ADVANCED FUNCTIONAL MATERIALS
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2024
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IF 18.5
Jianwen Feng,Jiayi Wang,Qiao Gu,Pingting Li,Hongli Xu,Yonghong Deng,Ping Gao
Gel polymer electrolytes (GPEs) hold great promise for lithium (Li) metal batteries (LMBs). Nevertheless, a critical challenge lies in reducing the thickness of GPEs while maintaining their mechanical integrity to achieve high-energy-density LMBs. Additionally, protecting the Li metal anode via electrolyte engineering in GPEs remains demanding. Herein, an innovative ultrathin (1 µm-thick) yet robust GPE developed using an in situ curing technique, featuring a nanofibrous, exceptionally strong polyethylene separator is presented. The unique microstructure, interfacial conformability, and ultrahigh mechanical robustness of the ultrathin polyethylene separator are thoroughly verified. Enhanced ionic association within the GPE is achieved due to the strong affinity of electrolyte solvent with the fluorinated polymer network, as confirmed by large-scale molecular dynamics simulations. The optimized solvation structure with high contact ion pairs and aggregate fractions contributes to forming an anion-derived inorganic-rich solid electrolyte interphase (SEI), thereby protecting the lithium anode. Benefiting from the ultrahigh robustness of GPE and the excellent interfacial stability, the Li metal full cell with a high mass loading LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathode (≈17.3 mg cm −2 ) and thin Li foil anode (50 µm) demonstrates 91% capacity retention after 200 cycles. This design demonstrates a feasible approach toward the practical quasi-solid-state LMBs.
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高影响因子
ACS Applied Polymer Materials
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2024
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IF 4.4
Yonghao Huang,Zhangyating Xie,Weiya Zhu,Changyong Mo,Weishan Li,Youhao Liao
To solve the problems of narrow oxidation decomposition potential and low room temperature ionic conductivity of the traditional poly(ethylene oxide) (PEO)-based solid polymer electrolyte (SPE), a polycarbonate-based SPE is developed by facile in situ ultraviolet-irradiated polymerization for high-energy-density lithium metal batteries (LMBs). Since the weak complexation between carbonate groups and Li+-ions in the vinyl ethylene carbonate (VEC) section provides the ionic transport capability, while the rigid hydroxyethyl methacrylate (HEMA) segment facilitates the mechanical strengths, the prepared P(VEC-HEMA) copolymer-based SPE exhibits a high ionic conductivity of 0.8 × 10–3 S cm–1 at room temperature, an antioxidation potential exceeding 5.0 V, and a high Young’s modulus value of 2.3 GPa that can effectively prevent the puncture of lithium dendrites. Notably, the P(VEC-HEMA) copolymer presents a stronger binding energy with TFSI– than that of the PVEC oligomer, ascribed to the hydroxyl group in HEMA section that also gives a fast transport pathway for Li+-ions through hydrogen bonds. Contributed by the advanced functional groups inhered from distinct monomers, the assembled Li∥SPE∥LiCoO2 full cell using P(VEC-HEMA) electrolyte exhibits excellent rate capacity and long cyclic stability, which shows the specific discharge capacity of 138.1 mA h g–1 at 0.1 C rate in the voltage range of 3.0–4.2 V, maintaining 93.5% of initial capacity after 100 cycles. For comparison, the full cell using PVEC electrolyte has a short circuit after 13 cycles. Therefore, the proposed polycarbonate solid electrolyte gives a bright future to revitalize the development of high-energy-density LMBs.
