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Materials Today Chemistry · 2023 · IF 7.3

Three-dimensional printed Li4Ti5O12@VSe2 composites as high-performance anode material in full 3D-printed lithium-ion batteries with three-dimensional -printed LiFePO4@AC/rGO cathode

J.P. Mwizerwa,K. Xu,C. Liu,N. Zhao,Y. Li,P. Ndagijimana,Z. Chen,J. Shen

Currently, the development of high-performance lithium-ion batteries (LIBs) with improved areal capacity is still challenging. The common strategy to improve areal capacity is to increase the thickness of electrode materials. However, the application of thick electrodes remains challenge due to poor mechanical properties , slow charge and ion transport, and poor electrolyte infiltration . In this study, thick electrodes are constructed by 3D printing a Li 4 Ti 5 O 12 @VSe 2 -based ink. The highly electrical conductor VSe 2 on the Li 4 Ti 5 O 12 surface improves the ion and charge transport and eases the internal resistance of the 3D-printed electrode during charge and discharge. As a result, LIBs employing these thick electrodes show a high-rate capability of 128.9 mAh/g at 10 C, improved areal capacities up to 6.2 mAh/cm 2 , and ultrastable cycling capability (84.5% of capacity retention after 1700 cycles). Moreover, full cells utilizing 3D-Li 4 Ti 5 O 12 @VSe 2 as the anode and 3D-LiFePO 4 @AC/rGO as the cathode with 1.81 V potential yield a high specific capacity of 152.5 mAh/g at 0.1C, a high specific energy density of 276.025 Wh/kg, and a power density of 30.5 W/kg at 0.1C. This work paves the way to designing thick electrodes for high-performance LIBs.

研究领域: 材料科学 · 能源技术
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Journal of Energy Storage · 2025 · IF 9.8

High gravimetric and volumetric energy densities enabled by 3D-printed thick anode

Jean Pierre Mwizerwa,Jie Li,Chen Li,Kun Xu,Pamphile Ndagijimana,Changyong Liu

Developing advanced Li-ion batteries with high areal capacity, and gravimetric and volumetric energy densities remains a challenge. This study uses additive manufacturing technology to prepare thick Li 4 Ti 5 O 12 -Li 4 SiO 4 (LTO-LSO) composite electrodes for Li-ion batteries with high area capacity and energy density. The 3D-printed electrodes are made of grid-patterned and closely stacked LTO-LSO composite, carbon black super p, and PVDF. The LSO nanoparticles are uniformly wrapped on the surface of LTO as a protective layer, resulting in increased ionic/electronic conductivity and abundant open and hierarchical macropores in the planned grid-lined 3D-printed LTO-LSO electrodes. The composite electrode has excellent conductivity (up to 4.13 × 10 2 μS cm −1 ) and low charge-transfer resistance, making it suitable for 3D-printed thick electrodes. The 3D-printed thick LTO-LSO composite electrodes (12 layers) have a high areal capacity of 6.56 mAh cm −2 , areal and volumetric energy densities of 388.04 mWh cm −2 and 241.46 mWh cm −3 , as well as excellent cycling performance at 10C after 450 cycles. Moreover, the full cell with a 3D-printed thick LTO-LSO anode and 3D-printed LiCoO 2 (LCO) cathode exhibits exceptional cycle stability, gravimetric and volumetric energy densities of 723.40 Wh kg −1 and 1200 Wh L −1 , respectively. Our strategies show that growing a highly conductive protective layer on the surface of electrodes and designing ultrathick electrodes are promising approaches to the fabrication of multidimensional structures with high area capacity, gravimetric and volumetric Li-ion batteries.

