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35 pages, 5230 KB  
Article
Electrochemical Performances of Li-Ion Batteries Based on LiFePO4 Cathodes Supported by Bio-Sourced Activated Carbon from Millet Cob (MC) and Water Hyacinth (WH)
by Wend-Waoga Anthelme Zemane and Oumarou Savadogo
Batteries 2025, 11(10), 361; https://doi.org/10.3390/batteries11100361 - 30 Sep 2025
Abstract
The electrochemical performance of Li-ion batteries employing LiFePO4 (LFP) cathodes supported by bio-sourced activated carbon derived from millet cob (MC) and water hyacinth (WH) were systematically investigated. Carbon activation was carried out using potassium hydroxide (KOH) at varying mass ratios of KOH [...] Read more.
The electrochemical performance of Li-ion batteries employing LiFePO4 (LFP) cathodes supported by bio-sourced activated carbon derived from millet cob (MC) and water hyacinth (WH) were systematically investigated. Carbon activation was carried out using potassium hydroxide (KOH) at varying mass ratios of KOH to precursor material: 1:1, 2:1, and 5:1 for both WH and MC-derived carbon. The physical properties (X-ray diffraction patterns, BET surface area, micropore and mesopore volume, conductivity, etc.) and electrochemical performance (specific capacity, discharge at various current rates, electrochemical impedance measurement, etc.) were determined. Material characterization revealed that the activated carbon derived from MC exhibits an amorphous structure, whereas that obtained from WH is predominantly crystalline. High specific surface areas were achieved with activated carbons synthesized using a low KOH-to-carbon mass ratio (1:1), reaching 413.03 m2·g−1 for WH and 216.34 m2·g−1 for MC. However, larger average pore diameters were observed at higher activation ratios (5:1), measuring 8.38 nm for KOH/WH and 5.28 nm for KOH/MC. For both biomass-derived carbons, optimal electrical conductivity was obtained at a 2:1 activation ratio, with values of 14.7 × 10−3 S·cm−1 for KOH/WH and 8.42 × 10−3 S·cm−1 for KOH/MC. The electrochemical performance of coin cells based on cathodes composed of 85% LiFePO4, 8% of these activated carbons, and 7% polyvinylidene fluoride (PVDF) as a binder, with lithium metal as the anode were studied. The LiFePO4/C (LFP/C) cathodes exhibited specific capacities of up to 160 mAh·g−1 at a current rate of C/12 and 110 mAh·g−1 at 5C. Both LFP/MC and LFP/WH cathodes exhibit optimal energy density at specific values of pore size, pore volume, charge transfer resistance (Rct), and diffusion coefficient (DLi), reflecting a favorable balance between ionic transport, accessible surface area, and charge conduction. Maximum energy densities relative to active mass were recorded at 544 mWh·g−1 for LFP/MC 2:1, 554 mWh·g−1 for LFP/WH 2:1, and 568 mWh·g−1 for the reference LFP/graphite system. These performance results demonstrate that the development of high-performing bio-sourced activated carbon depends on the optimization of various parameters, including chemical composition, specific surface area, pore volume and size distribution, as well as electrical conductivity. Full article
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16 pages, 4578 KB  
Article
Thermal Stability of Color Centers in Lithium Fluoride Crystals Irradiated with Electrons and N, O, Kr, U Ions
by Zhadra Malikova, Zhakyp T. Karipbayev, Abdirash Akilbekov, Alma Dauletbekova, Anatoli I. Popov, Vladimir N. Kuzovkov, Ainash Abdrakhmetova, Alyona Russakova and Muratbek Baizhumanov
Materials 2025, 18(19), 4441; https://doi.org/10.3390/ma18194441 - 23 Sep 2025
Viewed by 222
Abstract
Lithium fluoride (LiF) crystals are widely employed both as optical windows transparent in the ultraviolet spectral region and as efficient personal dosimeters, with their application scope recently expanding into lithium-ion technologies. Moreover, as an alkali halide crystal (AHC), LiF serves as a model [...] Read more.