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高影响因子
ACS Sustainable Chemistry & Engineering
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2024
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IF 7.1
Haozheng Hu,Xianghao Meng,Yin Li,Yusong Yang,Yanqiu Xu,Junxian Hu,Yaochun Yao
In the era of extensive deployment of LiFePO4 batteries in energy storage and electric vehicle domains, the recycling of lithium from spent LiFePO4 (SLFP) batteries has emerged as a focus, which helps in alleviating environmental pollution and resource shortages. Traditional recycling techniques, encompassing pyrometallurgical and hydrometallurgical methods, are often marred by low selectivity and extraction efficiency. Herein, an eco-friendly and low-consumption recycling strategy involving potassium pyrosulfate (K2S2O7)-assisted low-temperature roasting and subsequent water leaching has been developed for selectively recycling Fe and Li from SLFP batteries. The proposed strategy, compared to the conventional inorganic acid leaching method, mitigates the environmental hazards caused by acidic wastewater generation and reduces the costs associated with wastewater treatment. Investigations of thermal performance characterization and thermodynamic calculation analyses have revealed that K2S2O7 plays a pivotal role in extracting lithium from the Fe–P–O framework, converting lithium into a soluble sulfate variant and iron into insoluble compounds. This process culminates in the segregation of a lithium-rich leachate and an iron-enriched residue, which are further processed to synthesize Li2CO3 and FePO4. The effects on Li leaching of the mass ratio of K2S2O7 to SLFP, roasting time, roasting temperature, and water leaching time are systematically studied and 95.87% Li was leached in water under optimal conditions. In addition, the feasibility of the strategy was further illustrated by the regeneration of LiFePO4 produced by the recycled Li2CO3 and FePO4. Overall, this recovery strategy stands out for its effective lithium-iron segregation, environmental sustainability, and economic viability, which provide some inspiration for high-efficiency and environmentally friendly recovery metal from spent lithium-ion batteries.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Xue Bai,Yanzhi Sun,Rui He,Zhenfa Liu,Junqing Pan
With the rapid development of electric vehicles and digital devices, the accumulated spent lithium-ion batteries (LIBs) cause severe anxiety about lithium resources and environmental safety. However, the low capture rate of Li + and the high chemical consumption of the existing recovery methods lead to high Li loss, treatment costs and disposal fees. Herein, we propose a universal strategy of spent LIBs recovery via precise directional regulating structures (from layered to rock) to achieve ultrahigh lithium recovery rate with super-low chemical and energy consumption. Experimental characterization and theoretical calculations reveal the dissociation of structure, reorganization of Li–O bonds and phase transformation of the cathode materials in the limited-domain reduction process, realizing the complete recovery of Li + without consuming acid leaching agent. This process realizes an extra-high Li separation index (19154) and extra-long cycle half-life (173 cycles) which are far superior to those of traditional methods (9–191 and 7 cycles). Besides, ecological and economic analysis shows that the consumptions of chemicals and energy are only 9 % and 9.7 % those of the existing literature, respectively, providing a bright pathway for industrializable lithium batteries recycling.
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高影响因子
Materials Today Energy
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2024
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IF 9
Jiechen Song,Yuxing Xu,Yuncheng Zhou,Rui He,Aijia Wei,Qiangqiang Tan
Lithium metal batteries with polyethylene oxide (PEO) electrolytes have shown great potential to be one of the next-generation energy candidates. As the branch family of PEO electrolytes, poly(ethylene glycol) acrylates (PEGAs) attract more attention owing to their better electrochemical properties than that of PEO electrolytes. Introducing double bond-modified Li 6.75 La 3 Zr 1.75 Ta 0.25 O 12 fillers (KH@LLZTO) has been a popular method to improve the electrochemical properties of PEGAs electrolytes due to the homogeneous dispersion of LLZTO. However, in this work, an inverse phenomenon is discovered. The electrochemical properties of PEGAs electrolytes get worse when introducing KH@LLZTO. By exploring the Li + transport mechanism, the reason for the inverse phenomenon is revealed. More importantly, the design principle of PEGAs electrolytes with fast ionic conductor fillers is presented. Double bond-modified LLZTO can decrease the electrochemical properties of PEGAs electrolytes instead when there are low-molecular weight monomers that can participate in the PEGAs polymer network and interact with Li + , while the double bond-modified LLZTO can improve the electrochemical properties of PEGAs electrolytes when there are not aforementioned low-molecular weight monomers. This work provides a new understanding for componential design and optimization of PEGAs electrolytes with fast ionic conductors, hoping to promote the practical application of PEGAs electrolytes.