CAS / MDL: 13048-33-4 15625-89-5
研究领域: 材料科学 · 能源技术
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ELECTROCHIMICA ACTA · 2021 · IF 6.901

Mesoporous carbon rods capable of fast transport of axial electrons and radial ions for ultra-thick supercapacitor electrodes

Yongzhong Fu,Haitao Liu,Hongyu Liang,Lianshan Sun,Yongfeng Bu

Increasing the energy density ( E wt ) under large currents is always highly desired for supercapacitors using thick carbon electrodes. Herein, we report an ultra-thick carbon electrode composed of mesoporous carbon rods (MCR) with ultrahigh specific surface area. At 250 μm, it exhibits the highest capacitance ( C wt , 239 F g  −   1 at 1 A g  −   1 ) and C wt retention (53% at 100 A g  −   1 ) in EMIMBF 4 as far as we know, and ultrahigh E wt (132 Wh kg −1 ) and achievable power density ( P wt , 74 kW kg −1 ). Even at ultra-thick 600 μm, its E wt and P wt are still up to 95 Wh kg −1 and 70 kW kg −1 , respectively, with the decay of C wt at 50 A g  −   1 < 3% (much smaller than commercial carbon YP-50F). Such excellent performance is attributed to the unique MCR structure, i.e., the micron-sized rod-like frame structure consisted of interconnected carbon nanocages acting as axial electron channel, as well as the stacking pores formed by MCR serving as radial channels for ions, finally enabling electrons and ions to be rapidly transferred in the axial and radial directions, respectively. It fully demonstrates its potential application prospects in scenarios requiring high energy and high power at the same time.

研究领域: 材料科学 · 能源存储
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ELECTROCHIMICA ACTA · 2023 · IF 6.6

Electrochemical performance of lithium-ion batteries with two-layer gradient electrode architectures

Heyang Zhou,Li Ting Gao,Yimeng Li,Yuhang Lyu,Zhan-Sheng Guo

Thick electrodes whose active materials have high areal density may improve the energy densities of lithium-ion batteries. However, the weakened rate abilities and cycle lifetimes of such electrodes significantly limit their practical applications. In this study, a modified two-dimensional model was built to evaluate the influence of the electrode structure on the lithiation process. Gradient electrodes with different particle sizes along the thickness direction are designed and fabricated via a two-layer coating process . The gradient design in the thickness direction is confirmed by three-dimensional digital microscopy , energy-dispersive spectroscopy, X-ray diffraction, and scanning electron microscopy . Galvanostatic charge/discharge cycling tests and electrochemical impedance spectroscopy are performed to investigate the electrochemical properties of the fabricated gradient electrodes. The simulation results indicate that the gradient electrode structure can enhance the utilization of electrode particles on the current collector side and alleviate the nonuniformity of the solid-phase Li concentration along the thickness direction. High electrochemical performance and long-term cycling stability of the designed gradient electrodes are verified by electrochemical test. The gradient structure fabricated via multi-layer coating processes can be used to improve the electrochemical performance of thick electrodes.

CAS / MDL: 872-50-4
研究领域: 材料科学 · 电化学
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JOURNAL OF POWER SOURCES · 2025 · IF 7.9

Developing hierarchical supermacroporous wood-derived carbon structures for thick electrodes in high-energy storage devices

Jie Ouyang,Liangliang Zhou,Yuzhu Wang,Mengting Cheng,Wei Yin,Yijiao Geng,Jianhua Luo,Zhexuan Liu,Yongfeng Luo

The utilization of biomass energy, regarded as one of the most promising renewable energy sources, has emerged as current focal point in research for development of high-performance energy storage devices. Biomass-derived carbon electrodes possess the inherent porous structure of biomass, thereby endowing the electrode with abundant energy storage sites and exceptional conductivity. However, the current research on the porous structure of biomass-derived carbon primarily focuses on the development of micropores and mesopores, while neglecting the discussion on macropores and supermacroporous structures. Here, the surface of wood-derived carbon tracheids has been successfully coated with a highly structured supermacroporous layer through a straightforward filling process. The resulting supermacroporous wood-derived carbon (super-MWC-4) thick electrode preserves the micropore/mesopore structure and the wood tracheids architecture while significantly increasing its pore volume to 0.665 mL g −1 . Thanks to its unique structural features, the super-MWC-4 thick electrode exhibits excellent areal capacitance (6.4 F cm −2 ), remarkable energy density (0.48 mWh cm −2 ), superior rate performance, and long cycle stability when used in a symmetric supercapacitor configuration with another identical electrode. Our findings highlight the crucial role of macropore/supermacroporous in enhancing energy storage capabilities of thick electrodes derived from renewable biomass resources such as wood.

