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Keywords = binder-free electrodes

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17 pages, 3422 KB  
Article
Binder-Free Spinel Co2CuO4 Nanosheet Electrodes with Cu-Driven Kinetic Enhancement for Alkaline OER Applications
by Abu Talha Aqueel Ahmed, Momin M. Mujtaba, Abu Saad Ansari and Sangeun Cho
Materials 2026, 19(2), 301; https://doi.org/10.3390/ma19020301 - 12 Jan 2026
Viewed by 157
Abstract
Developing electrocatalysts that are efficient and durable for the oxygen evolution reaction (OER) is essential for improving the energy efficiency of alkaline water splitting. Spinel-type transition-metal oxides have emerged as promising non-noble alternatives; however, their catalytic performance is often limited by sluggish charge [...] Read more.
Developing electrocatalysts that are efficient and durable for the oxygen evolution reaction (OER) is essential for improving the energy efficiency of alkaline water splitting. Spinel-type transition-metal oxides have emerged as promising non-noble alternatives; however, their catalytic performance is often limited by sluggish charge transport and insufficient utilization of active sites. Herein, we present a systematic comparative study of electrodeposited Co3O4 (CO-300) and Cu-substituted Co2CuO4 (CCO-300) nanosheet films directly grown on Ni foam. Structural, morphological, and spectroscopic analyses reveal that Cu2+ integration into Co-oxide spinel lattice modifies the local electronic environment and produces a more open and interconnected nanosheet architecture, thereby enhancing conductivity and increasing the density of accessible redox-active sites. As a result, the optimized CCO-300 exhibits superior catalytic performance at higher current densities, along with a smaller Tafel slope (44 mV dec–1), a larger electrochemically active surface area (ECSA), and reduced charge-transfer resistance compared to CCO-300, indicating accelerated reaction kinetics and improved electron-ion transport. Furthermore, the multistep chronopotentiometry measurements and long-term stability tests over 100 h at current densities of 10 and 250 mA cm–2 highlight the excellent operational stability of the CCO-300 catalyst. Full article
(This article belongs to the Section Energy Materials)
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14 pages, 11633 KB  
Article
Molybdenum Nitride and Oxide Layers Grown on Mo Foil for Supercapacitors
by Dong Hyun Lim and Young-Il Kim
Materials 2025, 18(24), 5649; https://doi.org/10.3390/ma18245649 - 16 Dec 2025
Viewed by 389
Abstract
In this study, thin molybdenum nitride (MoNx) layers were directly synthesized on molybdenum foil via thermal treatment under an NH3 atmosphere, and their phase evolution, structural characteristics, and electrochemical performance were investigated. The thickness and morphology of the MoNx [...] Read more.
In this study, thin molybdenum nitride (MoNx) layers were directly synthesized on molybdenum foil via thermal treatment under an NH3 atmosphere, and their phase evolution, structural characteristics, and electrochemical performance were investigated. The thickness and morphology of the MoNx layers were controlled by varying ammonolysis time and temperature, while subsequent annealing in N2 converted the nitride layer into MoO2. Meanwhile, oxidation in air yielded crystalline MoO3 layers. X-ray diffraction and X-ray photoelectron spectroscopy confirmed progressive oxidation of molybdenum, with Mo 3d binding energies increasing in the sequence of Mo < MoNx < MoO2 < MoO3, consistent with their nominal oxidation states. Electrochemical characterization revealed that both MoNx/Mo and MoO2/Mo electrodes exhibit notable pseudocapacitive behavior in 0.5 M H2SO4 electrolyte, with areal specific capacitances reaching up to 520 mF cm−2 at 10 mV s−1. Increasing layer thickness led to enhanced capacitance, likely due to an increase in the electrochemically accessible surface area and the extension of ion diffusion pathways. MoO2-coated samples showed stronger faradaic contribution and superior rate capability compared to MoNx counterparts, along with a gradual shift from predominantly electric double-layer capacitance toward hybrid pseudocapacitive charge storage mechanisms. Full article
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10 pages, 2311 KB  
Article
CVD-Grown Carbon Nanofibers on Knitted Carbon Fabric for Enhanced Supercapacitor Performance
by Xiaojing Jia, Jiangsan Wang and Jing Dang
Crystals 2025, 15(12), 1049; https://doi.org/10.3390/cryst15121049 - 11 Dec 2025
Viewed by 345
Abstract
The escalating demand for high-performance energy storage devices has driven extensive research into flexible electrode materials for supercapacitors. Integrating structured carbon nanomaterials with flexible substrates to construct binder-free electrode architectures represents a promising strategy for improving supercapacitor capacitance and rate capability. However, achieving [...] Read more.