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高影响因子
APPLIED ENERGY
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2024
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IF 10.1
Enmin Xu,Luozhi Mo,Yingke Zhou,Zhe Cheng,Ping Li,Xiaohui Tian,Wei Yang,Caiting Lai,Peng Dou,Zhongzhi Yuan
Lithium batteries have been widely used in portable appliances and medical and aerospace devices, and further improving the energy density and power density is of great significance to the future development of related technologies. In this work, a high-dielectric polyvinylidene difluoride (PVDF) coating film was designed and realized on Cu foil by a polar solution-induced phase transition method. The PVDF40 coating film prepared at 40 °C displays a high β-phase content (91.68 %) and strong dielectric properties, which can effectively promote the dissociation of Li salt, and exhibits superior ionic conductivity of 4.06 × 10 −4 S cm −1 and greatly increased Li transference number of 0.652. The Li-CF x battery with coating film delivers an excellent specific discharge capacity of 947 mAh g −1 at 0.1C, and a superior rate capacity of 634 mAh g −1 even at 5C, attributed to the improved dissociate of lithium salt, Li coordination environment and ion transport. This study demonstrates a dielectric film protection strategy to achieve high-performance lithium batteries.
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高影响因子
Journal of Energy Chemistry
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2025
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IF 14.9
Vestince Balidi Mbayachi,Lixin Liang,Bao Zhang,Yaru Zhang,Guiming Zhong,Kuizhi Chen,Guangjin Hou
Composite polymer electrolytes (CPEs) are considered as promising electrolytes for next-generation lithium batteries due to their superior advantages in safety, mechanical stability/flexibility, cathode compatibility, etc. However, achieving high Li + conductivity remains a major challenge, particularly at low temperatures. A key obstacle lies in the limited understanding of the complex interplay among amorphous components, including fillers, plasticizers, and residual solvents, which significantly hampers the rational design of high-performing CPEs. In this contribution, a polyvinylidene fluoride (PVDF)-based composite electrolyte has been developed, exhibiting high room-temperature ionic conductivity/mobility (>1 mS cm −1 /0.95 × 10 −11 m 2 s −1 ), along with excellent electrochemical performances, including a wide stability window (4.8 V vs. Li/Li + ), superior charge/discharge capacity, and reversibility. By performing advanced solid-state nuclear magnetic resonance (ssNMR) techniques, in combination with systematic investigations into solid polymer electrolytes (SPEs), gel polymer electrolytes (GPEs), and CPEs, we establish an efficient NMR-based strategy for deconvoluting the structural and dynamic features of complex electrolyte systems. Notably, the simple 1 H magic-angle spinning (MAS) NMR spectroscopy enables the identification and monitoring of nearly all components in the composite matrix. Motion-Sensitive 1 H- 13 C and 1 H- 7 Li correlation experiments further reveal that the rigidity of PVDF polymer chain segments and the presence of residual solvents are two critical factors governing Li + mobility. Moreover, we demonstrate that the order of the filler and plasticizer addition during the CPE fabrication significantly influences the performance of the electrolyte by regulating the retention of residual solvents. This work not only provides molecular-level insights into the structure-ion mobility relationships in the PVDF-based CPEs but also establishes a general NMR-based characterization approach for investigating other complex composite electrolyte materials.
