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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Synergistic Enhancement of Biaxial Stretching and Multilayer Composites in All-Solid-State Polymer Electrolytes

Zhitao Yang,Zhen Zhang,Yong Liu,Yiping Fang,Cheng Li

As an important component of lithium-ion batteries, all-solid-state electrolytes should possess high ionic conductivity, excellent flexibility, and relatively high mechanical strength. All-solid-state polymer electrolytes (ASSPEs) based on polymers seem to be able to meet these requirements. However, pure ASSPEs have relatively low ionic conductivity, and the addition of inorganic fillers such as lithium salts will reduce their flexibility and mechanical strength. To address the above issues, in this paper, the solvent-free method was used to prepare a poly(vinylidenefluoride-co-hexafluoropropylene)/lithium bis(trifluoromethanesulfonyl) imide/poly(ethylene oxide) all-solid-state polymer electrolyte, which was then subjected to 4 × 4 magnification synchronous bidirectional stretching. Subsequently, it was multilayered with PEO-based composite polymer electrolytes to obtain multilayered composite polymer electrolytes (MCPEs). Bidirectional stretching provides superior in-plane and out-of-plane mechanical properties to MCPEs by inducing molecular chain orientation, which suppresses the growth of lithium dendrites. Concurrently, it facilitates the formation of the β-crystal form of PVDF-HFP, thereby weakening the ion solvation effect and reducing the lithium-ion migration energy barrier. Multilayered compounding improves the interfacial contact between MCPEs and electrodes, thereby reducing the interfacial impedance. Experiments have demonstrated that the MCPEs prepared in this paper exhibit high ionic conductivity at room temperature (1.83 × 10–4 S cm–1), low interfacial resistance (547 Ω cm–2), excellent mechanical properties (26 MPa), and excellent cycling rate performance (a capacity retention rate of 90% after 110 cycles at 0.1 C), which can meet the performance requirements of lithium-ion batteries for ASSPEs.

CAS / MDL: 90076-65-6 872-50-4
研究领域: 材料科学 · 电化学 · 能源存储 · 高分子科学
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eTransportation · 2023 · IF 11.9

Scalable wet-slurry fabrication of sheet-type electrodes for sulfide all-solid-state batteries and performance enhancement via optimization of Ni-rich cathode coating layer

Jing Gao,Jinghua Hao,Yuan Gao,Xiaolin Sun,Yuan Zhang,Depeng Song,Qing Zhao,Fuhua Zhao,Wenyan Si,Kun Wang,Takeo Ohsaka,Futoshi Matsumoto,Jianfei Wu,Haijiao Xie

All-solid-state Li or Li-ion batteries (ASSLBs) have attracted much attention due to their potential high energy density, high safety, and low manufacturing costs compared to commercial liquid electrolyte Li-ion batteries. However, the rate capacity and cycling performance could not satisfy the practical application. Here, an island-like amorphous Li 2 O–ZrO 2 (LZO) was coated on the surface of LiNi 0.88 Co 0.10 Al 0.02 (NCA) via a sol-gel method and low-temperature sintering. The electrochemical performance and density functional theory calculation results demonstrate that the LZO coating layer significantly boosts Li-ions transfer. Targeting large-scale production, a sheet-type cathode was prepared by a wet-slurry process with PVDF-HFP as a binder, which exhibits an initial specific capacity of 181.91 mAh·g −1 at 0.13C and 25 °C. Remarkably, the wet-slurry cathode with a high NCA loading of 20 mg cm −2 delivers an initial areal capacity of 2.936 mAh·cm −2 and capacity retention of 69.93% after 1000 cycles at a rate of 0.64C. By employing X-ray diffraction, X-ray photoelectron spectroscopy, and scanning electron microscopy, we reveal that the LZO coating layer and PVDF-HFP binder inhibited the decomposition of sulfide electrolyte and detrimental structure evolution of NCA active material. This work would guide designing high-performance ASSLBs for practical application and commercialization.

