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

Yongbiao Mu; 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; Lin Zeng

doi:10.1007/s40820-023-01301-4

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

Nanomicro Lett. 2024 Jan 12;16(1):86. doi: 10.1007/s40820-023-01301-4.

Authors

Yongbiao Mu^#^{1

2

3}, Shixiang Yu^#^{2

4}, Yuzhu Chen^#², Youqi Chu^#^{1

2

3}, Buke Wu^{1

2

3}, Qing Zhang^{1

2

3}, Binbin Guo², Lingfeng Zou^{1

2

3}, Ruijie Zhang^{2

3}, Fenghua Yu^{1

2

3}, Meisheng Han^{1

2

3}, Meng Lin^{5

6

7}, Jinglei Yang^{8

9}, Jiaming Bai¹⁰, Lin Zeng^{11

12

13}

Affiliations

¹ Shenzhen Key Laboratory of Advanced Energy Storage, Southern University of Science and Technology, Shenzhen, 518055, People's Republic of China.
² Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen, 518055, People's Republic of China.
³ SUSTech Energy Institute for Carbon Neutrality, Southern University of Science and Technology, Shenzhen, 518055, People's Republic of China.
⁴ 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.
⁵ Shenzhen Key Laboratory of Advanced Energy Storage, Southern University of Science and Technology, Shenzhen, 518055, People's Republic of China. linm@sustech.edu.cn.
⁶ Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen, 518055, People's Republic of China. linm@sustech.edu.cn.
⁷ SUSTech Energy Institute for Carbon Neutrality, Southern University of Science and Technology, Shenzhen, 518055, People's Republic of China. linm@sustech.edu.cn.
⁸ 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. maeyang@ust.hk.
⁹ HKUST Shenzhen-Hong Kong Collaborative Innovation Research Institute, Futian, Shenzhen, People's Republic of China. maeyang@ust.hk.
¹⁰ Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen, 518055, People's Republic of China. baijm@sustech.edu.cn.
¹¹ Shenzhen Key Laboratory of Advanced Energy Storage, Southern University of Science and Technology, Shenzhen, 518055, People's Republic of China. zengl3@sustech.edu.cn.
¹² Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen, 518055, People's Republic of China. zengl3@sustech.edu.cn.
¹³ SUSTech Energy Institute for Carbon Neutrality, Southern University of Science and Technology, Shenzhen, 518055, People's Republic of China. zengl3@sustech.edu.cn.

^# Contributed equally.

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.

Keywords: 3D printing; All-solid-state lithium metal batteries; Areal capacity; Composite solid electrolyte; Interfacial degradation.