Lithium fluoride (LiF) crystals are widely employed both as optical windows transparent in the ultraviolet spectral region and as efficient personal dosimeters, with their application scope recently expanding into lithium-ion technologies. Moreover, as an alkali halide crystal (AHC), LiF serves as a model system for studying and simulating radiation effects in solids. This work identifies radiation-induced defects formed in lithium fluoride upon irradiation with swift heavy ion beams (N, O, Kr, U) and intense pulsed electron beams, investigates their thermal stability, and performs computer modeling of annealing processes. The theoretical analysis of existing experimental kinetics for F-centers induced by electron and heavy ion irradiation reveals considerable differences in the activation energies for interstitial migration. A strong correlation between the activation energy Ea and the pre-exponential factor X(Ea) is observed; notably, X(Ea) is no longer constant but closely matches the potential function Ea. Indeed, with increasing irradiation dose, both the migration energy Ea and pre-exponential factor X decrease simultaneously, leading to an effective increase in the defect diffusion rate. Full article
(This article belongs to the Section Optical and Photonic Materials)
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17 pages, 2545 KB  
Article
Persulfate Activation of Iron-Based Battery Catalytic Material (LFP) Modified on Polymeric Membrane (LFP@PVDF) for the Treatment of Textile Dye Wastewater
by Ali Kemal Topaloğlu, Bekir Fatih Kahraman and Semih Engün
Sustainability 2025, 17(18), 8469; https://doi.org/10.3390/su17188469 - 21 Sep 2025
Viewed by 211
Abstract
In this study, a novel LFP–catalytic microfiltration membrane (LFP@PVDF) was fabricated by loading a lithium-ion battery material LiFePO4 (LFP) onto polymeric micro-porous polyvinylidene fluoride (PVDF) using a filter press coating method. The successful loading of LFP material onto the LFP@PVDF catalytic membrane [...] Read more.
In this study, a novel LFP–catalytic microfiltration membrane (LFP@PVDF) was fabricated by loading a lithium-ion battery material LiFePO4 (LFP) onto polymeric micro-porous polyvinylidene fluoride (PVDF) using a filter press coating method. The successful loading of LFP material onto the LFP@PVDF catalytic membrane was confirmed by the characterization of the material using FTIR, SEM, EDX, and XRD analysis. To evaluate the catalytic performance of the LFP@PVDF membrane, the reactive black 5 (RB5) dye-containing solution was used with or without the peroxymonosulfate (PMS) activator in a dead-end filtration under room conditions. The influence of parameters such as LFP loading, initial RB5 dye concentration, persulfate dosage, and solution pH on the performance of the persulfate oxidation process was comprehensively examined. It was found that the LFP@PVDF membrane/persulfate activation system can effectively remove RB5 dye with an efficiency of 97.3%. The RB5 dye removal by LFP@PVDF membranes with varying experimental conditions was found to fit the pseudo-second-order kinetic model. Quenching experiments showed that the reactive species HO, SO4 and 1O2 were responsible for the dye removal. The LFP@PVDF membrane/persulfate activation system appeared to be a promising approach for the removal of organic contaminants. Full article
(This article belongs to the Topic Advanced Oxidation Processes for Wastewater Purification)
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14 pages, 6680 KB  
Article
In Situ Engineered Plastic–Crystal Interlayers Enable Li-Rich Cathodes in PVDF-HFP-Based All-Solid-State Polymer Batteries
by Fei Zhou, Jinwei Tan, Feixiang Wang and Meiling Sun
Batteries 2025, 11(9), 334; https://doi.org/10.3390/batteries11090334 - 6 Sep 2025
Viewed by 872
Abstract
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 [...] Read more.
