Citation: Haotian Yang, Jinke Shen, Nan Qin, Yaoxin Du, Yuhan An, Chen Hu, Yifan Li, Wenlong Cai, Cunman Zhang, Zonghai Chen, Jim P. Zheng, Liming Jin. Tailoring layer-by-layer gradient porous ultra-thick electrodes via solvent-free processing method for high-areal-capacity and high-rate lithium-ion batteries[J]. Chinese Chemical Letters, ;2026, 37(7): 111833. doi: 10.1016/j.cclet.2025.111833 shu

Tailoring layer-by-layer gradient porous ultra-thick electrodes via solvent-free processing method for high-areal-capacity and high-rate lithium-ion batteries

Haotian Yang ^a ,
Jinke Shen ^a ,
Nan Qin ^a ,
Yaoxin Du ^a ,
Yuhan An ^b ,
Chen Hu ^c ,
Yifan Li ^a ,
Wenlong Cai ^d ,
Cunman Zhang ^a ,
Zonghai Chen ^e ,
Jim P. Zheng ^f ,
Liming Jin ^{a, *,}

a.
Clean Energy Automotive Engineering Center and School of Automotive Studies, Tongji University, Shanghai 201804, China
b.
College of Transportation Engineering, Tongji University, Shanghai 201804, China
c.
School of Materials Science and Engineering, Tongji University, Shanghai 201804, China
d.
Department of Advanced Energy Materials, College of Materials Science and Engineering, Sichuan University, Chengdu 610064, China
e.
Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL 60439, United States
f.
Department of Electrical Engineering, University at Buffalo, The State University of New York, Buffalo, NY 14260, United States

limingjin@tongji.edu.cn

Received Date: 20 July 2025
Revised Date: 3 September 2025
Accepted Date: 11 September 2025
Available Online: 12 September 2025

Figures(5)

Ultra-thick electrodes (UTEs) hold great promise for high-energy-density lithium-ion batteries (LIBs), yet the practical application is hindered by challenges in precise fabrication and reaction kinetics modification. In this contribution, a solvent-free processing method is introduced to tailor UTEs through layer-by-layer fabrication with positive, uniform, and negative gradient porosity from the separator side to the current collector side, denoted as P-UTEs, U-UTEs, and N-UTEs. In contrast to conventional slurry coating, the proposed solvent-free approach effectively circumvents capillary stress, thereby facilitating the fabrication of crack-free UTEs (> 300 µm) while simultaneously mitigating environmental toxicity concerns. The three-layer N-UTEs (> 220 µm) with a gradient porosity of (~34%, ~31%, ~27%) deliver an exceeding areal capacity over 5 mAh/cm² at 0.29 mA/cm² and a high-capacity retention over 62% at 2.9 mA/cm², indicating a favorable balance between the areal capacity and the high-rate behavior. Detailed mechanistic simulations reveal that the multi-center reaction pathways enabled by enhanced ionic accessibility in N-UTEs significantly improve reaction kinetics. This work offers new insights into the gradient porosity tailoring for high-areal-capacity and high-rate UTEs for the next generation LIBs.
- Gradient porous structure,
- Electrode kinetics,
- Ultra-thick electrodes,
- Solvent-free processing method,
- Lithium-ion battery
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