研究领域: 材料科学 · 电化学 · 储能技术 · 电池技术
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JOURNAL OF ALLOYS AND COMPOUNDS · 2026 · IF 6.7

Dual-salt coupled fluoroethylene carbonate synergistically regulated PVDF-HFP/phosphated Li6.4La3Zr1.4Ta0.6O12 composite polymer electrolytes enable Li metal batteries with stable dual interface

Yiping Gu,Qi Wei,Yun Hong,Ze Ma,Zihua Wang,Tao Zhang,Xiaoyu She,Wei Lu

Composite polymer electrolytes (CPEs) based on poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)/Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) are regarded as promising electrolyte systems for developing high-energy-density solid-state lithium batteries. However, the combination of ceramic fillers and the polymer matrix often leads to poor lithium metal interface stability and limited ion transport. Here, we constructed phosphated LLZTO/PVDF-HFP CPEs synergistically regulated by a dual-salt (LiTFSI-LiBOB) and fluoroethylene carbonate (FEC). Surface phosphation of LLZTO reduces interfacial side reactions, LiBOB alleviates interfacial corrosion at the cathode/Al current collector, while FEC and dual-salt synergistically facilitate the formation of a robust SEI layer and suppress SN-induced nitrile polymerization side reactions. The electrolyte exhibits a wide electrochemical window (5.0 V), a low activation energy (0.285 eV), and an excellent Li + transference number (0.62). Besides, the assembled Li|PHL-DLi-FEC|Li cell exhibits the lifespan of over 1000 h at 0.2 mA cm −2 at both 25 °C and 60 °C. The assembled LiFePO 4 (LFP) |PHL-DLi-FEC|Li cell displays an initial capacity of 144.6 mAh g −1 , 91.9% capacity retention after 500 cycles under 0.5 C, and approaching 100% coulombic efficiency after 500 cycles at 1 C. This work offers new insights into composite polymer electrolytes with stable dual interfaces for solid-state batteries.

CAS / MDL: 114435-02-8
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ACS Applied Materials & Interfaces · 2023 · IF 9.5

PVDF-HFP/PAN/PDA@LLZTO Composite Solid Electrolyte Enabling Reinforced Safety and Outstanding Low-Temperature Performance for Quasi-Solid-State Lithium Metal Batteries

Yang Wang,Zhen Chen,Yixin Wu,Yu Li,Ziyu Yue,Minghua Chen

Lithium-ion batteries (LIBs) have achieved a triumph in the market of portable electronic devices since their commercialization in the 1990s due to their high energy density. However, safety issue originating from the flammable, volatile, and toxic organic liquid electrolytes remains a long-standing problem to be solved. Alternatively, composite solid electrolytes (CSEs) have gradually become one of the most promising candidates due to their higher safety and stable electrochemical performance. However, the uniform dispersity of ceramic filler within the polymer matrix remains to be addressed. Generally, all-solid-state lithium metal batteries without any liquid components suffer from poor interfacial contact and low ionic conductivity, which seriously affect the electrochemical performance. Here we report a CSE consisting of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), polydopamine (PDA) coated Li6.4La3Zr1.4Ta0.6O12 (LLZTO) (denoted as PDA@LLZTO) microfiller, polyacrylonitrile (PAN), and poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP). Introducing only 4 μL of liquid electrolyte at the electrode|electrolyte interface, the CSE-based cells exhibit high ionic conductivity (0.4 × 10–3 S cm–1 at 25 °C), superior cycle stability, and excellent thermal stability. Even under low temperatures, the impressive electrochemical performance (78.8% of capacity retention after 400 cycles at 1 C, 0 °C, and decent capacities delivered even at low temperature of −20 °C) highlights the potential of such quasi-solid-state lithium metal batteries as a viable solution for the next-generation high-performance lithium metal batteries.

CAS / MDL: 62-31-7 77-86-1
研究领域: 材料科学 · 能源技术
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Combining Organic Plastic Salts with a Bicontinuous Electrospun PVDF–HFP/Li7La3Zr2O12 Membrane: LiF-Rich Solid-Electrolyte Interphase Enabling Stable Solid-State Lithium Metal Batteries