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–LiClO4 configuration exhibits a wide electrochemical stability window up to 4.7 V vs. Li+/Li and delivers a high ionic conductivity of 5.68 × 10−4 S cm−1 at 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−1 at 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. Full article
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13 pages, 3455 KB  
Article
Three-Dimensional-Printed Polymer–Polymer Composite Electrolytes for All-Solid-State Li Metal Batteries
by Hao Wang, Xin Xiong, Huie Hu and Sijie Liu
Polymers 2025, 17(17), 2369; https://doi.org/10.3390/polym17172369 - 30 Aug 2025
Viewed by 745
Abstract
High-performance batteries for military and extreme environment applications require alternatives to conventional liquid lithium-ion batteries (LIBs), which suffer from poor low-temperature performance and safety risks. All-solid-state lithium batteries (ASSLBs) offer enhanced safety and superior low-temperature capability. In this work, we designed and fabricated [...] Read more.
High-performance batteries for military and extreme environment applications require alternatives to conventional liquid lithium-ion batteries (LIBs), which suffer from poor low-temperature performance and safety risks. All-solid-state lithium batteries (ASSLBs) offer enhanced safety and superior low-temperature capability. In this work, we designed and fabricated composite solid-state electrolytes using polyvinylidene fluoride (PVDF) and polyacrylic acid (PAA) as polymer matrices, N,N-dimethylformamide (DMF) as the solvent, and lithium bis(trifluoromethane sulfonimide) (LiTFSI) as the lithium salt. Composite solutions with varying PAA mass ratios were prepared. Advanced three-dimensional (3D) printing technology enabled the rapid and precise fabrication of electrolyte membranes. An ionic conductivity of about 2.71 × 10−4 S cm−1 at 25 °C, high mechanical strength, and good thermal properties can be achieved through component and 3D printing process optimization. Assembled LiCoO2||PVDF@PAA||Li ASSLBs delivered an initial discharge capacity of 165.3 mAh/g at 0.1 mA cm−2 (room temperature), maintaining 98% capacity retention after 300 cycles. At 0 °C, these cells provided 157.4 mAh/g initial capacity with 85% retention over 100 cycles at 0.1 mA cm−2. This work identifies the optimal PAA ratio for enhanced electrochemical performance and demonstrates the viability of 3D printing for advanced ASSLB manufacturing. Full article
(This article belongs to the Special Issue Advances in Polymeric Additive Manufacturing—2nd Edition)
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14 pages, 3325 KB  
Article
Dual-Strategy Design Based on Polymer–Matrix Composite Cathode and Coated Separator for High-Performance Lithium–Iron Disulfide Batteries
by Fan Zhang, Qiang Lu, Jiachen Li, Qiongyue Zhang, Haotian Yu, Yahao Wang, Jinrui Li, Haodong Ren, Huirong Liang, Fei Shen and Xiaogang Han
Materials 2025, 18(17), 4058; https://doi.org/10.3390/ma18174058 - 29 Aug 2025
Viewed by 683
Abstract
Lithium–iron disulfide (Li-FeS2) batteries are plagued by the polysulfide shuttle effect and cathode structural degradation, which significantly hinder their practical application. This study proposes a dual-strategy design that combines a polyacrylonitrile–carbon nanotube (PAN-CNT) composite cathode and a polyvinylidene fluoride (PVDF)-conductive carbon-coated [...] Read more.
