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Keywords = PVDF-co-HFP

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13 pages, 2345 KB  
Article
Low-Power Electrochromic Displays Based on Electrocatalytic Counter Electrodes and PVDF-HFP Gel Polymer Electrolyte
by Liangliang Wu, Lili Liu, Fengchao Li, Qiang Li and Lingqi Wu
Materials 2026, 19(7), 1364; https://doi.org/10.3390/ma19071364 - 30 Mar 2026
Viewed by 382
Abstract
Electrochromic devices have emerged as promising candidates for non-emissive displays due to their particular photoelectric performance in complex lighting environments. They exhibit considerable potential in emerging fields such as Internet of Things terminals, flexible wearables and human–computer interaction interfaces. In this study, we [...] Read more.
Electrochromic devices have emerged as promising candidates for non-emissive displays due to their particular photoelectric performance in complex lighting environments. They exhibit considerable potential in emerging fields such as Internet of Things terminals, flexible wearables and human–computer interaction interfaces. In this study, we developed a low-power electrochromic display based on a Pt/FTO (Fluorine doped tin oxide) electrocatalytic counter electrode and a Poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) porous gel electrolyte. The Pt catalyst enhances Br/Br3− redox reactivity, which reduces the driving voltage from 2 V to 1 V, and accelerates the electrode reaction kinetics. It is systematically explained by the Density Functional Theory (DFT) calculations and electrochemical characterization. Furthermore, we demonstrate a proof-of-concept multicolor display incorporating the electrocatalytic counter electrode with various viologen derivatives. This approach provides a significant advancement toward next-generation high-performance displays and is supportive of the development of energy-efficient optoelectronic devices. Full article
(This article belongs to the Section Catalytic Materials)
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17 pages, 4143 KB  
Article
Simultaneous Optimization of Bulk Ion Transport and Interfacial Stability in Gel Polymer Electrolytes via a Multifunctional Triazole Additive
by Jie Zhao, Yubo Cheng, Maoyi Yi, Chunman Zheng and Qingpeng Guo
Batteries 2026, 12(3), 101; https://doi.org/10.3390/batteries12030101 - 16 Mar 2026
Viewed by 431
Abstract
Gel polymer electrolytes (GPEs) typically suffer from sluggish kinetics and interfacial instability at elevated temperatures and high voltages. Herein, 3-(trifluoromethyl)-1H-1,2,4-triazole (TTA) is employed to construct an ultrathin (~25 μm), robust, and homogeneous GPE. TTA acts as a molecular bridge, significantly improving compatibility between [...] Read more.
Gel polymer electrolytes (GPEs) typically suffer from sluggish kinetics and interfacial instability at elevated temperatures and high voltages. Herein, 3-(trifluoromethyl)-1H-1,2,4-triazole (TTA) is employed to construct an ultrathin (~25 μm), robust, and homogeneous GPE. TTA acts as a molecular bridge, significantly improving compatibility between the PVDF-HFP (Poly(vinylidene fluoride-co-hexafluoropropylene)) matrix and LLZTO (Li6.4La3Zr1.4Ta0.6O12) fillers to create continuous ion-conducting pathways. Consequently, the TTA-GPEs exhibits high ionic conductivity (0.267 mS cm−1 at room temperature), low activation energy (0.181 eV), and an increased lithium-ion transference number (0.425). Advanced surface analysis reveals that TTA preferentially reacts to form a dense, gradient hierarchical interphase (solid electrolyte interphase/cathode electrolyte interphase, SEI/CEI) enriched with inorganic species (LiF, Li3N, and Li2S) on the inner side. This architecture suppresses parasitic reactions and lithium dendrite growth. Accordingly, NCM811(LiNi0.8Co0.1Mn0.1O2)//Li batteries with TTA-GPEs demonstrate stable cycling at 80 °C and 1C, retaining 57.68% capacity after 125 cycles—significantly outperforming benchmarks. This study offers a molecular engineering strategy to simultaneously optimize bulk transport and interfacial stability for high-energy-density solid-state batteries. Full article
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17 pages, 5259 KB  
Article
Harnessing the Dual-Charge Characteristics of Halloysite Nanotubes for High-Performance Composite Polymer Electrolytes in Lithium-Ion Batteries
by Yunxiang Li, Xuehui Li, Ke Wang, Peilin Chen, Xiaowei Li, Guocheng Lv and Libing Liao
Minerals 2026, 16(3), 307; https://doi.org/10.3390/min16030307 - 14 Mar 2026
Viewed by 312
Abstract
Naturally occurring halloysite nanotubes (HNTs), a clay mineral characterized by a unique dual-charge architecture, offer a promising strategy for enhancing the performance of composite polymer electrolyte (CPE). In this work, HNTs are introduced as a low-cost, functional filler to simultaneously address two key [...] Read more.