Zhiqiang Fang,Ming Zhao,Yan Peng,Shiyou Guan

Solid-state electrolytes can guarantee the safe operation of high-energy density lithium metal batteries (LMBs). However, major challenges still persist with LMBs due to the use of solid electrolytes, that is, poor ionic conductivity and poor compatibility at the electrolyte/electrode interface, which reduces the operational stability of solid-state LMBs. Herein, a novel fiber-network-reinforced composite polymer electrolyte (CPE) was designed by combining an organic plastic salt (OPS) with a bicontinuous electrospun polyvinylidene fluoride-co-hexafluoropropylene (PVDF–HFP)/Li7La3Zr2O12 (LLZO) membrane. The presence of LLZO in the composite helps to promote the dissociation of FSI– from OPSs. Subsequently, the dissociated FSI– is then involved in the formation of a LiF-rich solid electrolyte interphase (SEI) layer on the lithium anode via a reductive decomposition reaction, which was affirmed by theoretical calculations and experimental results. Due to the LiF-rich SEI layer, the Li/Li symmetric cell was able to demonstrate a long cyclic life of over 2600 h at a current density of 0.1 mA cm–2. More importantly, the as-prepared CPE achieved a high ionic conductivity of 2.8 × 10–4 S cm–1 at 25 °C, and the Li/LiFePO4 cell based on the CPE exhibited a high discharge capacity and 83.3% capacity retention after 500 cycles at 1.0 C. Thus, the strategy proposed in this work can inspire the future development of highly conductive solid electrolytes and compatible interface designs toward high-energy density solid-state LMBs.

研究领域: 材料科学 · 储能 · 电化学 · 电池技术
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INDUSTRIAL CROPS AND PRODUCTS · 2023 · IF 5.9

Flexible PVDF-HFP based hybrid composite solid electrolyte membrane co-filled with hydroxypropyl methyl cellulose and Li6.4La3Zr1.4Ta0.6O12 for high-performance solid-state lithium batteries

Chao Gao,Xinping Li,Guijuan Wei,Shoujuan Wang,Xixia Zhao,Fangong Kong

Solid polymer electrolytes (SPEs) have sparked attention due to their superior mechanical robustness and excellent security in solid-state lithium batteries. However, intrinsic limitations, such as poor ionic transport properties and large interface impedance, severely hinder their practical applications. Herein, a novel composite solid electrolyte (PLHL-CSE) membrane, which consists of poly (vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP), hydroxypropyl methyl cellulose (HPMC), lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), and Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO), was prepared by solution-casting technique. The incorporation of HPMC into PVDF-HFP-based electrolyte played crucial roles in reducing the crystallinity of PVDF-HFP, promoting the dissociation of lithium salt, and increasing the amount of mobile Li + . With synergistic effects of HPMC and LLZTO, the mechanical and electrochemical performance of PVDF-HFP-based electrolytes were greatly enhanced. The obtained PLHL-CSE membrane showed better mechanical strength (3.0 MPa), enhanced ionic conductivity (0.25 mS/cm at 25 °C), greater lithium-ion transference number (0.7), and broadened electrochemical window of 5.0 V (vs. Li + /Li) than the PVDF-HFP/LiTFSI solid polymer electrolyte (PL-SPE) membrane. After 300 cycles at 1 C, the assembled LiFePO 4 /PLHL-CSE/Li cell with PLHL-CSE membrane as the hybrid composite solid electrolyte displayed a high capacity retention (95.6%). In addition, the positive effects of HPMC and LLZTO on promoting the generation of stable SEI and the uniform lithium deposition were also confirmed by the SEM results of cycled lithium metals. These findings point to the good potential of PLHL-CSE membrane as a hybrid composite solid electrolyte for practical application in lithium batteries.

CAS / MDL: 9004-65-3 872-50-4
研究领域: 材料科学 · 电化学
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ACS Applied Materials & Interfaces · 2025 · IF 8.2

Enhanced Liquid–Solid Triboelectric Nanogenerators with SiO2@Cu-Doped Composite Coating for Droplet Energy Harvesting

Yuxi Yang,Xiaojing Liang,Liang Ma,Min Chen,Limin Wu

Rainwater is a clean and abundant energy source, and the liquid–solid triboelectric nanogenerator (LS-TENG) has emerged as a promising technology for harvesting and converting raindrop energy into electricity. Despite its potential, practical applications of LS-TENG have been limited by its low output performance and complex fabrication processes. Herein, we propose a simple and efficient strategy for constructing high-performance LS-TENG by introducing a novel composite triboelectric layer composed of poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) doped with SiO2@Cu and 1H,1H,2H,2H-perfluorooctyltriethoxysilane. This design simultaneously enhances the dielectric constant and hydrophobicity of the triboelectric coating through a polarization effect and surface tuning. As a result, the LS-TENG achieves an excellent output voltage of 19 V and a current of 6.7 μA from a single waterdrop, corresponding to 2.5 and 2.8 times those of undoped PVDF-HFP, and can successfully power small electronic devices. Furthermore, the entire LS-TENG, including both the triboelectric and electrode layers, is fabricated via facile, in situ coating processes, offering good scalability, substrate adaptability, and optical transparency. Therefore, this work integrates material-level output enhancement with process-level simplicity, holding great potential for practical applications in droplet energy harvesting.