The escalating demand for high-performance energy storage devices has driven extensive research into flexible electrode materials for supercapacitors. Integrating structured carbon nanomaterials with flexible substrates to construct binder-free electrode architectures represents a promising strategy for improving supercapacitor capacitance and rate capability. However, achieving stable, binder-free integration of structure-controlled nanostructured carbon materials with flexible substrates remains a critical challenge. In this study, we report a direct synthesis approach for one-dimensional (1D) carbon nanofibers (CNFs) on commercial flexible carbon fabric (CF) via chemical vapor deposition (CVD). The resulting CNFs exhibit two typical average diameters—approximately 25 nm and 50 nm—depending on the growth temperature, with both displaying highly graphitized structures. Electrochemical characterization of the CNFs/CF composites in 1 M H2SO4 electrolyte revealed typical electric double-layer capacitor (EDLC) behavior. Notably, the 25 nm-CNFs/CF electrode achieves a high specific capacitance of 87.5 F/g, significantly outperforming the 50 nm-CNFs/CF electrode, which reaches 50.2 F/g. Compared with previously reported carbon nanotube CNTs/CF electrodes, the 25 nm-CNFs/CF electrode exhibits superior capacitance and lower resistance. Full article
(This article belongs to the Special Issue Advanced Catalytic Materials in Energy and Environment)
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3 pages, 1051 KB  
Correction
Correction: Moniruzzaman et al. Two-Dimensional Core-Shell Structure of Cobalt-Doped@MnO2 Nanosheets Grown on Nickel Foam as a Binder-Free Battery-Type Electrode for Supercapacitor Application. Nanomaterials 2022, 12, 3187
by Md Moniruzzaman, Yedluri Anil Kumar, Mohan Reddy Pallavolu, Hammad Mueen Arbi, Salem Alzahmi and Ihab M. Obaidat
Nanomaterials 2025, 15(23), 1784; https://doi.org/10.3390/nano15231784 - 27 Nov 2025
Viewed by 231
Abstract
In the published paper [...] Full article
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15 pages, 2807 KB  
Article
One-Step Electrospun LTO Anode for Flexible Li-Ion Batteries
by Edi Edna Mados, Roni Amit, Noy Kluska, Diana Golodnitsky and Amit Sitt
Batteries 2025, 11(11), 405; https://doi.org/10.3390/batteries11110405 - 4 Nov 2025
Viewed by 786
Abstract
Fiber-based and fabric batteries signify a groundbreaking development in energy storage, allowing for the straightforward incorporation of power sources into wearable fabrics, intelligent apparel, and adaptable electronics. In this study, we introduce a novel strategy for one-step fabrication of a flexible lithium titanate [...] Read more.
Fiber-based and fabric batteries signify a groundbreaking development in energy storage, allowing for the straightforward incorporation of power sources into wearable fabrics, intelligent apparel, and adaptable electronics. In this study, we introduce a novel strategy for one-step fabrication of a flexible lithium titanate oxide (Li4Ti5O12, LTO) anode directly on a copper current collector via electrospinning, eliminating the need for high-temperature post-processing. Based on our previous work with electrospun nanofiber cathodes and carbon-based current collector, we prepared the LTO electrode using polyethylene oxide (PEO) as a binder and carbon additives to enhance mechanical integrity and conductivity. LTO fiber mats detached from the current collector were found to endure multiple instances of bending, twisting, and folding without any structural damage. LTO/Li cells incorporating electrospun fiber LTO electrodes with 72 wt% active material loading deliver a high capacity of 170 mAh g−1 at 0.05 C. In addition, they demonstrate excellent cycling stability with a capacity loss of only 0.01% per cycle over 200 cycles and maintain a capacity of 160 mAh g−1 at 0.1 C. The scalability of the heat-treatment-free method for fabricating flexible LTO anodes, together with the improved mechanical durability and electrochemical performance, offers a promising route toward the development of next-generation flexible and wearable energy storage devices. Full article
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15 pages, 2241 KB  
Article
Vertically Aligned Carbon Nanotubes Grown on Copper Foil as Electrodes for Electrochemical Double Layer Capacitors
by Chinaza E. Nwanno, Ram Chandra Gotame, John Watt, Winson Kuo and Wenzhi Li
Nanomaterials 2025, 15(19), 1506; https://doi.org/10.3390/nano15191506 - 1 Oct 2025
Cited by 1 | Viewed by 1277
Abstract
This study reports a binder-free, catalyst-free method for fabricating vertically aligned carbon nanotubes (VACNTs) directly on copper (Cu) foil using plasma-enhanced chemical vapor deposition (PECVD) for electrochemical double-layer capacitor (EDLC) applications. This approach eliminates the need for catalyst layers, polymeric binders, or substrate [...] Read more.