Naturally occurring halloysite nanotubes (HNTs), a clay mineral characterized by a unique dual-charge architecture, offer a promising strategy for enhancing the performance of composite polymer electrolyte (CPE). In this work, HNTs are introduced as a low-cost, functional filler to simultaneously address two key limitations of poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)-based CPE: low ionic conductivity and inadequate lithium-ion transference number. The negatively charged outer surface of HNTs facilitates Li+ transport, while the positively charged inner lumen confines anions such as TFSI. Controlled acid etching (6 M HCl, 12 h) further optimizes this structure by removing surface impurities and enlarging the lumen, thereby enhancing both charge-directed ion transport pathways. The resulting HNT-modified CPE achieves a high ionic conductivity of 6.1 × 10−4 S⋅cm−1 and a Li+ transference number of 0.73. When assembled into Li||CPE||LiFePO4 cells, the electrolyte enables stable cycling over 300 cycles at 0.2C, retains 119.2 mAh/g at 2C, and delivers 85.7 mAh/g even at 5C, demonstrating excellent cycling stability and rate capability. This study reveals the potential of mineral-derived nanomaterials, with their inherent structural and physicochemical properties, to serve as key functional components in high-performance batteries. Full article
(This article belongs to the Special Issue Clay Minerals for Environmental Remediation and Sustainable Energy)
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22 pages, 2829 KB  
Article
Preparation of Poly(vinylidene fluoride-co-hexafluoropropylene) Doped Cellulose Acetate Films for the Treatment of Calcium-Based Hardness from Aqueous Solution
by Khaleke Veronicah Ramollo, Lutendo Evelyn Macevele, Abayneh Ataro Ambushe and Takalani Magadzu
Physchem 2025, 5(4), 45; https://doi.org/10.3390/physchem5040045 - 20 Oct 2025
Viewed by 1098
Abstract
Calcium (Ca2+ ions) is one of the dominant elements that contribute to water hardness, scaling in pipes, bathroom faucets, and kitchen utensils. Herein, we report on the development of poly(vinylidene fluoride-co-hexafluoropropylene) cellulose acetate (PVDF-HFP/CA) films for the treatment of Ca2+ ions [...] Read more.