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ELECTROCHIMICA ACTA
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2025
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IF 5.6
Yaqin Ji,Wenjuan Yang,Jian Ma,Haoran Du,Xulai Yang,Zhenzhen Liu,Sheng Liang,Lingli Liu,Lei Hu,Xin Liang
It is a persistent goal for solid-state electrolytes to enhance their ionic conductivity while maintaining good mechanical strength to potentially inhibit lithium dendrites. In this work, we introduce garnet-type Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) fillers and polyacrylonitrile (PAN) into thermoplastic polyurethane (TPU) to fabricate a composite solid-state electrolyte. The TPU matrix contains hard segments (−NH−COO−) that provide efficient mechanical support and soft segments (−O−) responsible for good flexibility and elasticity. When blended with PAN, hydrogen bonds form between the functional groups of PAN and TPU, establishing strong intermolecular connections that further enhance the structural/electrochemical stability of the electrolyte. A stable polymer/filler interface can be constructed through the ion-dipole coordination interaction between the metal ions at the LLZTO surface and the −CN groups of PAN. Benefiting from the intricate interactions among the PAN/TPU dual polymers and the LLZTO filler, the composite electrolyte exhibits not only exceptional flexibility (a tensile strain of 208%) and tensile strength (40 MPa), but also a good ionic conductivity of 2.33 × 10 −4 S cm⁻¹ at room temperature, a high oxidation potential of 4.48 V, and an excellent Li + transference number of 0.79. The Li||LiFePO 4 battery employing this composite solid-state electrolyte exhibits remarkable electrochemical stability, delivering an initial discharge capacity of 127.4 mAh g −1 at 0.3C and room temperature, and maintains a capacity retention of 91.9% after 600 cycles. This work provides a new electrolyte modification strategy for next-generation solid-state lithium metal batteries.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Hongye Lv,Xuyong Tian,Haowei Feng,Chunlei Wang,Liying Wei,Xiuping Li,Haolong Xue,Changfa Xiao,Dawei Ji
In recent years, many researchers have focused on incorporating functional nanomaterials into thin-film composite (TFC) membranes to synthesize thin-film nanocomposite (TFNi) nanofiltration (NF) membranes with intermediate layers. The stability of the intermediate layer was very important for the TFNi NF membranes. This study constructed a unique structure of ZIF-8@CNTs-OH@PEI nanocomposite intermediate layers on the polysulfone (PSF) supporting membranes, where hydroxyl-functionalized carbon nanotubes (CNT-OH) captured 2-methylimidazole through its porous structure and hydrogen bonding with hydroxyl groups, enabling zeolitic imidazolate framework-8 (ZIF-8) to grow on CNT-OH. In addition, polyethylenimine (PEI) could act as the “adhesive” among ZIF-8 and CNT-OH due to the strong adhesion of hydrogen bonding with abundant –NH 2 groups. Thus, the nanocomposite particles could form a stable intermediate layer on the surface of PSF membrane. Furthermore, the positively charged PA/ZIF-8@CNTs-OH@PEI/PSF composite NF membranes with strong interlayer bonding were synthesized through further interfacial polymerization reactions on the intermediate layer. In particular, the synthesized nanocomposite suspension of ZIF-8@CNTs-OH@PEI address the particle aggregation and poor dispersibility. Moreover, the structure of intermediate layer features abundant voids, which can reduce the transmembrane resistance of water and enhance permeation performance. Compared to the PA/M−0 without the intermediate layer, the PA/M−30 exhibited a significantly improved flux of 70.6 L m -2 h −1 , that was 2.6 times higher compared to that for PA/M−0. Additionally, the optimized PA/ZIF-8@CNTs-OH@PEI/PSF composite NF membranes achieved Li + and Mg 2+ retention rates of −25.5 % and 95.2 %, respectively, with a Mg 2+ /Li + separation factor (SLi, Mg) equal to 29.9, which showed good long-term operational stability.