This study reports a binder-free, catalyst-free method for fabricating vertically aligned carbon nanotubes (VACNTs) directly on copper (Cu) foil using plasma-enhanced chemical vapor deposition (PECVD) for electrochemical double-layer capacitor (EDLC) applications. This approach eliminates the need for catalyst layers, polymeric binders, or substrate pre-treatments, simplifying electrode design and enhancing electrical integration. The resulting VACNTs form a dense, uniform, and porous array with strong adhesion to the Cu substrate, minimizing contact resistance and improving conductivity. Electrochemical analysis shows gravimetric specific capacitance (Cgrav) and areal specific capacitance (Careal) of 8 F g−1 and 3.5 mF cm−2 at a scan rate of 5 mV/s, with low equivalent series resistance (3.70 Ω) and charge transfer resistance (0.48 Ω), enabling efficient electron transport and rapid ion diffusion. The electrode demonstrates excellent rate capability and retains 92% of its initial specific capacitance after 3000 charge–discharge cycles, indicating strong cycling stability. These results demonstrate the potential of directly grown VACNT-based electrodes for high-performance EDLCs, particularly in applications requiring rapid charge–discharge cycles and sustained energy delivery. Full article
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11 pages, 2071 KB  
Article
Composite Electroforming of a Binder-Free Porous Ni/S-PTh Electrode for Li–S Batteries by Combining 3D Printing, Pulse Plating, and Composite Electrodeposition
by Wassima El Mofid, Robin Arnet, Oliver Kesten and Timo Sörgel
Batteries 2025, 11(9), 343; https://doi.org/10.3390/batteries11090343 - 19 Sep 2025
Viewed by 1728
Abstract
A novel process for the synthesis of binder-free, porous nickel/polythiophene-functionalized sulfur (Ni/S-PTh) composite cathodes for lithium–sulfur (Li–S) batteries is introduced in this paper. Initially, a polyvinyl butyl polymer scaffold is 3D printed, then coated with a graphite-based conducting layer, and, finally, it is [...] Read more.
A novel process for the synthesis of binder-free, porous nickel/polythiophene-functionalized sulfur (Ni/S-PTh) composite cathodes for lithium–sulfur (Li–S) batteries is introduced in this paper. Initially, a polyvinyl butyl polymer scaffold is 3D printed, then coated with a graphite-based conducting layer, and, finally, it is pulse-plated for nickel deposition to produce a high-surface-area, mechanically stable current collector. S-PTh particles are afterwards co-deposited into the Ni matrix through composite electrodeposition. After the dissolution of the polymer template, the resulting self-standing electrodes still maintain porous structure with uniform sulfur distribution and a distinct transition between the dense Ni layer and the Ni/S-PTh composite layer. Electrochemical characterization of the Ni/S-PTh composite cathodes by galvanostatic cycling at C/10 rate results in an initial specific discharge capacity of ~1120 mAh·g−1 and a specific capacity of ~910 mAh·g−1 after 200 cycles, resulting in a high capacity retention of ~81 %. For our novel approach, no steps at high temperatures or toxic solvents are involved and the need for polymer binders and conductive additives is avoided. These results demonstrate the potential of composite electrodeposition in combination with 3D printing for producing sustainable, high-performance sulfur cathodes with tunable architecture. Full article
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15 pages, 6893 KB  
Article
One-Step LCVD Fabrication of Binder-Free Porous Graphene@SiC Heterostructures for Lithium-Ion Battery Anodes
by Song Zhang, Feiyang Ji, Wei Huang, Chitengfei Zhang, Chongjie Wang, Cuicui Li, Qingfang Xu and Rong Tu
Materials 2025, 18(18), 4341; https://doi.org/10.3390/ma18184341 - 17 Sep 2025
Viewed by 822
Abstract
The potential of silicon carbide (SiC) as a promising high-capacity and stable anode material is hindered by poor electronic conductivity and slow lithium diffusion kinetics. Here, we report a one-step laser chemical vapor deposition (LCVD) process to directly synthesize porous graphene@SiC heterostructures on [...] Read more.