Calcium (Ca2+ ions) is one of the dominant elements that contribute to water hardness, scaling in pipes, bathroom faucets, and kitchen utensils. Herein, we report on the development of poly(vinylidene fluoride-co-hexafluoropropylene) cellulose acetate (PVDF-HFP/CA) films for the treatment of Ca2+ ions as one of the constituents that causes water hardness. CA and PVDF-HFP polymers, and their blend consisting of 3 wt.% PVDF-HFP/CA, were effectively synthesised through the phase inversion technique. Analysis using thermogravimetric analysis (TGA), Fourier transform infrared (FTIR) spectroscopy, and scanning electron microscopy (SEM) confirmed the effective incorporation of 3 wt.% PVDF-HFP into the cellulose acetate film. Parameters such as temperature, initial concentration, pH, adsorbent dosage and contact time were investigated in batch studies during the removal of Ca2+ ions in synthetic water samples. Under optimal conditions (pH 7, adsorbent dosage of 0.5 mg/L, and concentration of 120 mg/L), the 3 wt.% PVDF-HFP/CA film achieved a 99% adsorption efficiency for Ca2+ ions in 90 min. The adsorption process adhered to pseudo-second-order and Freundlich isotherm models, which suggest that the adsorption of Ca2+ ions is heterogeneous. The maximum adsorption efficiency achieved was 56 mg/g, indicating an endothermic physisorption process. The 3 wt.% PVDF-HFP/CA film maintained higher adsorption in the presence of counter ions and in a binary system, and it could be recycled at least three times. Thus, the findings demonstrated that the 3 wt.% PVDF-HFP/CA film could be a valuable material for Ca2+ ions removal to acceptable drinking water levels. Full article
(This article belongs to the Section Surface Science)
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12 pages, 1639 KB  
Article
Assessing the Stability of Polymer Inclusion Membranes: The Case of Aliquat 336-Based Membranes
by Kalina Velikova, Todor Dudev, Tsveta Sarafska, Lea Kukoc-Modun, Spas D. Kolev and Tony Spassov
Membranes 2025, 15(10), 309; https://doi.org/10.3390/membranes15100309 - 13 Oct 2025
Cited by 2 | Viewed by 1149
Abstract
Leaching of the extractant from polymer inclusion membranes (PIMs) into the feed and receiving aqueous solutions shortens their life. Therefore, when a particular PIM extractant has been selected, it is important to choose a base polymer that will minimize to the greatest extent [...] Read more.
Leaching of the extractant from polymer inclusion membranes (PIMs) into the feed and receiving aqueous solutions shortens their life. Therefore, when a particular PIM extractant has been selected, it is important to choose a base polymer that will minimize to the greatest extent extractant leaching compared to other base polymers, thus providing the best stability of the PIM. However, comparisons of the stability of PIMs composed of the same extractant and different base polymers is usually conducted by multiple cycles of extraction and back-extraction steps, which are time-consuming and labor-intensive. An alternative approach based on thermal analysis (thermogravimetric analysis (TGA) and differential thermal analysis (DTA)) was developed and applied to PIMs containing 40 wt.% Aliquat 336, one of the most frequently used PIM extractants, and the three most frequently used PIM base polymers, i.e., poly(vinyl chloride) (PVC), cellulose triacetate (CTA), and poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP). The temperatures and enthalpies associated with Aliquat 336 release were compared, with PVDF-HFP exhibiting the highest values, indicating the strongest interaction between the extractant and the polymer matrix and, thus, the highest stability. The PVC-based PIM was predicted to be the most prone to extractant leaching among the PIMs studied. This stability ranking was confirmed theoretically by quantum chemistry (DFT) calculations, which provided molecular-level insights into the likely interaction sites between Aliquat 336 and the polymer chains. An experimental validation of the above leaching order was also provided by PIM leaching experiments in aqueous 0.1 M and 0.05 M NaCl solutions, where membrane mass losses over a 24 h period were determined. The results of the current study demonstrated thermal analysis to be a fast and viable approach in comparing the stability of PIMs with the same extractant but different base polymers. Full article
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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 2751
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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22 pages, 4829 KB  
Article
Development of a Flexible and Conductive Heating Membrane via BSA-Assisted Electroless Plating on Electrospun PVDF-HFP Nanofibers
by Mun Jeong Choi, Dae Hyeob Yoon, Yoo Sei Park, Hyoryung Nam and Geon Hwee Kim
Appl. Sci. 2025, 15(14), 8023; https://doi.org/10.3390/app15148023 - 18 Jul 2025
Cited by 1 | Viewed by 1459
Abstract
Planar heaters are designed to deliver uniform heat across broad surfaces and serve as critical components in applications requiring energy efficiency, safety, and mechanical flexibility, such as wearable electronics and smart textiles. However, conventional metal-based heaters are limited by poor adaptability to curved [...] Read more.