研究领域: 纳米能源 · 功能材料科学 · 微纳器件 · 可再生能源技术 · 表面工程
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Intelligent Off/On switchable electromagnetic wave absorbing material based on VO2 nanowires

Shuhui Liang,Huan Guan,Hainan Zhang,Xiangge Han,Jia Gao,Jiupeng Zhao,Shuliang Dou,Yao Li

With the development of modern communication devices, the demand for intelligent electromagnetic wave (EMW) absorbing materials that dynamically respond to environmental changes is ever-growing. However, the design and fabrication of high-performance EMW absorbing materials with adapt features remains challenging. Here, we report a temperature-responsive composite comprising VO 2 nanowires (NWs) and polyvinylidene fluoride-hexafluoropropylene copolymer (PVDF-HFP). Benefiting from the phase transition characteristics of VO 2 and the high aspect ratio of NWs, the composite demonstrates two distinct off/on switchable EMW absorbing performances as the temperature increases at low filler loading of VO 2 . The composite with 10 wt% VO 2 NWs transitions from transmission to absorption, showcasing a maximum change in reflection loss (RL) and effective absorption bandwidth (EAB) values of 53.09 dB and 4.85 GHz at the thin thickness of 2.5 mm and 2 mm, respectively. While the composite with 30 wt% VO 2 NWs shows a switch from absorption to reflection with the highest ΔEAB and ΔRL values of 3.59 GHz (1.5 mm) and 44.29 dB (2.5 mm), respectively. Additionally, radar cross-sectional (RCS) simulations verify the intelligent EMW absorbing performance of the composite. The work provides an effective and sustainable approach to harness the potential of VO 2 for developing tunable and high-performance wave-absorbing materials.

研究领域: 材料科学 · 电磁工程 · 纳米技术
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Journal of Nanomaterials · 2020 · IF 1.98

Electrospun High-Thermal-Resistant Inorganic Composite Nonwoven as Lithium-Ion Battery Separator

Yuan Xu,Jian-Wei Zhu,Jun-Bo Fang,Xiao Li,Miao Yu,Yun-Ze Long

Separators are key materials to ensure the safety of lithium-ion batteries and improve their performance. Currently, commercial lithium-ion battery separators are mainly polyolefin organic diaphragms, but their temperature instability leads to battery short circuit and fire risk. A flexible SiO2 nanofiber membrane combined with a poly(vinylidene fluoride-hexafluoropropylene) (PVDF-HFP) nanofiber membrane is prepared by an electrospinning method. The mechanical strength of the SiO2/PVDF-HFP composite nanofiber membrane (SPF) is twice as high as the pure SiO2 nanofiber membrane and at 200°C, there are almost no dimensional changes of the SPF separators. Compared to commercial polyethylene (PE) separators, SPF shows excellent thermal stability and large-area closed cells at 180°C when used in lithium-ion battery separators. The porosity of SPF is 89.7%, which is more than twice than that of an ordinary PE separator. The liquid absorption rate of SPF is much higher than an ordinary PE separator and has reached 483%. Furthermore, the cycle and rate performance of lithium-ion batteries prepared by SPF has been improved significantly. These excellent properties, as well as the potential for large-scale production of electrospinning technology, make SPF an ideal choice for high-power battery separators.

研究领域: 材料科学 · 能源存储 · 纳米技术
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Journal of Energy Chemistry · 2023 · IF 13.1

Bifunctional flame retardant solid-state electrolyte toward safe Li metal batteries

Qiang Lv,Yajie Song,Bo Wang,Shangjie Wang,Bochen Wu,Yutong Jing,Huaizheng Ren,Shengbo Yang,Lei Wang,Lihui Xiao,Dianlong Wang,Huakun Liu,Shixue Dou

Solid polymer electrolytes (SPEs) are one of the most promising alternatives to flammable liquid electrolytes for building safe Li metal batteries. Nevertheless, the poor ionic conductivity at room temperature (RT) and low resistance to Li dendrites seriously hinder the commercialization of SPEs. Herein, we design a bifunctional flame retardant SPE by combining hydroxyapatite (HAP) nanomaterials with N-methyl pyrrolidone (NMP) in the PVDF-HFP matrix. The addition of HAP generates a hydrogen bond network with the PVDF-HFP matrix and cooperates with NMP to facilitate the dissociation of LiTFSI in the PVDF-HFP matrix. Consequently, the prepared SPE demonstrates superior ionic conductivity at RT, excellent fireproof properties, and strong resistance to Li dendrites. The assembled Li symmetric cell with prepared SPE exhibits a stable cycling performance of over 1200 h at 0.2 mA cm −2 , and the solid-state LiFePO 4 ||Li cell shows excellent capacity retention of 85.3% over 600 cycles at 0.5 C.

