Polymer Molecular Engineering Enables Rapid Electron/Ion Transport in Ultra‐Thick Electrode for High‐Energy‐Density Flexible Lithium‐Ion Battery

Zhang, Yangfan; Li, Fuzhen; Yang, Kang; Liu, Xiu; Chen, Yaoguang; Lao, Zhengqi; Mai, Kancheng; Zhang, Zishou

doi:10.1002/adfm.202100434

Cited by 37 publications

(38 citation statements)

References 49 publications

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“…(g) Cycling performance of a 45 mg cm –2 bilayer LFP electrode at the current density of 3.4 mA cm –2 . (h) Comparison of the 100 mg cm –2 bilayer LFP electrode with recently reported thick electrodes. ,,,− …”

Section: Resultsmentioning

confidence: 99%

Ultrahigh-Capacity and Scalable Architected Battery Electrodes via Tortuosity Modulation

Zhang

et al. 2021

ACS Nano

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A thick electrode with high areal capacity is a straightforward approach to maximize the energy density of batteries, but the development of thick electrodes suffers from both fabrication challenges and electron/ion transport limitations. In this work, a low-tortuosity LiFePO4 (LFP) electrode with ultrahigh loadings of active materials and a highly efficient transport network was constructed by a facile and scalable templated phase inversion method. The instant solidification of polymers during phase inversion enables the fabrication of ultrathick yet robust electrodes. The open and aligned microchannels with interconnected porous walls provide direct and short ion transport pathways, while the encapsulation of active materials in the carbon framework offers a continuous pathway for electron transport. Benefiting from the structural advantages, the ultrathick bilayer LiFePO4 electrodes (up to 1.2 mm) demonstrate marked improvements in rate performance and cycling stability under high areal loadings (up to 100 mg cm–2). Simulation and operando structural characterization also reveal fast transport kinetics. Combined with the scalable fabrication, our proposed strategy presents an effective alternative for designing practical high energy/power density electrodes at low cost.

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Section: Resultsmentioning

confidence: 99%

Ultrahigh-Capacity and Scalable Architected Battery Electrodes via Tortuosity Modulation

Zhang

et al. 2021

ACS Nano

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“…The designs of thick electrodes in silicon-based materials not merely require favorable electron-transfer kinetics, but also need to reserve an effective space to preserve the electrolyte infiltrate and accommodate the volume expansion during cycles. [20][21][22] In the last decade, the fabrication and structural designs of thick electrodes, such as laser processing, [20][21][22] slurrycasting technique, [24] layer-by-layer spray deposition, [21] electrostatic-assisted self-assembly approach, [25] suspension-casting method, [26] roll-and-cut method, [27] layer-by-layer assembly, [28] aerosol jet printing [29] and freeze-casting process [30] were widely studied. Recently, the 3D printing technology has been constantly utilized in the thick electrode design.…”

Section: Introductionmentioning

confidence: 99%

3D Printed Multilayer Graphite@SiO Structural Anode for High‐Loading Lithium‐Ion Battery

Chen

Jiang

et al. 2022

Batteries & Supercaps

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To satisfy the increasing demand for higher energy density, the fabrication and structural designs of three‐dimensional (3D) thick electrodes have received considerable attention. In this work, cheap commercial graphite (Gt) and silicon monoxide (SiO) were chosen as raw materials. We have took advantage of the multi‐layer biscuit structure feature to the 3D Gt@GS (Gt@Gt/SiO) electrode with high loading through a modified 3D printing technology. Such a unique structure can not only effectively accommodate the volume expansion in all directions, but also provide a 3D transport channel to enhance the mobility of electrons and ions in the thick electrodes. The obtained 3D Gt@GS electrode, as a freestanding material, shows high capacity and good cycling stability. Especially, the 3D Gt@GS electrode after 120 cycles has achieved a reversible capacity of 3.52 mAh cm−2 at 3.6 mA cm−2. In addition, we have successfully fabricated a 3D plane‐shaped batteries via a direct ink writing technology and a fused deposition technology. The heterotypic battery assembled can be utilized as an external power supply for the aircraft model. This work demonstrates that the structural battery combined with structural load and 3D printing technology is versatile enough to meet the demand of energy storage systems for high energy density.