Planar heaters are designed to deliver uniform heat across broad surfaces and serve as critical components in applications requiring energy efficiency, safety, and mechanical flexibility, such as wearable electronics and smart textiles. However, conventional metal-based heaters are limited by poor adaptability to curved or complex surfaces, low mechanical compliance, and susceptibility to oxidation-induced degradation. To overcome these challenges, we applied a protein-assisted electroless copper (Cu) plating strategy to electrospun poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) nanofiber substrates to fabricate flexible, conductive planar heating membranes. For interfacial functionalization, a protein-based engineering approach using bovine serum albumin (BSA) was employed to facilitate palladium ion coordination and seed formation. The resulting membrane exhibited a dense, continuous Cu coating, low sheet resistance, excellent durability under mechanical deformation, and stable heating performance at low voltages. These results demonstrate that the BSA-assisted strategy can be effectively extended to complex three-dimensional fibrous membranes, supporting its scalability and practical potential for next-generation conformal and wearable planar heaters. Full article
(This article belongs to the Section Applied Thermal Engineering)
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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
Cited by 3 | Viewed by 3116
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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12 pages, 2463 KB  
Article
Metal–Organic Frameworks (MOF)-Derived Gel Electrolyte via UV Cross-Linking for High-Performance Lithium Metal Batteries
by Naiyao Mao, Lingxiao Lan, Qiankun Hun, Jianghua Wei, Xinghua Liang and Yifeng Guo
Gels 2025, 11(6), 409; https://doi.org/10.3390/gels11060409 - 29 May 2025
Cited by 4 | Viewed by 1903
Abstract
Gel electrolytes (GEs) play a pivotal role in the advancement of lithium metal batteries by offering high energy density and enhanced rate capability. Nevertheless, their real-world application is hampered by relatively low ionic conductivity and significant interfacial resistance at room temperatures. In this [...] Read more.
Gel electrolytes (GEs) play a pivotal role in the advancement of lithium metal batteries by offering high energy density and enhanced rate capability. Nevertheless, their real-world application is hampered by relatively low ionic conductivity and significant interfacial resistance at room temperatures. In this work, we developed a gel electrolyte membrane (GEM) by embedding Zeolitic Imidazolate Framework-8 (ZIF-8) metal–organic frameworks (MOFs) material into a poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) matrix through UV curing. The composite membrane, with 4 wt% ZIF-8, exhibited an ionic conductivity of 1.17 × 10−3 S/cm, an electrochemical stability window of 4.7 V, and a lithium-ion transference number of 0.7. The test results indicate that the electrochemical performance of LFP//GEM//Li battery has an initial specific capacity of 168 mAh g−1 at 0.1 C rate. At 1 C, the discharge capacity was 88 mAh g−1, and at 2 C, it was 68 mAh g−1. Enhanced ionic transport, improved electrochemical stability, and optimized lithium-ion migration collectively contributed to superior rate performance and prolonged cycle life. This study offers novel insights and methodological advances for next-generation lithium metal batteries technologies. Full article
(This article belongs to the Special Issue Research Progress and Application Prospects of Gel Electrolytes)
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14 pages, 4225 KB  
Article
Preparation and Performance of PVDF-HFP/PAN-Based Gel Polymer Electrolytes
by Xiubing Yao, Lingxiao Lan, Qiankun Hun, Xuanan Lu, Jianghua Wei, Xinghua Liang, Pengcheng Shen, Ying Long and Yifeng Guo
Gels 2025, 11(5), 317; https://doi.org/10.3390/gels11050317 - 24 Apr 2025
Cited by 7 | Viewed by 5433
Abstract
Solid-state electrolytes are widely expected to enhance the performance of lithium-ion batteries, providing higher energy density and improved safety. However, challenges still need to be solved in their practical application due to low ionic conductivity and high interfacial resistance at room temperature. In [...] Read more.