The potential of silicon carbide (SiC) as a promising high-capacity and stable anode material is hindered by poor electronic conductivity and slow lithium diffusion kinetics. Here, we report a one-step laser chemical vapor deposition (LCVD) process to directly synthesize porous graphene@SiC heterostructures on carbon fiber substrates. This in situ method yields an integral, binder-free electrode architecture that enhances mechanical robustness against pulverization. A critical feature of this heterostructure is the built-in electric field at the graphene–SiC interface, which is revealed by theoretical calculations to significantly accelerate charge transport and lithium-ion diffusion. The resulting anode delivers a high reversible capacity of 668 mAh·g−1 after 100 cycles at 0.1 A·g−1. More remarkably, a unique multi-stage activation mechanism is discovered, leading to an unprecedented capacity rebound to 735 mAh·g−1 after cycling at rates up to 5 A·g−1. This activation process is observed to accelerate with increasing current density in the 0.1–2 A·g−1 range. Furthermore, post-cycling analysis via XRD, TEM, and XPS confirms both the structural durability of the electrode and a reversible lithium intercalation mechanism, providing a critical foundation for the future design of high-performance LIB anodes. Full article
(This article belongs to the Section Electronic Materials)
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16 pages, 2240 KB  
Article
Defect-Engineered MnO2@Ni Foam Electrode for Zinc-Ion Batteries Toward Mobile Robotics Applications
by Shilin Li, Dong Xie, Taoyun Zhou, Qiaomei Zhao, Muzhou Liu and Xinyu Li
Nanomaterials 2025, 15(17), 1312; https://doi.org/10.3390/nano15171312 - 26 Aug 2025
Viewed by 1168
Abstract
Aqueous zinc-ion batteries (AZIBs) have gained significant attention as promising candidates for next-generation energy storage systems, especially in mobile robotics, due to their inherent safety, environmental friendliness, and low cost. However, the practical application of AZIBs is often hindered by slow Zn2+ [...] Read more.
Aqueous zinc-ion batteries (AZIBs) have gained significant attention as promising candidates for next-generation energy storage systems, especially in mobile robotics, due to their inherent safety, environmental friendliness, and low cost. However, the practical application of AZIBs is often hindered by slow Zn2+ diffusion and the poor structural stability of the cathode materials under high-rate or long-term operation. To address these challenges, a defect-engineered, binder-free MnO2 electrode, with a MnO2 loading of 1.35 mg·cm−2, is synthesized via in situ hydrothermal growth of ultrathin MnO2 nanosheets directly on a 3D conductive nickel foam scaffold, followed by reductive annealing to introduce abundant oxygen vacancies. These oxygen-rich defect sites significantly enhance Zn2+ adsorption, improve charge transfer kinetics, and contribute to enhanced pseudocapacitive behavior, further improving overall electrochemical performance. The intimate contact between the MnO2 and Ni substrate ensures efficient electron transport and robust structural integrity during repeated cycling. With this synergistic architecture, the MnO2@Ni electrode achieves a high specific capacity of 122.9 mAh·g−1 at 1 A·g−1, demonstrating excellent cycling durability with 94.24% capacity retention after 800 cycles and nearly 99% coulombic efficiency. This study offers a scalable strategy for designing high-performance, structurally stable Zn-ion battery cathodes with improved rate capability, making it a promising candidate for energy-intensive mobile robotic and flexible electronic systems. Full article
(This article belongs to the Special Issue Novel Electrode Materials for Solid-State Batteries)
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16 pages, 3716 KB  
Article
Binder-Free Fe2O3/MWCNT/Al Electrodes for Supercapacitors
by Alena A. Mitina, Evgene E. Yakimov, Maxim A. Knyazev, Victor I. Korotitsky and Arkady N. Redkin
Nanomaterials 2025, 15(16), 1222; https://doi.org/10.3390/nano15161222 - 10 Aug 2025
Viewed by 1244
Abstract
This work presents a method for preparing an Fe2O3/MWCNT/Al composite electrode without the use of a binder. Synthesizing the composite material directly on conductive substrates allows one to obtain ready-made supercapacitor electrodes characterized by high values of specific capacity, [...] Read more.