CAS / MDL: 497-19-8 56570-89-9
研究领域: 材料科学 · 能源技术
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ADVANCED FUNCTIONAL MATERIALS · 2021 ·Vol. 32 ·期 12 ·2108669 · IF 18.808

Low Tortuosity and Reinforced Concrete Type Ultra-Thick Electrode for Practical Lithium–Sulfur Batteries

Zhilong Han,Shuping Li,Ruoyu Xiong,Zhipeng Jiang,Mengjun Sun,Wei Hu,Linfeng Peng,Renjie He,Huamin Zhou,Chuang Yu,Shijie Cheng,Jia Xie

High-energy density and ultra-long cycling lifespan are of great significance in pursuit of practical lithium–sulfur (Li-S) batteries, in which the construction of ultrathick, high-areal-capacity, and stable-cycling sulfur cathodes remains challenging. Here, a unique layered reinforced concrete structure (LRCS) is reported by integrating an ice-template method with incorporating carbon fibers in the thick electrodes for Li-S batteries. The LRCS enables aligned through-channel structure and intertwined conductive network, which lead to both fast kinetics of ions/electrons transport and strengthened electrode integrity to tolerate the volume change during cycling and the dimensional deformation under a high compaction density. Benefiting from the unique structure, the ultra-thick Se 0.05 S 0.95 @ pPAN cathode (20.2 mg cm −2 ) delivers a high capacity of 10 mAh cm −2 and excellent capacity retention of 80.8% over 140 cycles at a low electrolyte-to-sulfur ratio of 2 and a negative-to-positive capacity ratio of 2.7, corresponding to a calculated energy density of 390 Wh kg −1 . This investigation not only provides guidance for the design of thick sulfur electrodes but also paves the way for the development of practical Li-S batteries.

CAS / MDL: 16627-68-2
研究领域: 材料科学 · 能源技术
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ADVANCED FUNCTIONAL MATERIALS · 2020 ·Vol. 30 ·期 24 ·2001484 · IF 16.836

Densified Metallic MoS2/Graphene Enabling Fast Potassium-Ion Storage with Superior Gravimetric and Volumetric Capacities

Kai Yao,Zhanwei Xu,Meng Ma,Jiayin Li,Fanyu Lu,Jianfeng Huang

The potassium-ion battery (PIB) is an attractive energy storage device that possesses the potential advantages of high energy density and low cost. Herein, a pure 1T-MoS 2 is synthesized on graphene oxide and assembled into a hydrogel. The hydrogel is further tightened to a compact 1T-MoS 2 /graphene (CTMG) bulk by a densifying strategy of capillary tension. When employed as an anode for PIBs, the CTMG electrode can store K + through reversible intercalation and conversion electrochemistry, accompanied with fast kinetics since the 1T-MoS 2 induces a pseudocapacitive storage mechanism and the extraordinary K + transportation ability. Consequently, the CTMG electrode delivers the high and reversible rate capacities of 511 and 327 mAh g -1 at 0.1 and 1 A g -1 , respectively. Moreover, the compact architecture reduces the electrode thickness by ≈33% enabling a high volumetric capacity (512 mAh cm -3 at 0.1 A g -1 after 100 cycles), as well as holding a promising application in thick electrode.