Solid-state electrolytes are widely expected to enhance the performance of lithium-ion batteries, providing higher energy density and improved safety. However, challenges still need to be solved in their practical application due to low ionic conductivity and high interfacial resistance at room temperature. In this study, we successfully developed a high-performance gel polymer electrolyte (GPEs) by blending poly(vinylidene fluoride-co-hexafluoropropylene)(PVDF-HFP) and polyacrylonitrile (PAN) through UV curing, cross-linking with ethoxylated trimethylolpropane triacrylate (ETPTA), and incorporating Li6.4La3Zr1.4Ta0.6O12 (LLZTO). At room temperature, the ionic conductivity of the GPEs was 2.8 × 10−4 S/cm, with a lithium-ion transference number of 0.6. Moreover, during lithium plating/stripping tests, the assembled Li/PPEL/Li symmetric cell exhibited stable cycling for up to 600 h at a current density of 0.1 mA/cm2. Notably, the GPEs enabled the LiFePO4/GPEs/Li battery to achieve excellent performance, delivering high discharge capacities at room temperature (164.3 mAh g−1 at 0.1 C and 88.8 mAh g−1 at 1 C), with a capacity retention of 89.4% after 200 cycles at 0.5 C. Therefore, solid-state batteries using this electrolyte exhibit excellent performance, including adequate capacity and cycling stability. Full article
(This article belongs to the Special Issue Research Progress and Application Prospects of Gel Electrolytes)
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16 pages, 3222 KB  
Article
Anisotropic Conductivity and Mechanical Strength Enhancements in Gel Polymer Electrolyte Films by Hot Pressing
by Zhifan Fang, Hao Zhang and Shuangjun Chen
Materials 2025, 18(8), 1751; https://doi.org/10.3390/ma18081751 - 11 Apr 2025
Cited by 3 | Viewed by 1164
Abstract
Gel polymer electrolyte (GPE) with a polymer matrix swollen in liquid electrolytes offers several advantages over conventional liquid electrolytes, including no leakage, lightweight properties, and high reliability. While poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)-based GPEs show promise for lithium-ion batteries, their practical application is hindered by [...] Read more.
Gel polymer electrolyte (GPE) with a polymer matrix swollen in liquid electrolytes offers several advantages over conventional liquid electrolytes, including no leakage, lightweight properties, and high reliability. While poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)-based GPEs show promise for lithium-ion batteries, their practical application is hindered by the intrinsic trade-off between ionic conductivity and mechanical robustness in conventional PVDF systems. Typical strategies relying on excessive plasticizers (e.g., ionic liquids) compromise mechanical integrity. Here, we propose a novel hot-pressing-induced recrystallization strategy to synergistically enhance both anisotropic ionic conductivity and puncture strength in PVDF-based GPE films. By blending PVDF with controlled amounts of 1-hexyl-3-methylimidazolium chloride ([HMIM]Cl), followed by solution casting and hot pressing, we achieve microstructural reorganization that dramatically improves through-thickness ion transport and mechanical performance. Crucially, hot-pressed PVDF with only 25 wt% [HMIM]Cl exhibits a 12.5-fold increase in ionic conductivity (reaching 4.7 × 10−4 S/cm) compared to its solution-cast counterparts. Remarkably, this formulation surpasses the conductivity of PVDF-HFP composites with a higher [HMIM]Cl content (35 wt%, 1.7 × 10−4 S/cm), demonstrating performance optimization of anisotropic conductivity. What is more, the mechanical strength of the piercing strength perpendicular to the GPE film after hot pressing increased by 42% compared to the solution-cast film. This work establishes a scalable processing route to break the conductivity–strength dichotomy in GPEs, offering critical insights for designing high-performance polymer electrolytes. Full article
(This article belongs to the Special Issue Polymer Electrolytes: Fundamentals, Approaches and Applications)
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14 pages, 4382 KB  
Article
One-Step Fabrication of Poly(vinylidene Fluoride-Co-Hexafluoropropylene)/Perfluorodecyltriethoxysilane Fibrous Membranes with Waterproof, Breathable, and Radiative Cooling Properties
by Aohan Hou, Juan Xie, Xiaohui Wu, Guichun Lin, Yayi Yuan, Xi Liu, Yancheng Wu, Feng Gan, Yangling Li, Yuxiao Wu, Gang Huang, Zhengrong Li and Jing Zhao
Molecules 2025, 30(4), 763; https://doi.org/10.3390/molecules30040763 - 7 Feb 2025
Cited by 3 | Viewed by 1970
Abstract
Functional membranes with waterproof, breathable, and thermal regulation capabilities are increasingly sought after across various industries. However, developing such functional membranes commonly involves complex multi-step preparation processes. Herein, we introduced perfluorodecyltriethoxysilane (FAS) into the poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) solution for one-step electrospinning, successfully fabricating [...] Read more.