This work presents a method for preparing an Fe2O3/MWCNT/Al composite electrode without the use of a binder. Synthesizing the composite material directly on conductive substrates allows one to obtain ready-made supercapacitor electrodes characterized by high values of specific capacity, as well as resistance to numerous charge/discharge cycles. Using an array of multi-walled carbon nanotubes (MWCNTs) as a conductive base for the synthesis of iron oxide allows for the production of a composite material that combines the positive properties of both materials. The Fe2O3/MWCNT/Al composite was formed using electrochemical oxidation of the MWCNT/Al material in a mixture of 0.1 M aqueous solution of Fe(NH4)2(SO4)2 (iron ammonium sulfate) and 0.08 M CH3COONa (sodium acetate) in a 1:1 ratio. The proposed approaches to fabricating composite electrodes provide excellent performance characteristics, namely high cyclic stability and fast response time. For the first time, an Fe2O3/MWCNT/Al composite was obtained using electrochemical oxidation of Fe2+ on the surface of MWCNTs grown directly on aluminum foil. The specific capacitance of the obtained composite material reaches 175 F/g at a scanning rate of 100 mV/s. The capacity loss during cyclic measurements does not exceed 25% after 10,000 charge/discharge cycles. Full article
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21 pages, 5680 KB  
Article
Polyvinylpyrrolidone-Functionalized NiCo2O4 Electrodes for Advanced Asymmetric Supercapacitor Application
by Rutuja U. Amate, Mrunal K. Bhosale, Pritam J. Morankar, Aviraj M. Teli and Chan-Wook Jeon
Polymers 2025, 17(13), 1802; https://doi.org/10.3390/polym17131802 - 28 Jun 2025
Cited by 3 | Viewed by 1132
Abstract
Designing advanced electrode architectures with tailored morphology and redox synergy is essential for achieving high-performance supercapacitive energy storage. In this study, a PVP-assisted hydrothermal approach was employed to synthesize binder-free NiCo2O4 nanostructured electrodes directly on nickel foam substrates. By modulating [...] Read more.
Designing advanced electrode architectures with tailored morphology and redox synergy is essential for achieving high-performance supercapacitive energy storage. In this study, a PVP-assisted hydrothermal approach was employed to synthesize binder-free NiCo2O4 nanostructured electrodes directly on nickel foam substrates. By modulating the PVP concentration (0.5–2 wt%), hierarchical flower-like nanosheets were engineered, with the NiCo-P1 sample (1 wt% PVP) exhibiting an optimized structure, superior electroactive surface area, and enhanced ion accessibility. Comprehensive electrochemical analysis revealed that NiCo-P1 delivered an outstanding areal capacitance of 36.5 F/cm2 at 10 mA/cm2, along with excellent cycling stability over 15,000 cycles with 80.97% retention. Kinetic studies confirmed dominant diffusion-controlled redox behavior with high OH diffusion coefficients and minimal polarization. An asymmetric pouch-type supercapacitor device (NiCo-P1//AC) exhibited a wide operating window of 1.5 V, achieving a remarkable areal capacitance of 187 mF/cm2, energy density of 0.058 mWh/cm2, and capacitive retention of 78.78% after 5000 cycles. The superior performance is attributed to the synergistic integration of mixed-valence Ni and Co species, engineered nanosheet morphology, and low interfacial resistance. This work underscores the significance of surfactant-directed design in advancing cost-effective, high-performance electrodes for next-generation flexible energy storage technologies. Full article
(This article belongs to the Section Polymer Applications)
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15 pages, 11303 KB  
Article
Hierarchical Manganese-Doped Nickel–Cobalt Oxide Electrodes with Graphene for Use as High-Energy-Density Supercapacitors
by Kuan-Ching Lee, Guan-Ting Pan, Thomas Chung-Kuang Yang, Po-Cheng Shen, Kuan Lun Pan, Timm Joyce Tiong, Aleksandar N. Nikoloski and Chao-Ming Huang
Surfaces 2025, 8(3), 43; https://doi.org/10.3390/surfaces8030043 - 25 Jun 2025
Viewed by 1156
Abstract
Thin films of manganese–nickel–cobalt oxide with graphene (G@MNCO) were deposited on copper foam using electrochemical deposition. NiCo2O4 is the main phase in these films. As the proportion of graphene in the precursor solution increases, the oxygen vacancies in the samples [...] Read more.