Lithium–iron disulfide (Li-FeS2) batteries are plagued by the polysulfide shuttle effect and cathode structural degradation, which significantly hinder their practical application. This study proposes a dual-strategy design that combines a polyacrylonitrile–carbon nanotube (PAN-CNT) composite cathode and a polyvinylidene fluoride (PVDF)-conductive carbon-coated separator to synergistically address these bottlenecks. The PAN-CNT binder establishes chemical anchoring between polyacrylonitrile and FeS2, enhancing electronic conductivity and mitigating volume expansion. Specifically, the binder boosts the initial discharge capacity by 35% while alleviating the stress-induced pulverization associated with volume changes. Meanwhile, the PVDF-conductive carbon-coated separator enables effective polysulfide trapping via dipole–dipole interactions between PVDF’s polar C-F groups and Li2Sx species while maintaining unobstructed ion transport with an ionic conductivity of 1.23 × 103 S cm1, achieving a Coulombic efficiency of 99.2%. The electrochemical results demonstrate that the dual-modified battery delivers a high initial discharge capacity of 650 mAh g−1 at 0.5 C, with a capacity retention rate of 61.5% after 120 cycles, significantly outperforming the control group’s 47.5% retention rate. Scanning electron microscopy and electrochemical impedance spectroscopy confirm that this synergistic design suppresses polysulfide migration and enhances interfacial stability, reducing the charge transfer resistance from 26 Ω to 11 Ω. By integrating polymer-based functional materials, this work presents a scalable and cost-effective approach for developing high-energy-density Li-FeS2 batteries, providing a practical pathway to overcome key challenges in their commercialization. Full article
(This article belongs to the Section Energy Materials)
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29 pages, 5199 KB  
Review
Recent Progress on Synthesis and Electrochemical Performance of Iron Fluoride Conversion Cathodes for Li-Ion Batteries
by Jiabin Tian, Ziyi Yang, Yayun Zheng and Zhengfei Chen
Solids 2025, 6(3), 47; https://doi.org/10.3390/solids6030047 - 22 Aug 2025
Viewed by 834
Abstract
Despite notable advancements in lithium-ion battery (LIB) technology, growing industrialization, rising energy demands, and evolving consumer electronics continue to raise performance requirements. As the primary determinant of battery performance, cathode materials have become a central research focus. Among emerging candidates, iron-based fluorides show [...] Read more.
Despite notable advancements in lithium-ion battery (LIB) technology, growing industrialization, rising energy demands, and evolving consumer electronics continue to raise performance requirements. As the primary determinant of battery performance, cathode materials have become a central research focus. Among emerging candidates, iron-based fluorides show great promise due to their high theoretical specific capacities, elevated operating voltages, low cost (owing to abundant iron and fluorine), and structurally diverse crystalline forms such as pyrochlore and tungsten bronze types. These features make them strong contenders for next-generation high-energy, low-cost LIBs. This review highlights recent progress in iron-based fluoride cathode materials, with an emphasis on structural regulation and performance enhancement strategies. Using pyrochlore-type hydrated iron trifluoride (Fe2F5·H2O), synthesized via ionic liquids like BmimBF4, as a representative example, we discuss key methods for tuning physicochemical properties—such as electronic conductivity, ion diffusion, and structural stability—via doping, compositing, nanostructuring, and surface engineering. Advanced characterization tools (XRD, SEM/TEM, XPS, Raman, synchrotron radiation) and electrochemical analyses are used to reveal structure–property–performance relationships. Finally, we explore current challenges and future directions to guide the practical deployment of iron-based fluorides in LIBs. This review provides theoretical insights for designing high-performance, cost-effective cathode materials. Full article
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25 pages, 1218 KB  
Article
Enhancing the Selectivity of Nitroso-R-Salt for the Determination of Co(II) in Lithium Bioleaching Recovery of Smartphone Batteries Using a Combinatorial Methodology Approach
by David Ricart, Antonio David Dorado, Mireia Baeza and Conxita Lao-Luque
Nanomaterials 2025, 15(16), 1264; https://doi.org/10.3390/nano15161264 - 16 Aug 2025
Viewed by 521
Abstract
The selectivity of the colorimetric method for Co(II) determination using the nitroso-R-salt (NRS) in samples with complex matrices has been improved. Interferences caused by Cu(II), Fe(II), Fe(III), Mn(II), Al(III) and Ni(II) ions, which were present in the bioleach ate of lithium-ion batteries, have [...] Read more.