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米材料 · 电池技术
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MATERIALS LETTERS · 2025 · IF 2.7

Effect of binder modification on the performance of thick electrodes with microstructures fabricated by femtosecond laser

Tengyu Guo,Xiaowei Han,Hongshui Wang,Donghui Wang,Chunyong Liang

Lithium iron phosphate (LFP) thick electrodes have emerged as a key strategy to enhance the energy density of lithium-ion batteries. However, their practical performance is limited by sluggish ion/electron transport. While femtosecond laser-induced porous micro/nanostructures effectively mitigate transport limitations, this structuring approach often reduces mechanical cohesion and risks electrode delamination. The conventional polyvinylidene fluoride (PVDF) binder, with weak adhesion and insulating properties, worsens these issues. This study developed a multifunctional composite binder (PPC) of PVDF, polyacrylonitrile (PAN), and carboxylated multi-walled carbon nanotubes via ultrasonic dispersion. The PPC binder improves interfacial adhesion through polar nitrile interactions and establishes a conductive network, enhancing mechanical robustness and electronic conductivity. The synergistic integration of laser-structured structure and the composite binder significantly enhances electrode adhesion, rate capability, and long-term cycling stability, offering a solution to the performance–durability trade-off in thick electrodes.

CAS / MDL: 68-12-2 25014-41-9
研究领域: 电化学 · 材料科学 · 能源存储 · 纳米技术 · 表面工程 · 高分子材料
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ELECTROCHIMICA ACTA · 2019 · IF 5.383

Thick electrodes upon biomass-derivative carbon current collectors: High-areal capacity positive electrodes for aluminum-ion batteries

Ya Chen,Zhili Zhou,Na Li,Shuqiang Jiao,Haosen Chen,Wei-Li Song,Daining Fang

Rechargeable aluminum-ion batteries (AIBs) are considered as low-cost safe energy storage devices beyond lithium-ion batteries, due to the high volumetric capacity and rich abundance of aluminum . However, the highly corrosive room temperature ionic liquid electrolyte causes serious problems in the traditional metal current collectors, and electrochemical inert metals with higher density have been commonly used, which leads to dramatic decreased material utilization in the positive electrode. For addressing such issues, here a biomass-derivative carbon (BDC) current collector is demonstrated to construct millimeter-scale thick positive electrodes based on two types of graphite active materials (with different planar sizes) and two electrode configurations. The results suggest the strategy of using single-side casting process with graphite of smaller planar size would be more promising to promote the overall electrochemical properties and energy storage performance. The as-assembled thick electrode (with thickness up to ∼2 mm) using the same type of graphite is able to deliver much enlarged areal loading (36 mg cm −2 ), showing greater areal capacity for energy storage. The strategy and mechanism in this work offers a considerable approach for improving the current collectors and promoting the graphite proportion in AIBs.

CAS / MDL: 7782-42-5 872-50-4
研究领域: 能源存储 · 材料科学 · 电化学
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JOURNAL OF POWER SOURCES · 2024 · IF 8.1

Scalable thick Ni-rich layered oxide cathode design for high energy/power balanced lithium-ion battery

Danmin Cai,Meiting Gao,Sifei Luo,Xueyin Wu,Yuhan Yang,Yong Xie,Licai Zhu,Xiaolong Deng,Yajuan Ji,Zhongzhi Yuan

We have applied a scalable multilayer coating method to design three porous cathodes (90 μm thickness, areal loading ca. 25 mg cm −2 , areal capacity ca. 5.3 mAh cm −2 ) based on LiNi 0.9 Co 0.05 Mn 0.05 O 2 active materials in the form of small single-crystal (SSC) particles, large polycrystalline (LPC) secondary particles, and small polycrystalline (SPC) secondary particles. The V-type electrode facilitates Li + transport, has a high characteristic thickness (46–57 μm), long cycle life with an active material utilization of 49.67% and a capacity retention of 88.24% after 100 cycles. The A-type electrode exhibits restricted Li + transport, lower characteristic thickness (23–30 μm), fast cyclic capacity decay with an active material utilization of 26.31% and a capacity retention of 68.76% after 100 cycles. The small particles on the upper layer of the A-type electrode exhibit high-rate characteristics, exceeding 82.5% of the discharge capacity of a single-layer electrode with a uniform mixture of LPC and SSC at a 4C discharge rate. The combination of SSC and LPC particles facilitates high specific energy and cycling stability with optimum stability when stored at 60 °C under 100% state of charge (SOC). The design strategy that is proposed offers a commercial route to boosting battery energy density from 220 Wh kg −1 to above 300 Wh kg −1 .