Thin films of manganese–nickel–cobalt oxide with graphene (G@MNCO) were deposited on copper foam using electrochemical deposition. NiCo2O4 is the main phase in these films. As the proportion of graphene in the precursor solution increases, the oxygen vacancies in the samples also increase. The microstructure of these samples evolves into hierarchical vertical flake structures. Cyclic voltammetry measurements conducted within the potential range of 0–1.2 V reveal that the electrode with the highest graphene content achieves the highest specific capacitance, approximately 475 F/g. Furthermore, it exhibits excellent cycling durability, maintaining 95.0% of its initial capacitance after 10,000 cycles. The superior electrochemical performance of the graphene-enhanced, manganese-doped nickel–cobalt oxide electrode is attributed to the synergistic contributions of the hierarchical G@MNCO structure, the three-dimensional Cu foam current collector, and the binder-free fabrication process. These features promote quicker electrolyte ion diffusion into the electrode material and ensure robust adhesion of the active materials to the current collector. Full article
(This article belongs to the Special Issue Surface Science in Electrochemical Energy Storage)
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13 pages, 2207 KB  
Article
Electrostatic Dual-Layer Solvent-Free Cathodes for High-Performance Lithium-Ion Batteries
by Haojin Guo, Chengrui Zhang, Yujie Ma, Ning Liu and Zhifeng Wang
Energies 2025, 18(12), 3112; https://doi.org/10.3390/en18123112 - 12 Jun 2025
Cited by 1 | Viewed by 1690
Abstract
Slurry-cast (SLC) electrode manufacturing faces problems such as thickness limitation and material stratification, which are caused by applying toxic organic solvents. Solvent-free electrode technology, as a sustainable alternative, could get rid of issues generated by solvents. In this study, dual-layer NCM811 solvent-free electrodes [...] Read more.
Slurry-cast (SLC) electrode manufacturing faces problems such as thickness limitation and material stratification, which are caused by applying toxic organic solvents. Solvent-free electrode technology, as a sustainable alternative, could get rid of issues generated by solvents. In this study, dual-layer NCM811 solvent-free electrodes (DLEs) are fabricated via an electrostatic powder deposition method with an active material-rich upper layer to provide high energy output, while the more binder–conductor content base layer improves conductivity and contact with current collectors. The dual-layered structure overwhelms the single-layer electrode (SE) with stable cycling performance caused by more regulated pore structures. DLE maintains 74% capacity retention after 100 cycles at 0.3 C, while the SLC shows only 60% capacity retention. Additionally, DLE shows excellent rate performance at various rates, with 207.3 mAh g−1, 193.9 mAh g−1, 173.9 mAh g−1, 157.3 mAh g−1, and 120.4 mAh g−1 at 0.1 C, 0.2 C, 0.5 C, 1.0 C, and 2.0 C, respectively. The well-designed DLE cathodes exhibit superior discharge-specific capacities, rate performance, and improved cycling stability than traditional SLC cathodes. It enlightens the path toward new structure innovations of solvent-free electrodes. Full article
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12 pages, 2936 KB  
Article
Binder-Free Metal–Organic Framework-Derived Zn(CN)2/V2O3/Carbon Cathode Fabricated via Electrophoretic Deposition for High-Performance Zn-Ion Batteries
by Hyemin Lee and Byoungnam Park
Inorganics 2025, 13(6), 194; https://doi.org/10.3390/inorganics13060194 - 11 Jun 2025
Viewed by 1376
Abstract
In this study, a Zn(CN)2–V2O3–C composite cathode was synthesized via AC electrophoretic deposition (EPD) and evaluated for application in aqueous zinc-ion batteries (ZIBs). Here, we report for the first time a binder-free Zn(CN)2–V2O [...] Read more.