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高影响因子
DESALINATION
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2025
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IF 9.8
Yueyu Liu,Lili Gao,Shiwei Li,Libo Zhang,Shaohua Yin
Nanofiltration (NF) has been recognized as a sustainable approach for lithium extraction from salt lakes. However, conventional thin-film nanocomposite (TFN) membranes face persistent challenges in overcoming the “trade-off”. This study reports a tunable growth strategy of MOF nanocrystals within the selective layer, enabling enhanced permeability and ion selectivity for lithium recovery from brine. Based on a “De novo synthesis” strategy, ultrasound-assisted in situ growth of smaller-sized NH 2 -ZIF-8 nanocrystals is achieved through controlled ligand substitution and nanocrystal size modulation within the separation layer. The optimized membrane exhibited outstanding performance, with a high Mg 2+ /Li + selectivity ( S Li/Mg = 113.97), high permeability (18.52 L m −2 h −1 bar −1 (LMH/bar)), and long-term stability over a 336-hour separation test. Furthermore, the mass transfer behavior during nanofilm formation has been elucidated by theoretically analyzing monomer diffusion kinetics and the variation of monomer concentration at the reactive interface. This work presents an efficient strategy for MOF generation and provides a promising pathway for the high-efficiency extraction of lithium from complex brine resources.
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高影响因子
Science Bulletin
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2025
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IF 21.1
Shida Xue,Xiangming Yao,Zhikang Deng,Jianjun Fang,Yingkang Liu,Yuxiang Huang,Xiaohu Wang,Guobiao Jin,Zhaohuang Zhan,Hongkai Yang,Zijin Xu,Zu-Wei Yin,Luyi Yang,Feng Pan
As a promising deep eutectic quasi-solid electrolyte (DES) for Li-ion batteries, the application of dimethyl sulfone (DMS) is limited by its stability at the electrode-electrolyte interface. A common strategy to address this issue involves introducing additional anions into the Li-ion (Li + ) solvation sheath to stabilize the interphase. However, this approach often comes at the expense of ionic conductivity, which can negatively impact battery performance. In this work, a strategy to decouple Li + conduction and coordination structure is proposed. The introduction of lithium difluoroxalate borate (LiDFOB) promotes an anion-rich Li + solvation sheath, which facilitates the formation of stable interphases. More importantly, the incorporation of polyvinylidene fluoride (PVDF) frameworks regulates localized coordination structures and constructs fast Li + transport channels, liberating the movement of Li + from the constraints of their sluggish solvation clusters. As a result, this hierarchical regulation strategy not only achieves improved ionic conductivity, enabling high-rate operation, but also ensures the formation of stable interphases on 4.6 V LiCoO 2 cathode and graphite anode, exhibiting exceptional high-voltage operation stability for DESs. This work presents a promising approach to addressing critical challenges of DESs by achieving a balance between conductivity and interfacial stability, providing significant insights for their practical application.
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PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2025
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IF 19
Jingbo Mu,Shimin Liao,Shengsheng Wang,Feng Xu,Bihai Su,Linlin Shi,Xiaojing Wang,Xuewei Hao,Zengcai Guo,Zhongkai Huang,Tian Tian
Achieving lithium-ion flux regulation in composite solid electrolytes (CSEs) remains a critical challenge for developing solid-state Li-metal batteries suppressing dendrite growth with high-voltage compatibility. Here, a new concept of Li⁺ transport gradient soft-rigid structure CSEs is introduced, which comprises a poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) matrix integrated with acetate-functionalized cellulose nanocrystals (CNC-PVAc) and ZIF-8. This structure enables directed and fast Li⁺ conduction through low-tortuosity channels, significantly inhibiting lithium dendrite nucleation and growth. The electrochemical stability window of PHCF spans up to 4.82 V versus Li⁺/Li. Theoretical simulations reveal a synergistic intrinsic origin of the exceptional performance for this designed Li⁺ transport gradient soft-rigid structure CSEs. Consequently, the synthesized CSEs demonstrate high ionic conductivity (1.79 × 10 −4 S cm −1 ) and a notably high Li⁺ transference number (t Li⁺ ) of 0.79 at 60 °C. Corresponding all-solid-state LiFePO 4 ||Li and NCM811|| Li cells deliver impressive specific capacities of 163.78 (0.1C) and 190.67 mAh g −1 (0.5C) at 60 °C, respectively. This work presents a high-performance CSEs with intrinsic safety, providing valuable insights for novel design concept of solid-state batteries (SMBs).
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危险品化学品经营许可证（带存储）