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Vol. 16 (2024)

Highly Efficient Aligned Ion-Conducting Network and Interface Chemistries for Depolarized All-Solid-State Lithium Metal Batteries

https://doi.org/10.1007/s40820-023-01301-4
Yongbiao Mu
Shenzhen Key Laboratory of Advanced Energy Storage, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China
Shixiang Yu
Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China
Yuzhu Chen
Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China
Youqi Chu
Shenzhen Key Laboratory of Advanced Energy Storage, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China
Buke Wu
Shenzhen Key Laboratory of Advanced Energy Storage, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China
Qing Zhang
Shenzhen Key Laboratory of Advanced Energy Storage, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China
Binbin Guo
Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China
Lingfeng Zou
Shenzhen Key Laboratory of Advanced Energy Storage, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China
Ruijie Zhang
Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China
Fenghua Yu
Shenzhen Key Laboratory of Advanced Energy Storage, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China
Meisheng Han
Shenzhen Key Laboratory of Advanced Energy Storage, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China
Meng Lin
Shenzhen Key Laboratory of Advanced Energy Storage, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China
Jinglei Yang
Department of Mechanical and Aerospace Engineering, Hong Kong University of Science and Technology, Kowloon 997077, Hong Kong Special Administrative Region of China, People’s Republic of China
Jiaming Bai
Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China
Lin Zeng
Shenzhen Key Laboratory of Advanced Energy Storage, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China

Corresponding Author: Lin Zeng

zengl3@sustech.edu.cn

Nano-Micro Letters, Vol. 16 (2024), Article Number: 86

Abstract

Improving the long-term cycling stability and energy density of all-solid-state lithium (Li)-metal batteries (ASSLMBs) at room temperature is a severe challenge because of the notorious solid–solid interfacial contact loss and sluggish ion transport. Solid electrolytes are generally studied as two-dimensional (2D) structures with planar interfaces, showing limited interfacial contact and further resulting in unstable Li/electrolyte and cathode/electrolyte interfaces. Herein, three-dimensional (3D) architecturally designed composite solid electrolytes are developed with independently controlled structural factors using 3D printing processing and post-curing treatment. Multiple-type electrolyte films with vertical-aligned micro-pillar (p-3DSE) and spiral (s-3DSE) structures are rationally designed and developed, which can be employed for both Li metal anode and cathode in terms of accelerating the Li+ transport within electrodes and reinforcing the interfacial adhesion. The printed p-3DSE delivers robust long-term cycle life of up to 2600 cycles and a high critical current density of 1.92 mA cm−2. The optimized electrolyte structure could lead to ASSLMBs with a superior full-cell areal capacity of 2.75 mAh cm−2 (LFP) and 3.92 mAh cm−2 (NCM811). This unique design provides enhancements for both anode and cathode electrodes, thereby alleviating interfacial degradation induced by dendrite growth and contact loss. The approach in this study opens a new design strategy for advanced composite solid polymer electrolytes in ASSLMBs operating under high rates/capacities and room temperature.


Highlights:
1 This study introduces an innovative 3D-printed electrolyte with vertically aligned ion transport network, which contains well-dispersed nanoscale Ta-doped Li7La3Zr2O12 in a poly(ethylene glycol) diacrylate matrix.
2 The 3DSE architecture enables efficient ion transport across the Li/electrolyte and electrolyte/cathode interfaces, which allows for increased active material mass loading and enhanced interfacial adhesion.
3 The p-3DSE Li symmetric cell displays an impressive critical current density value of 1.92 mA cm−2 and stable operation for 2600 h at room temperature. Full cells using p-3DSE achieve notable areal capacities.

Keywords

All-solid-state lithium metal batteries Composite solid electrolyte 3D printing Areal capacity Interfacial degradation
Mu, Yongbiao, Shixiang Yu, Yuzhu Chen, Youqi Chu, Buke Wu, Qing Zhang, Binbin Guo, Lingfeng Zou, Ruijie Zhang, Fenghua Yu, Meisheng Han, Meng Lin, Jinglei Yang, Jiaming Bai, and Lin Zeng. 2024. “Highly Efficient Aligned Ion-Conducting Network and Interface Chemistries for Depolarized All-Solid-State Lithium Metal Batteries”. Nano-Micro Letters 16 (January):86. https://doi.org/10.1007/s40820-023-01301-4.
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