Functional membranes with waterproof, breathable, and thermal regulation capabilities are increasingly sought after across various industries. However, developing such functional membranes commonly involves complex multi-step preparation processes. Herein, we introduced perfluorodecyltriethoxysilane (FAS) into the poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) solution for one-step electrospinning, successfully fabricating membranes that combine these properties. The hydrophobicity of the PVDF-HFP/FAS membrane was greatly improved with the water contact angle increased from 120.6° to 142.9° and the solar reflectance rising from 72% to 92% due to the presence of fluorocarbon segments. The synergistic effect of enhanced hydrophobicity, small pore size, and elevated solar reflectivity resulted in robust water resistance (62 kPa), excellent water vapor transmission rate (12.4 kg m−2 d−1), and superior cooling performance (6.4 °C lower than commercial cotton fabrics). These findings suggest that the proposed PVDF-HFP/FAS membranes, characterized by desired multifunction characteristics and scalable production, hold great potential for application in diverse strategic fields. Full article
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24 pages, 5157 KB  
Article
Ceramic-Rich Composite Separators for High-Voltage Solid-State Batteries
by Kevin Vattappara, Martin Finsterbusch, Dina Fattakhova-Rohlfing, Idoia Urdampilleta and Andriy Kvasha
Batteries 2025, 11(2), 42; https://doi.org/10.3390/batteries11020042 - 21 Jan 2025
Cited by 1 | Viewed by 4210
Abstract
Composite solid electrolytes are gaining interest regarding their use in Li-metal solid-state batteries. Although high ceramic content improves the electrochemical stability of ceramic-rich composite separators (C-SCE), the polymeric matrix also plays a vital role. In the first generation of C-SCE separators with a [...] Read more.
Composite solid electrolytes are gaining interest regarding their use in Li-metal solid-state batteries. Although high ceramic content improves the electrochemical stability of ceramic-rich composite separators (C-SCE), the polymeric matrix also plays a vital role. In the first generation of C-SCE separators with a PEO-based matrix, the addition of 90–95 wt% of Li6.45Al0.05La3Zr1.6Ta0.4O12 (LLZO) does not make C-SCE stable for cell cycling with high-voltage (HV) cathodes. For the next iteration, the objective was to find an HV-stable polymeric matrix for C-SCEs. Herein, we report results on optimizing C-SCE separators with different ceramics and polymers which can craft the system towards better stability with NMC622-based composite cathodes. Both LLZO and Li1.3Al0.3Ti1.7(PO4)3 (LATP) were utilized as ceramic components in C-SCE separators. Poly(diallyldimethylammonium) bis(trifluoromethanesulfonyl)imide (PDDA-TFSI) and poly (vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) were used as polymers in the “polymer/LiTFSI/plasticizer”-based matrix. The initial phase of the selection criteria for the separator matrix involved assessing mechanical stability and ionic conductivity. Two optimized separator formulations were then tested for their electrochemical stability with both Li metal and HV composite cathodes. The results showed that Li/NMC622 cells with LP70_PVDF_HFP and LZ70_PDDA-TFSI separators exhibited more stable cycling performance compared to those with LZ90_PEO300k-based separators. Full article
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13 pages, 3118 KB  
Article
Preparation and Study of Poly(Vinylidene Fluoride-Co-Hexafluoropropylene)-Based Composite Solid Electrolytes
by Meihong Huang, Lingxiao Lan, Pengcheng Shen, Zhiyong Liang, Feng Wang, Yuling Zhong, Chaoqun Wu, Fanxiao Kong and Qicheng Hu
Crystals 2024, 14(11), 982; https://doi.org/10.3390/cryst14110982 - 14 Nov 2024
Cited by 4 | Viewed by 2343
Abstract
Solid-state electrolytes are widely anticipated to revitalize lithium-ion batteries with high energy density and safety. However, low ionic conductivity and high interfacial resistance at room temperature pose challenges for practical applications. This study combines the rigid oxide electrolyte LLZTO with the flexible polymer [...] Read more.