In this study, a Zn(CN)2–V2O3–C composite cathode was synthesized via AC electrophoretic deposition (EPD) and evaluated for application in aqueous zinc-ion batteries (ZIBs). Here, we report for the first time a binder-free Zn(CN)2–V2O3–C composite cathode, using AC-EPD to create an ultrathin architecture optimized for probing the electrode–electrolyte interface without interference from additives or bulk effects. The composite combines Zn(CN)2 for structural support, V2O3 as the redox-active material, and carbon for improved conductivity. X-ray diffraction confirmed the presence of Zn(CN)2 and V2O3 phases, while scanning electron microscopy revealed a uniform, ultrathin film morphology. Electrochemical analysis demonstrated a hybrid charge storage mechanism with a b-value of 0.64, indicating both capacitive and diffusion-controlled contributions. The electrode delivered a high specific capacity (~250 mAh/g at 500 mA/g) with stable cycling performance. These results highlight the potential of metal–organic framework-derived composites for high-performance ZIB cathodes. The composite is especially effective when prepared via AC-EPD, which yields ultrathin, uniform films with strong adhesion and low agglomeration. This enhances energy storage performance and provides a reliable platform for focusing on interfacial charge storage, excluding the effect of binders on electrochemical performance. Full article
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16 pages, 4986 KB  
Article
Performance of 3D Network-Structured LiFePO4@Li3V2(PO4)3/Carbon Nanofibers via Coaxial Electrospinning as Self-Supporting Cathode for Lithium-Ion Batteries
by Ruixia Chu, Hongtao Zhang, Wanyou Huang, Fangyuan Qiu, Yan Wang, Zhenyu Li and Xiaoyue Jin
Materials 2025, 18(9), 1969; https://doi.org/10.3390/ma18091969 - 26 Apr 2025
Cited by 1 | Viewed by 1278
Abstract
Lithium-ion batteries (LIBs) with high power, high capacity, and support for fast charging are increasingly favored by consumers. As a commercial electrode material for power batteries, LiFePO4 was limited from further wide application due to its low conductivity and lithium-ion diffusion rate. [...] Read more.
Lithium-ion batteries (LIBs) with high power, high capacity, and support for fast charging are increasingly favored by consumers. As a commercial electrode material for power batteries, LiFePO4 was limited from further wide application due to its low conductivity and lithium-ion diffusion rate. The development of advanced architectures integrating rational conductive networks with optimized ion transport pathways represents a critical frontier in optimizing the performance of cathode materials. In this paper, a novel self-supporting cathode material (designated as LFP@LVP-CES) was synthesized through an integrated coaxial electrospinning and controlled pyrolysis strategy. This methodology directly converts LiFePO4, Li3V2(PO4)3, and polyacrylonitrile (PAN)) into flexible, binder-free cathodes with a hierarchical structural organization. The 3D carbon nanofiber (CNF) matrix synergistically integrates LiFePO4 (Li/Fe/POx) and Li3V2(PO4)3 (Li/V/POx) nanoparticles, where CNFs act as a conductive scaffold to enhance electron transport, while the POx polyanionic frameworks stabilize Li+ diffusion pathways. Morphological characterizations (SEM and TEM) revealed a 3D cross-connected carbon nanofiber matrix (diameter: 250 ± 50 nm) uniformly embedded with active material particles. Electrochemical evaluations demonstrated that the LFP@LVP-CES cathode delivers an initial specific capacity of 165 mAh·g−1 at 0.1 C, maintaining 80 mAh·g−1 at 5 C. Notably, the material exhibited exceptional rate capability and cycling stability, demonstrating a 96% capacity recovery after high-rate cycling upon returning to 0.1 C, along with 97% capacity retention over 200 cycles at 1 C. Detailed kinetic analysis through EIS revealed significantly reduced Rct and increased Li+ diffusion. This superior electrochemical performance can be attributed to the synergistic effects between the 3D conductive network architecture and dual active materials. Compared with traditional coating processes and high-temperature calcination, the preparation of controllable electrospinning and low-temperature pyrolysis to some extent avoid the introduction of harmful substances and reduce raw material consumption and carbon emissions. This original integration strategy establishes a paradigm for designing freestanding electrode architectures through 3D structural design combined with a bimodal active material, providing critical insights for next-generation energy storage systems. Full article
(This article belongs to the Section Advanced Nanomaterials and Nanotechnology)
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