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米技术 · 应用物理 · 化学工程 · 先进制造
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JOURNAL OF POWER SOURCES · 2022 · IF 9.794

Fabricating ultrathick, dense electrodes for compact rechargeable batteries with ultrahigh areal and volumetric capacity

Zhonggang Liu,Junlu Zhu,Dongzhen Lu,Wei Wang,Liguo Yue,Yunyong Li

Thick electrode engineering greatly enhances the areal loading of electroactive materials and gravimetric energy density of batteries , but it brings sluggish electron/ion diffusion kinetics and fluffy structure (high porosity) owing to its prolonged electronic/ionic diffusion length . Herein, we develop a general soft chemical strategy to fabricate a series of ultrathick yet dense electrodes with high conductivity, which achieves high utilization of electroactive materials, ultrahigh areal and volumetric capacities. Specifically, the ultrathick dense graphene-encapsulated Na 3 V 2 (PO 4 ) 3 electrode (loading: 120 mg cm −2 , thickness: 492 μm) and graphene-encapsulated LiFePO 4 (HD-LFP@G) electrode (loading: 152 mg cm −2 , thickness: 623 μm) achieve the utilization ratios of 73 and 90%, and the ultrahigh areal capacities of 9.3 and 21 mAh cm −2 , respectively. Importantly, the ultrathick and dense HD-LFP@G//graphene-encapsulated graphite (HD-graphite@G) full batteries also displayed a high areal capacity of 9.4 mAh cm −2 . Detailed mechanism analysis revealed that such superior electrochemical performance stems from its 3D high-conductivity and network-like graphene-encapsulated structure, which maintains good electronic/ionic diffusion kinetics and structural stability, while the dense structure endows high volumetric performance in the ultrathick dense electrodes. This work provides an universal strategy to design ultrathick, dense electrodes towards compact energy storage with high volumetric and gravimetric energy density in practical applications.

研究领域: 材料科学 · 电化学 · 能源存储
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Advanced Energy Materials · 2022 ·Vol. 13 ·期 9 ·2202939 · IF 29.698

Intermolecular Cross-Linking Reinforces Polymer Binders for Durable Alloy-Type Anode Materials of Sodium-Ion Batteries

Qian Yao,Yansong Zhu,Cheng Zheng,Nana Wang,Dongdong Wang,Fang Tian,Zhongchao Bai,Jian Yang,Yitai Qian,Shixue Dou

Sodium-ion batteries show promising potential for large-scale energy storage. However, the large size and heavy mass of Na + always results in huge volume change and inferior electrochemical stability, especially in alloy-type anode materials. Here, molecular engineering of the polymer binders, i.e., cross-linking of poly(acrylic acid) with glycerin (PAA-GLY), reinforces the mechanical properties, eliminates the active protons of PAA, and benefits electrolyte diffusion, thereby remarkably improving electrochemical performance. Using µ-Sn as an example, the cycle life at 2 A g −1 is extended from ≈26 cycles of PAA to ≈2000 cycles of PAA-GLY. Meanwhile, the initial Coulombic efficiency is promoted to 90.3%, allowing the fabrication step of electrode presodiation for full cells to be eliminated. Thus, the full cells run 300 cycles at 2 A g −1 . In addition, the binder allows the thick electrode to exhibit an areal capacity of 6.8 mAh cm −2 . This binder is also applied for µ-Bi and µ-Sb. The simple operation, remarkable improvement, and wide applications indicate the promising prospects of this strategy for advanced electrodes in sodium ion batteries.

研究领域: 材料科学 · 电化学 · 能源存储
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