Solid-state electrolytes are widely anticipated to revitalize lithium-ion batteries with high energy density and safety. However, low ionic conductivity and high interfacial resistance at room temperature pose challenges for practical applications. This study combines the rigid oxide electrolyte LLZTO with the flexible polymer electrolyte poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) to achieve effective coupling of rigidity and flexibility. The semi-interpenetrating network structure endows the PEL composite solid electrolyte with excellent lithium-ion transport capabilities, resulting in an ionic conductivity of up to 5.1 × 10−4 S cm−1 and lithium-ion transference number of 0.41. The assembled LiFePO4/PEL/Li solid-state battery demonstrates an initial discharge capacity of 132 mAh g−1 at a rate of 0.1 C. After 100 charge–discharge cycles, the capacity retention is 81%. This research provides a promising strategy for preparing composite solid electrolytes in solid-state lithium-ion batteries. Full article
(This article belongs to the Special Issue Research on Electrolytes and Energy Storage Materials)
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14 pages, 2445 KB  
Article
Electronically Conductive Polymer Enhanced Solid-State Polymer Electrolytes for All-Solid-State Lithium Batteries
by Md Gulam Smdani, Md Wahidul Hasan, Amir Abdul Razzaq and Weibing Xing
Energies 2024, 17(17), 4295; https://doi.org/10.3390/en17174295 - 28 Aug 2024
Cited by 4 | Viewed by 4250
Abstract
All-solid-state lithium batteries (ASSLBs) have gained enormous interest due to their potential high energy density, high performance, and inherent safety characteristics for advanced energy storage systems. Although solid-state ceramic (inorganic) electrolytes (SSCEs) have high ionic conductivity and high electrochemical stability, they experience some [...] Read more.
All-solid-state lithium batteries (ASSLBs) have gained enormous interest due to their potential high energy density, high performance, and inherent safety characteristics for advanced energy storage systems. Although solid-state ceramic (inorganic) electrolytes (SSCEs) have high ionic conductivity and high electrochemical stability, they experience some significant drawbacks, such as poor electrolyte/electrode interfacial properties and poor mechanical characteristics (brittle, fragile), which can hinder their adoption for commercialization. Typically, SSCE-based ASSLBs require high cell stack pressures exerted by heavy fixtures for regular operation, which can reduce the energy density of the overall battery packages. Polymer–SSCE composite electrolytes can provide inherently good interfacial contacts with the electrodes that do not require high cell stack pressures. In this study, we explore the feasibility of incorporating an electronically and ionically conducting polymer, polypyrrole (PPy), into a polymer backbone, polyvinylidene fluoride-co-hexafluoropropylene (PVDF-HFP), to improve the ionic conductivity of the resultant polymer–SSCE composite electrolyte (SSPE). The electronically conductive polymer-incorporated composite electrolyte showed superior room temperature ionic conductivity and electrochemical performance compared to the baseline sample (without PPy). The PPy-incorporated polymer electrolyte demonstrated a high resilience to high temperature operation compared with the liquid-electrolyte counterpart. This performance advantage can potentially be employed in ASSLBs that operate at high temperatures. In our recent development efforts, SSPEs with optimal formulations showed room temperature ionic conductivity of 2.5 × 10−4 S/cm. The data also showed, consistently, that incorporating PPy into the polymer backbone helped boost the ionic conductivity with various SSPE formulations, consistent with the current study. Electrochemical performance of ASSLBs with the optimized SSPEs will be presented in a separate publication. The current exploratory study has shown the feasibility and benefits of the novel approach as a promising method for the research and development of next-generation solid composite electrolyte-based ASSLBs. Full article
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