The selectivity of the colorimetric method for Co(II) determination using the nitroso-R-salt (NRS) in samples with complex matrices has been improved. Interferences caused by Cu(II), Fe(II), Fe(III), Mn(II), Al(III) and Ni(II) ions, which were present in the bioleach ate of lithium-ion batteries, have been solved through the sequential addition of masking agents: acetate, fluoride, ethylenediaminetetraacetic acid (EDTA), and strong acids (H2SO4). The absorbance of the NRS-Co(II) complex was typically measured at 525 nm, but it was also studied at 550 nm due to minimal interferences observed at 550 nm. The sequence of the masking agent’s addition showed a significant influence on the interference effect. The optimal sequence was sample, acetate–acetic acid buffer solution with dissolved fluoride, NRS, EDTA and H2SO4. The proposed method demonstrated robust performance at 550 nm, with a relative standard deviation (RSD) around 2%, and good accuracy (RV% around 100%). The limit of detection (LoD) was 0.1 mg L−1 and the limit of quantification (LoQ) was 0.3 mg L−1. The linear range extended up to 15 mg L−1 (R2 = 0.998). Real samples analyzed using the optimized method showed no significant differences when compared to results from atomic absorption spectroscopy, confirming its reliability. Full article
(This article belongs to the Section 2D and Carbon Nanomaterials)
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19 pages, 5196 KB  
Article
Exploring Different Metal-Oxide Cathode Materials for Structural Lithium-Ion Batteries Using Dip-Coating
by David Petrushenko, Thomas Burns, Paul Ziehl, Ralph E. White and Paul T. Coman
Energies 2025, 18(16), 4354; https://doi.org/10.3390/en18164354 - 15 Aug 2025
Viewed by 561
Abstract
In this study, a selection of active materials were coated onto commercially available intermediate modulus carbon fibers to form and analyze the performance of novel composite cathodes for structural power composites. Various slurries containing polyvinylidene fluoride (PVDF), active material powders, 1-methyl-2-pyrrolidone (NMP) and [...] Read more.
In this study, a selection of active materials were coated onto commercially available intermediate modulus carbon fibers to form and analyze the performance of novel composite cathodes for structural power composites. Various slurries containing polyvinylidene fluoride (PVDF), active material powders, 1-methyl-2-pyrrolidone (NMP) and carbon black (CB) were used to coat carbon fiber tows by immersion. Four active materials—lithium cobalt oxide (LCO), lithium iron phosphate (LFP), lithium nickel manganese cobalt oxide (NMC), and lithium nickel cobalt aluminum oxide (NCA)—were individually tested to assess their electrochemical reversibility. The cells were prepared with a polymer separator and liquid electrolytes and assembled in 2025-coin cells. Electrochemical analysis of the cathode materials showed that at C/5 and room temperature the measured capacities ranged from 39.8 Ah kg−1 to 64.7 Ah kg−1 for the LFP and NCA active materials, respectively. The full cells exhibited capacities of 18.1, 23.5, 27.2, and 28.2 Ah kg−1 after 55 cycles for LFP, LCO, NCA, and NMC811, respectively. Finally, visual and elemental analysis were performed via scanning electron microscope (SEM) and energy-dispersive x-ray (EDX) confirming desirable surface coverage and successful transfer of the active materials onto the carbon fiber tows. Full article
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13 pages, 3182 KB  
Article
Improved Electrochemical Performance Using Transition Metal Doped ZnNi/Carbon Nanotubes as Conductive Additive in Li/CFx Battery
by Fangmin Wang, Jiayin Li, Yuxin Zheng, Xue Dong, Yuzhen Zhao, Zemin He, Manni Li, Lei Lin, Danyang He, Zongcheng Miao, Haibo Zhang, Hua Tan and Jianfeng Huang
Catalysts 2025, 15(8), 758; https://doi.org/10.3390/catal15080758 - 8 Aug 2025
Viewed by 609
Abstract
Lithium/carbon fluoride (Li/CFx) batteries are promising for specialized applications due to their high theoretical capacity (>865 mAh·g−1) and energy density. However, their practical deployment is hindered by the intrinsically low conductivity of CFx and sluggish reaction kinetics. While [...] Read more.
