 2 C. This work offers an in-depth understanding of the critical role of dual-salts in DES and provides an approach to designing safe electrolytes for high voltage LiCoO2||Li cells.Keywords:non-flammable;high Li+transference number;deep eutectic solvent;high voltage LCO;lithium metal battery
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Yang Xia,Qiyue Wang,Yaning Liu,Jun Zhang,Xinhui Xia,Hui Huang,Yongping Gan,Xinping He,Zhen Xiao,Wenkui Zhang
The replacement of traditional liquid electrolytes with polyethylene oxide (PEO) based composite polymer electrolytes (CPEs) is an important strategy to address the current flammability and explosiveness of lithium batteries since PEO CPEs have high flexibility, excellent processability and moderate cost. However, the insufficient ionic conductivity and inferior mechanical strength of PEO CPEs do not suit the operating requirements of all-solid-state lithium metal batteries at room temperature. Herein, three-dimensional (3D) framework composed of interweaved high-modulus polyimide (PI) nanofibers along with functional succinonitrile (SN) plasticizers are employed to synergistically reinforce the ionic conductivity and mechanical strength of PEO CPEs. Impressively, benefitting from the synergistic effects of 3D PI framework and SN plasticizer, PI-PEO-SN CPEs exhibits high ionic conductivity of 1.03 × 10 −4 S cm −1 at 30 °C, remarkable tensile strength of 4.52 MPa, and superior Li dendrites blocking ability (>400 h at 0.1 mA cm −2 ). Such favorable features of PI-PEO-SN CPEs endow LiFePO 4 /PI-PEO-SN/Li solid-state prototype cells with high specific capacity (151.2 mA h g −1 at 0.2 C), long cycling lifespan (>150 cycles with 91.7 % capacity retention), and superior operating safety even under bending, folding and cutting harsh conditions. This work will pave the avenues to design and fabricate new high-performance PEO CPEs for the high energy density and safety all-solid-state batteries.
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高影响因子
危险品化学品经营许可证（带存储）