CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yaqi Zhang,Pengbin Lai,Xiaodie Deng,Peng Zhang,Jinbao Zhao
Designing suitable electrolytes and interphases is crucial for lithium metal batteries (LMBs), which are susceptible to excessive side reactions and lithium dendrite at the anode. Regulating the solvation ability of solvents and anions to tune the solvation structure and constructing an appropriate solid electrolyte interphase (SEI) are effective strategies for these problems. Herein, two different dissociated lithium salts (LiTFSI and LiBF 4 ) are screened to study the anion-oriented solvation regulation for SEI formation at the anode. It is found that BF 4 - is less likely to be displaced from the inner layer by solvents compared to TFSI - . Moreover, the resulting SEI with either an overly high or low content of inorganic components is not advantageous for long-term cycling performance. On the contrary, the dual salt electrolyte not only preferentially decomposes to form protective and balanced SEI with low impedance, but also maintains favorable bulk ion transport down to − 40 ℃. As a result, 4.3 V Li||LiCoO 2 full cells using the dual salt electrolyte deliver 88.7 % capacity retention after 200 cycles at 1C. This work highlights the significance of anion-oriented regulation in optimizing the performance of LMBs.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Materials Letters
·
2021
·
IF 8.312
Tao Li,Yan Li,Yiling Sun,Zhengfang Qian,Renheng Wang
Localized high-concentration electrolytes (LHCEs) have captured considerable attention, since they retain the merits of high-concentration electrolytes while circumventing the disadvantages of high viscosity and high costs. Herein, a systematic comparison between two representative LHCEs (i.e., dimethyl carbonate (DMC)-based LHCE and 1,2-dimethoxyethane (DME)-based LHCE) in high-voltage Li metal batteries was performed. The results showed that DME-based LHCE possesses better compatibilty with Li metal anodes than DMC-based LHCE, and the underlying mechanism is clarified from the point of solid electrolyte interphase (SEI) formation. The two representative LHCEs showed comparable reductive stability, while Li+–DME showed better reductive stability than Li+–DMC. This means the more prominent decomposition of anions in DME-based LHCE, since SEI is derived from the competitive decomposition products of solvents and anions, which is further verified by the more-complete anion decomposition products found in SEI formed in DME-based LHCE. The inorganic-rich SEI with superior passivating ability is reponsible for the good compatibility of DME-based LHCE with Li metal anodes. The findings in this study provides fresh understandings on the stable nature of ether-based LHCE with Li metal anodes, which can serve as guidelines for advanced electrolytes engineering.
研究领域:
材料科学
·
电化学
·
能源存储技术
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-15
·
IF 15.7
Li Wenbin,Duan Yijie,Ge Shaohua,Wu Wenbo,Song Keming,Zhang Jiyu,Tang Guochuan,Zhao Lingfei,Yan Pengfei,Wang Enhui,Zhang Zhiguo,Cao Yuliang,Yang Yong,Chen Weihua
The unstable electrolyte–electrode interface and the trace H 2 O in commercial organic electrolytes critically limit the cycling life of batteries. Herein, a locking-chain sodium 4,4′-(1,4-phenylenebis(oxy))-bis(butane-1-sulfonate)−15-crown-5 (15PBS) is designed for phase-to-interface electrolyte optimization. In the electrolyte phase, the strong hydrophilic sulfonate groups and 15-crown-5 in 15PBS effectively transform H 2 O from a reactive aggregated state (strong H-bond) into an inactive state (weak H-bond) through adsorption, effectively suppressing H 2 O-induced electrolyte decomposition. At the electrolyte–electrode interface, 15PBS preferentially adsorbed onto hard carbon, displacing solvents within the electric double layer to form insoluble phenyl-rich sulfide solid electrolyte interphase with fast Na + transport. Simultaneously, 15PBS facilitates the formation of stable cathode-electrolyte interphase on Na 0.72 Ni 0.32 Mn 0.68 O 2 , improving Na + migration kinetics and cycling reversibility. The hard carbon | |Na 0.72 Ni 0.32 Mn 0.68 O 2 full cell with high specific energy of 191.7 Wh kg −1 (based on the total active-material mass) delivers long lifespan of 2000 cycles at 500 mA g −1 . Moreover, 15PBS is compatible with ester-based electrolytes in lithium-ion batteries, enabling stable cycling of commercial graphite and Si/C negative electrodes. This work provides an effective approach for durable electrolytes towards safe and high-performance batteries.