Lithium/carbon fluoride (Li/CFx) batteries are promising for specialized applications due to their high theoretical capacity (>865 mAh·g−1) and energy density. However, their practical deployment is hindered by the intrinsically low conductivity of CFx and sluggish reaction kinetics. While conventional conductive additives improve electron transport, their physical mixing with active materials yields weak interfacial contacts and fails to catalytically facilitate C–F bond cleavage. To address these dual limitations, this study proposes a dual-functional conductive-catalytic additive strategy. We engineered zinc-nickel/carbon nanotube (ZnNi/CNT) composites modified with transition metal dopants (Fe, W, Cu) to integrate conductive networks with nanoscale-dispersed catalytic sites. Fe-doped ZnNi/CNT (ZnFeNiC) emerged as the optimal system, delivering a discharge plateau of 2.45 V and a specific capacity of 810.3 mAh·g−1 at 0.1 C. This performance is attributed to Fe-doping accelerates Li+ diffusion, and promotes reversible Ni redox transitions (Ni2+↔Ni0) that catalyze C–F bond dissociation. This work establishes a design paradigm for high-performance Li/CFx batteries, bridging the gap between conductive enhancement and catalytic activation. Full article
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19 pages, 3737 KB  
Article
Short-Term Morphological Response of Polypropylene Membranes to Hypersaline Lithium Fluoride Solutions: A Multiscale Modeling Approach
by Giuseppe Prenesti, Pierfrancesco Perri, Alessia Anoja, Agostino Lauria, Carmen Rizzuto, Alfredo Cassano, Elena Tocci and Alessio Caravella
Int. J. Mol. Sci. 2025, 26(15), 7380; https://doi.org/10.3390/ijms26157380 - 30 Jul 2025
Viewed by 515
Abstract
Understanding the early-stage physical interactions between polymeric membranes and supersaturated salt solutions is crucial for advancing membrane-assisted crystallization (MCr) processes. In this study, we employed molecular dynamics (MD) simulations to investigate the short-term morphological response of an isotactic polypropylene (PP) membrane in contact [...] Read more.
Understanding the early-stage physical interactions between polymeric membranes and supersaturated salt solutions is crucial for advancing membrane-assisted crystallization (MCr) processes. In this study, we employed molecular dynamics (MD) simulations to investigate the short-term morphological response of an isotactic polypropylene (PP) membrane in contact with LiF solutions at different concentrations (5.8 M and 8.9 M) and temperatures (300–353 K), across multiple time points (0, 150, and 300 ns). These data were used as input for computational fluid dynamics (CFD) analysis to evaluate structural descriptors of the membrane, including tortuosity, connectivity, void fraction, anisotropy, and deviatoric anisotropy, under varying thermodynamic conditions. The results show subtle but consistent rearrangements of polymer chains upon exposure to the hypersaline environment, with a marked reduction in anisotropy and connectivity, indicating a more compact and isotropic local structure. Surface charge density analyses further suggest a temperature- and concentration-dependent modulation of chain mobility and terminal group orientation at the membrane–solution interface. Despite localized rearrangements, the membrane consistently maintains a net negative surface charge. This electrostatic feature may influence ion–membrane interactions during the crystallization process. While these non-reactive, short-timescale simulations do not capture long-term degradation or fouling mechanisms, they provide mechanistic insight into the initial physical response of PP membranes under MCr-relevant conditions. This study lays a computational foundation for future investigations bridging atomistic modeling and membrane performance in real-world applications. Full article
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18 pages, 4914 KB  
Article
Preparation and Failure Behavior of Gel Electrolytes for Multilayer Structure Lithium Metal Solid-State Batteries
by Chu Chen, Wendong Qin, Qiankun Hun, Yujiang Wang, Xinghua Liang, Renji Tan, Junming Li and Yifeng Guo
Gels 2025, 11(8), 573; https://doi.org/10.3390/gels11080573 - 23 Jul 2025
Viewed by 520
Abstract
High safety gel polymer electrolyte (GPE) is used in lithium metal solid state batteries, which has the advantages of high energy density, wide temperature range, high safety, and is considered as a subversive new generation battery technology. However, solid-state lithium batteries with multiple [...] Read more.