研究领域: 材料科学 · 电化学 · 能源存储
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Materials Today Bio · 2024 · IF 8.7

Piezoelectrically-activated antibacterial catheter for prevention of urinary tract infections in an on-demand manner

Xiaofeng Duan,Yongde Xu,Zhifa Zhang,Xinbo Ma,Cui Wang,Wenjing Ma,Fan Jia,Xiaoying Pan,Yang Liu,Yantao Zhao,Qihong Li,Zhiqiang Liu,Yong Yang

Catheter-associated urinary tract infection (CAUTI) is a common clinical problem, especially during long-term catheterization, causing additional pain to patients. The development of novel antimicrobial coatings is needed to prolong the service life of catheters and reduce the incidence of CAUTIs. Herein, we designed an antimicrobial catheter coated with a piezoelectric zinc oxide nanoparticles (ZnO NPs)-incorporated polyvinylidene difluoride-hexafluoropropylene (ZnO-PVDF-HFP) membrane. ZnO-PVDF-HFP could be stably coated onto silicone catheters simply by a one-step solution film-forming method, very convenient for industrial production. In vitro , it was demonstrated that ZnO-PVDF-HFP coating could significantly inhibit bacterial growth and the formation of bacterial biofilm under ultrasound-mediated mechanical stimulation even after 4 weeks. Importantly, the on and off of antimicrobial activity as well as the strenth of antibacterial property could be controlled in an adaptive manner via ultrasound. In a rabbit model, the ZnO-PVDF-HFP-coated catheter significantly reduced the incidence CAUTIs compared with clinically-commonly used catheters under assistance of ultrasonication, and no side effect was detected. Collectively, the study provided a novel antibacterial catheter to prevent the occurrence of CAUTIs, whose antibacterial activity could be controlled in on-demand manner, adaptive to infection situation and promising in clinical application.

研究领域: 生物医学工程 · 材料科学 · 传染病学 · 纳米技术
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IONICS · 2025 · IF 2.6

Incorporating lithium salts into two-dimensional metal–organic frameworks (MOFs) to create high-performance solid-state lithium metal batteries

Yin Ning,Li Qiaoxia,Wang Fuming,Min Yulin,Xu Qunjie

Composite solid electrolytes (CSEs) combine the advantages of solid polymer electrolytes and inorganic solid electrolytes, making them promising candidates for all-solid-state lithium metal batteries. However, current CSEs exhibit deficiencies such as low ionic conductivity, lithium dendrite growth, and susceptibility to damage of the electrolyte membrane, which hinder their practical applications. Therefore, designing composite solid electrolytes with novel structures is crucial for enhancing the overall performance of batteries. In this study, PVDF-HFP was chosen as the polymer electrolyte matrix, while a network structure filled with two-dimensional MOF (UMCM-309a) served as the skeleton. The composite solid electrolyte (CSE) was prepared using a simple solution casting method, incorporating PVDF-HFP, lithium bis (trifluoromethanesulfonyl) imide (LiTFSI), and two-dimensional MOF (UMCM-309a). The developed PVDF-HFP/LiTFSI/MOF (PLM) electrolyte demonstrates remarkable ionic conductivity of 5.7 × 10 −4 S cm −1 at 60 °C, along with an extensive electrochemical stability window of 4.8 V. The Li|10% PLM CSE|LiFePO 4 cell exhibits exceptional cycling performance and longevity, maintaining 95% capacity retention after 1000 cycles of stable operation at 60 °C and a rate of 1 C. Furthermore, the Li | Li symmetric cell illustrates strong interfacial compatibility, achieving stable cycling for 1100 h at a current density of 0.1 mA cm −2 . Therefore, the PLM CSE composite provides a straightforward and effective approach for achieving high-performance lithium batteries, facilitating ultra-stable operation in solid-state lithium metal batteries. Graphical

CAS / MDL: 50446-44-1
研究领域: 材料科学 · 储能 · 电化学 · 纳米材料
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