研究领域:
电化学
·
能源材料
·
电池技术
·
界面化学
·
应用化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Small
·
2025
·
IF 12.1
Xiangxiang Chen,Junru Wu,Wentao Zhang,Ji Li,Ziyao Gao,Xu Zhao,Kuang Yu,Yan-Bing He,Baohua Li,Feiyu Kang,Lele Peng
Constructing robust solid-electrolyte interphase (SEI) on electrodes is crucial for achieving stable lithium metal batteries in liquid electrolytes. However, intrinsic issues associated with liquid electrolytes remain unavoidable, such as the continuous corrosion of SEI and the high costs involved. Herein, a novel lithium salt-free solid-state polymer electrolyte (SPE) is introduced enabled by in situ polymerization of 1,3-dioxolane and 1,3,5-trioxane with the addition of ionic liquid to eliminate the drawbacks of liquid electrolyte. The homogeneous interaction between the polymer and ionic liquid constructs a synergistic Li + conduction pathway, promoting the extraction of Li + out of the cathode/anode and the smooth transport throughout the polymer network to endow a higher Li + transference number (0.63) and a comparable ionic conductivity (1.21 mS cm −1 ) to the conventional liquid electrolyte (0.45 and 5.51 mS cm −1 ). The absence of lithium salt prevents the oxidative decomposition of lithium salts in electrolytes to generate hazardous and corrosive acidic species. More intriguingly, an anion-dominated solvation configuration can be realized by the incorporation of ionic liquid with the polymer matrix, inducing the formation of an inorganic-rich and anti-corrosive SEI on the electrodes. The resulting salt-free SPE enables superior cycling stability in lithium||LiFePO 4 battery with a high capacity retention of over 92% after 780 cycles.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Advanced Physics Research
·
2025
·
IF 2.8
Jiaxiao Qi,Yongjing Wang,Haixiong Tang,Jiayu Zhao,Yu Hong,Qiong Li,Ming Jiang,Lijie Dong
Solid-state electrolytes (SSEs) are promising for lithium batteries with higher safety, cycling stability, and energy density. Among the various SSEs, solid polymer electrolytes (SPEs) are a highly preferred choice due to their high thermal stability, thin design, and good formability. However, polymer electrolytes have low ionic conductivity, for example, polyethylene oxide (PEO), one of the most dominant polyelectrolyte materials, has a low ionic conductivity at room temperature due to its high crystallinity. Theoretically, increasing the ionic active sites by decreasing its crystallinity is an effective strategy, but this may lead to its inability to form films or poor mechanical strength. In this work, the crystallinity of PEO is reduced by introducing succinonitrile (SN), and solution blow-spun polyacrylonitrile (PAN) fiber film is employed as the skeleton of the SPE to provide good mechanical strength. PEO-LiTFSI-SN/PAN SPEs have a tensile strength of at least 4.5 MPa. To provide more Li + active sites, PEO-LiTFSI-SN/MXene@PAN composite SPEs are fabricated by doping the PAN fibers with MXene rich in functional groups. The specific capacity of the LFP|PEO-LiTFSI-SN/MXene@PAN|Li button cell reaches 134.8 mAh g −1 in the first cycle, and the capacity retention rate of 100 cycles is 75.8% at 0.5 C at room temperature.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED MATERIALS
·
2021
·Vol. 33
·期 42
·2102134
·
IF 30.849
Yi-Hong Tan,Gong-Xun Lu,Jian-Hui Zheng,Fei Zhou,Mei Chen,Tao Ma,Lei-Lei Lu,Yong-Hui Song,Yong Guan,Junxiong Wang,Zheng Liang,Wen-Shan Xu,Yuegang Zhang,Xinyong Tao,Hong-Bin Yao
Electrolyte engineering via fluorinated additives is promising to improve cycling stability and safety of high-energy Li-metal batteries. Here, an electrolyte is reported in a porous lithium fluoride (LiF) strategy to enable efficient carbonate electrolyte engineering for stable and safe Li-metal batteries. Unlike traditionally engineered electrolytes, the prepared electrolyte in the porous LiF nanobox exhibits nonflammability and high electrochemical performance owing to strong interactions between the electrolyte solvent molecules and numerous exposed active LiF (111) crystal planes. Via cryogenic transmission electron microscopy and X-ray photoelectron spectroscopy depth analysis, it is revealed that the electrolyte in active porous LiF nanobox involves the formation of a high-fluorine-content (>30%) solid electrolyte interphase layer, which enables very stable Li-metal anode cycling over one thousand cycles under high current density (4 mA cm −2 ). More importantly, employing the porous LiF nanobox engineered electrolyte, a Li || LiNi 0.8 Co 0.1 Mn 0.1 O 2 pouch cell is achieved with a specific energy of 380 Wh kg −1 for stable cycling over 80 cycles, representing the excellent performance of the Li-metal pouch cell using practical carbonate electrolyte. This study provides a new electrolyte engineering strategy for stable and safe Li-metal batteries.