High safety gel polymer electrolyte (GPE) is used in lithium metal solid state batteries, which has the advantages of high energy density, wide temperature range, high safety, and is considered as a subversive new generation battery technology. However, solid-state lithium batteries with multiple layers and large capacity currently have poor cycle life and a large gap between the actual output cycle capacity retention rate and the theoretical level. In this paper, polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP)/polyacrylonitrile (PAN)—lithium perchlorate (LiClO4)—lithium lanthanum zirconium tantalate (LLZTO) gel polymer electrolytes was prepared by UV curing process using a UV curing machine at a speed of 0.01 m/min for 10 s, with the temperature controlled at 30 °C and wavelength 365 nm. In order to study the performance and failure mechanism of multilayer solid state batteries, single and three layers of solid state batteries with ceramic/polymer composite gel electrolyte were assembled. The results show that the rate and cycle performance of single-layer solid state battery with gel electrolyte are better than those of three-layer solid state battery. As the number of cycles increases, the interface impedance of both single-layer and three-layer electrolyte membrane solid-state batteries shows an increasing trend. Specifically, the three-layer battery impedance increased from 17 Ω to 42 Ω after 100 cycles, while the single-layer battery showed a smaller increase, from 2.2 Ω to 4.8 Ω, indicating better interfacial stability. After 100 cycles, the interface impedance of multi-layer solid-state batteries increases by 9.61 times that of single-layer batteries. After 100 cycles, the corresponding capacity retention rates were 48.9% and 15.6%, respectively. This work provides a new strategy for large capacity solid state batteries with gel electrolyte design. Full article
(This article belongs to the Special Issue Research Progress and Application Prospects of Gel Electrolytes)
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15 pages, 4059 KB  
Article
Surface Fluorination for the Stabilization in Air of Garnet-Type Oxide Solid Electrolyte for Lithium Ion Battery
by Michael Herraiz, Saida Moumen, Kevin Lemoine, Laurent Jouffret, Katia Guérin, Elodie Petit, Nathalie Gaillard, Laure Bertry, Reka Toth, Thierry Le Mercier, Valérie Buissette and Marc Dubois
Batteries 2025, 11(7), 268; https://doi.org/10.3390/batteries11070268 - 16 Jul 2025
Viewed by 646
Abstract
After reviewing the state of the art of the fluorination of inorganic solid electrolytes, an application of gas/solid fluorination is given and how it can be processed. Garnet-type oxide has been chosen. These oxides with an ideal structure of chemical formula A3 [...] Read more.