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“…From various dimensions such as loading density, areal capacity, and capacity retention rate, our printed thick electrodes surpass those of other LFP/LTO‐based thick electrodes (Table S1, Supporting Information). [ 24,28,40–44 ]…”

Section: Resultsmentioning

confidence: 99%

“…From various dimensions such as loading density, areal capacity, and capacity retention rate, our printed thick electrodes surpass those of other LFP/LTO-based thick electrodes (Table S1, Supporting Information). [24,28,[40][41][42][43][44] Since thick vertical channel LFP/CNT/CNF cathode and LTO/CNT/CNF anode exhibit approximate capacities of 153.8 and 168.5 mAh g −1 at 0.2 C, LFP/LTO full cells are assembled with two identical layered cathode and anode, and their electrochemical performance are studied under different loading densities and deformation conditions. The electrochemical performance of full cells assembled with different layered cathode and anode are tested and the corresponding results are listed in Table 1.…”

Section: Resultsmentioning

confidence: 99%

“…proposed a kind of copolymer ethylene vinyl acetate (EVA) to provide flexible supports and ion channels for ultrathick flexible LIBs. [ 24 ] It turns out that the specific capacity is maintained with the increased electrode thickness. However, the kinetic acceleration of the ion transfer provided by EVA under high loading and fast charge/discharge is gradually becoming inadequate.…”

Section: Introductionmentioning

confidence: 99%

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Directional Freezing Assisted 3D Printing to Solve a Flexible Battery Dilemma: Ultrahigh Energy/Power Density and Uncompromised Mechanical Compliance

Ling

Zeng

et al. 2022

Advanced Energy Materials

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Flexible lithium‐ion batteries (LIBs) have been in the spotlight with the booming development of flexible/wearable electronics. However, the dilemma of simultaneously balancing excellent energy density with mechanical compliance in flexible electrodes impedes their practical applications. Here, for the first time, a directional freezing assisted 3D printing strategy is proposed to construct flexible, compressible, and ultrahigh energy/power density LIBs. Cellulose nanofibers (CNFs) and carbon nanotubes (CNTs) are entangled with each other to form an interwoven network and uniformly wrap the active materials, ensuring fast electron transfer and stress release through the entire printed electrode. Furthermore, vertical channels induced by directional freezing can act as high‐speed ion diffusion paths, which effectively solve the sluggish ion transport limitation of flexible 3D printed electrodes as the mass loading increases. As expected, the 3D printed LIB delivers a record‐high energy density (15.2 mWh cm–2) and power density (75.9 mW cm–2), outperforming all previously reported flexible LIBs. Meanwhile, the printed flexible full LIBs maintains favorable electrochemical stability in both bending and compression states. This work suggests a feasible avenue for the design of LIBs that resolves the long‐standing issue of high electrochemical performance and mechanical deformation in wearable and smart electronics.

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Polymer Molecular Engineering Enables Rapid Electron/Ion Transport in Ultra‐Thick Electrode for High‐Energy‐Density Flexible Lithium‐Ion Battery

Cited by 37 publications

References 49 publications

Ultrahigh-Capacity and Scalable Architected Battery Electrodes via Tortuosity Modulation

Ultrahigh-Capacity and Scalable Architected Battery Electrodes via Tortuosity Modulation

3D Printed Multilayer Graphite@SiO Structural Anode for High‐Loading Lithium‐Ion Battery

Directional Freezing Assisted 3D Printing to Solve a Flexible Battery Dilemma: Ultrahigh Energy/Power Density and Uncompromised Mechanical Compliance

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