研究领域:
材料科学
·
电化学
·
储能
·
电池技术
✓ 已验证
DOI
高影响因子
Nano Research
·
2020
·Vol. 13
·期 9
·2431-2437
·
IF 8.183
Wang Zijian,Yang Kai,Song Yongli,Lin Hai,Li Ke,Cui Yanhui,Yang Luyi,Pan Feng
Lithium (Li) metal is one of the most promising anodes for next-generation energy storage systems. However, the Li dendrite formation and unstable solid-electrolyte interface (SEI) have hindered its further application. Lithium nitrate (LiNO 3 ) is extensively used as an effective electrolyte additive in ether-based electrolytes to improve the stability of lithium metal. Nevertheless, it is rarely utilized in carbonate electrolytes due to its low solubility. Here, a novel gel polymer electrolyte (GPE) consisting of poly(vinylidene fluoride) (PVDF), poly(methyl methacrylate) (PMMA), poly(ethylene oxide) (PEO) with LiNO 3 additive is proposed to solve this issue. In this GPE, polyether-based PEO serves as a matrix for dissolving LiNO 3 which can be decomposed into a fast Li-ion conductor (Li 3 N) in conventional carbonate electrolytes to enhance the stability and Li + conductivity of the SEI film. As a result, dendrite formation is effectively suppressed, and a significantly improved average Coulombic efficiency (CE) of 97.2% in Li-Cu cell is achieved. By using this novel GPE coupled with Li anode and LiNi 0.5 Mn 0.3 Co 0.2 O 2 (NMC532), excellent capacity retention of 94.1% and high average CE of over 99.2% are obtained after 200 cycles at 0.5 C. This work presents fresh insight into practical modification strategies on high-voltage Li metal batteries.
研究领域:
电化学
·
材料科学
·
能源存储
·
高分子化学
·
界面化学
·
锂电池技术
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Haifeng Tu,Linge Li,Yuzhen Hu,Yongyi Zhang,Yongjiang Wang,Wei Huang,Zhiqiang Ren,Hongzhen Lin,Meinan Liu
Lithium-metal batterie (LMB) is regarded as one the most promising high energy battery systems, however the safety concern from lithium dendrites and organic liquid electrolytes seriously impedes its widely application. Herein, a non-flammable liquid “polymer-in-salt” composite electrolyte with superior dendrite-suppression capability is well designed and achieved by using lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) salt, polyethylene glycol dimethyl ether (PEGDME) and 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropylether (TTE). Non-flammable TTE used here is on one hand to reduce the high viscosity of this “PEGDME polymer in LiTFSI salt” electrolyte (PISE), and thus enhance its wettability; on the other hand, to maintain the merits of highly contented salt. By taking advantage of these localized highly concentrated lithium salts, aggregated ion clusters are generated in this PISE-TTE system, which construct fast ionic transportation channels, and thus accelerates Li + transportation. Furthermore, this PISE-TTE electrolyte system interacts with Li anode forming a robust organic/inorganic dual layer solid electrolyte interphase (SEI) layer. With the assistance of this tough SEI, the optimized PISE 0.7 -TTE 90 exhibits outstanding anti-dendrite growth behavior in Li/Li and Li/Cu cells. Moreover, PISE 0.7 -TTE 90 also delivers an impressive performance in both Li/LiFePO 4 (LFP, a capacity of 150 mAh g −1 at 0.5C after 150 cycles) and Li@Cu/LFP (electrochemically deposited Li on Cu current collector, a capacity of 150 mAh g −1 at 0.5C after 50 cycles) cells.
研究领域:
电化学
·
能源材料
·
电池技术
·
纳米材料
·
界面化学
·
高分子科学
·
电化学储能
✓ 已验证
DOI
高影响因子
LANGMUIR
·
2017
·
IF 3.833
Jian Zhang,Ran Kou,Guangming Liu
Strong polyelectrolyte brushes (SPB) and weak polyelectrolyte brushes (WPB) have different origins with response to pH, which makes their pH-responsive properties sensitive to salt concentration in different ways. Herein, we have employed poly[2-(methacryloyloxy)ethyl trimethylammonium chloride] (PMETAC) and poly[2-(dimethylamino)ethyl methacrylate] (PDMAEMA) brushes as model systems for SPB and WPB, respectively, to investigate the effect of salt concentration on the pH responses of SPB and WPB using several surface-sensitive techniques. The pH-responsive properties of the PMETAC brushes are governed by the reorganization of the interchain hydrogen bonds between the grafted chains, whereas the pH response of the PDMAEMA brushes is controlled by the charge of the grafted chains. The response of the properties of the PMETAC brushes including hydration, conformation, and surface wettability becomes weaker with increasing salt concentration induced by the competitive adsorption of counterions to the brushes between OH– and Cl–. The weakening of the pH response of the PMETAC brushes is more remarkable at the relatively high pH values. The pH response of the PDMAEMA brushes also exhibits a salt-concentration dependence. As the salt concentration increases, the weakening of the pH response of the PDMAEMA brushes is attributed to the decrease in osmotic pressure within the brushes at relatively low pH values.