After reviewing the state of the art of the fluorination of inorganic solid electrolytes, an application of gas/solid fluorination is given and how it can be processed. Garnet-type oxide has been chosen. These oxides with an ideal structure of chemical formula A3B2(XO4)3 are mainly known for their magnetic and dielectric properties. Certain garnets may have a high enough Li+ ionic conductivity to be used as solid electrolyte of lithium ion battery. The surface of LLZO may be changed in contact with the moisture and CO2 present in the atmosphere that results in a change of the conductivity at the interface of the solid. LiOH and/or lithium carbonate are formed at the surface of the garnet particles. In order to allow for handling and storage under normal conditions of this solid electrolyte, surface fluorination was performed using elemental fluorine. When controlled using mild conditions (temperature lower or equal to 200 °C, either in static or dynamic mode), the addition of fluorine atoms to LLZO with Li6,4Al0,2La3Zr2O12 composition is limited to the surface, forming a covering layer of lithium fluoride LiF. The effect of the fluorination was evidenced by IR, Raman, and NMR spectroscopies. If present in the pristine LLZO powder, then the carbonate groups disappear. More interestingly, contrary to the pristine LLZO, the contents of these groups are drastically reduced even after storage in air up to 45 days when the powder is covered with the LiF layer. Surface fluorination could be applied to other solid electrolytes that are air sensitive. Full article
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14 pages, 4141 KB  
Article
Preparation and Electrochemical Performance of Zinc-Doped Copper Fluoride
by Peng Dou, Pengcheng Liu and Zhiyong Yu
Energies 2025, 18(14), 3752; https://doi.org/10.3390/en18143752 - 15 Jul 2025
Viewed by 339
Abstract
To enhance the specific energy and rate performance of lithium primary batteries, the development of advanced cathode materials with superior electrochemical properties is essential. Fluorides, composed of light fluorine elements and multivalent cations, exhibit multi-electron reaction characteristics, possess a high theoretical voltage, and [...] Read more.
To enhance the specific energy and rate performance of lithium primary batteries, the development of advanced cathode materials with superior electrochemical properties is essential. Fluorides, composed of light fluorine elements and multivalent cations, exhibit multi-electron reaction characteristics, possess a high theoretical voltage, and demonstrate high discharge-specific energy. However, owing to fluorine’s high electronegativity, which leads to the formation of strong ionic bonds with other elements, most fluorides exhibit poor electronic conductivity, thereby constraining their electrochemical performance when used as cathode materials. Copper fluoride (CuF2) exhibits a high theoretical specific capacity and discharge voltage but is constrained by its large bandgap, poor electronic conductivity, and difficulties in synthesizing anhydrous CuF2 materials, which significantly limit its electrochemical activity. In this study, zinc (Zn) was chosen as a dopant for copper fluoride. By combining theoretical calculations with experimental validation, the impacts of Zn doping on the structural stability and electrochemical performance of copper fluoride were comprehensively analyzed. The resultant highly active Zn-doped copper fluoride achieved a discharge specific capacity of 528.6 mAh/g at 0.1 C and 489.1 mAh/g at 1 C, showcasing superior discharge-specific energy and good rate performance. This material holds great potential as a promising cathode candidate for lithium batteries, providing both high specific energy and power density. Full article
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14 pages, 4456 KB  
Article
Investigation into PVDF-HFP and PVP Polymer Blend Electrolytes with Lithium Ions for Energy Storage Application
by Bilash Jyoti Gogoi, M. Murugesan, N. Nallamuthu, P. Devendran, Arumugam Murugan, Radak Blange and Muthaiah Shellaiah
Polymers 2025, 17(13), 1758; https://doi.org/10.3390/polym17131758 - 25 Jun 2025
Viewed by 1244
Abstract
To improve solid-state lithium batteries, solution casting has been employed to create lithium ion-conducting copolymer electrolytes involving poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)/polyvinylpyrrolidone (PVP) blend polymers with various compositions. Following X-ray diffraction and Fourier transformation (FTIR), the structural characterisation and identification of molecular bonding in polymer [...] Read more.
To improve solid-state lithium batteries, solution casting has been employed to create lithium ion-conducting copolymer electrolytes involving poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)/polyvinylpyrrolidone (PVP) blend polymers with various compositions. Following X-ray diffraction and Fourier transformation (FTIR), the structural characterisation and identification of molecular bonding in polymer electrolytes were confirmed. Through AC impedance analysis, the electrical characteristics of the solid-state polymer films were investigated. The dielectric conductivity of the sample was found to obey the modified Arrhenius relationship, while in the case of a sample with higher conductivity, it followed Arrhenius behaviour. The relaxation parameters and dielectric behaviour of the samples are demonstrated and discussed. Full article
(This article belongs to the Special Issue Advanced Polymer Materials for Safe Ion Batteries)
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