研究领域:
材料科学
·
表面化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Jiaming Xu,Chao Ma,Chengyue Chang,Xiaofeng Lei,Yinwei Fu,Jian Wang,Xizheng Liu,Yi Ding
Hybrid solid/gel electrolytes (SGEs) have generated much research attentions because of their capability to suppress Li dendrite growth and improve battery safety. However, the interfacial compatibility of the electrode/electrolyte or polymer/inorganic ceramics within hybrid electrolytes remains challenging for practical applications. Herein, an SGE is fabricated by confining ceramic particles (Li7La3Zr2O12; LLZO) into in situ formed tetraethylene glycol dimethyl ether (G4)-based gel electrolytes within assembled cells. A hierarchical layered structure is formed when LLZO settles near the Li anode within the liquid electrolyte during the gradual gelatinization process. Good interfacial compatibility is obtained from good contact with the liquid G4 component. The LLZO layer also serves as an ionic sieve to redistribute the Li deposition. This SGE endows stable Li stripping/plating cycling over 800 h at 0.5 mA/cm2 (60 °C). Moreover, Li-metal batteries with an SGE coupled with LiFePO4 and an air cathode both exhibit superior cycling performance. This work presents a promising strategy for hierarchically layered SGEs for high-performance Li-metal batteries.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Rong Zheng,Baojun Wang,Yuchen Liu,Jingze Zhang,Chengyi Hou,Qinghong Zhang,Kerui Li,Yaogang Li,Hongzhi Wang
Aqueous zinc-ion batteries (ZIBs) have emerged as promising candidates for next-generation energy storage systems due to their inherent safety, cost-effectiveness, and high energy density. However, challenges such as hydrogen evolution reactions induced by active water in liquid electrolytes and the formation of zinc dendrites severely limit their practical application. To address the adverse effects of free water, various quasi-solid-state electrolytes are developed. In this study, a solid-liquid hybrid inorganic silica gel electrolyte (ISE) is synthesized via a facile sol-gel process. The ISE enables efficient zinc-ion transport through the synergistic interaction of a solid silica-oxygen framework and liquid water. Consequently, the ISE demonstrates an ionic conductivity of 1.39 × 10 –4 S cm –1 and exceptional long-term cycling stability, with over 800 h of long-term charge-discharge operation. Furthermore, the full cell retains 70 % of its capacity after 1800 cycles, with a low self-discharge rate and a capacity retention of up to 90 %.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Qian Zhang,Kun Liu,Kang Liu,Junpeng Li,Chunjie Ma,Liang Zhou,Yaping Du
Improving the safety and performance of lithium ion batteries (LIB) sparked the idea of using a solid electrolyte to construct all-solid-state ones. In this study, a composite solid polymer electrolyte based on Li 6.40 La 3 Zr 1.40 Ta 0.60 O 12 (LLZTO) nanoparticles and a random copolymer , poly(vinyl pyrrolidone- co -poly(oligo(ethylene oxide) methyl ether methacrylate) (PPO), was successfully prepared and investigated in detail. The copolymer PPO is mixed with LiTFSI and LLZTO at different ratios and the Li conductivity and other electrochemical properties were studied. The copolymer matrix shows the highest ionic conductivity , 2.43 × 10 −5 S/cm at 60 °C, at the content of 20 wt% LiTFSI, the highest lithium ion transference number is determined to be 0.33 at room temperature , and the electrochemical stability reaches 4.3 V vs. Li + /Li. Interestingly, when compounded with LLZTO nanoparticles , the ionic conductivity is not improved much. For example, the highest ionic conductivity increases a little to 2.74 × 10 −5 S/cm at 60 °C when 5 wt% LLZTO is added. However, a large increase in electrochemical stability to 5.0 V is obtained for the sample of PPO-20%-10LLZTO. Both PPO and the composite electrolyte show good cycling performance during a plating/stripping experiment at a current density of 0.01 mA/cm 2 . The limited improvement of properties is possibly due to the poor interface contact between PPO and LLZTO nanoparticles . The result may shed light on the complexity of fabricating composite electrolytes using mixtures of polymer and lithium-conducting ceramics.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）