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

• Published in: Nano-micro letters 2024-12, Vol.16 (1), p.86-18, Article 86
• Main Authors: Mu, Yongbiao, Yu, Shixiang, Chen, Yuzhu, Chu, Youqi, Wu, Buke, Zhang, Qing, Guo, Binbin, Zou, Lingfeng, Zhang, Ruijie, Yu, Fenghua, Han, Meisheng, Lin, Meng, Yang, Jinglei, Bai, Jiaming, Zeng, Lin
• Format: Article
• Language: English
• Subjects: 3D printing; Adhesion; All-solid-state lithium metal batteries; Areal capacity; Cathodes; Composite solid electrolyte; Contact loss; Critical current density; Design; Electrocatalysis; Electrodes; Electrolytes; Electrolytic cells; Engineering; Interfacial degradation; Ion transport; Lithium batteries; Molten salt electrolytes; Nanoscale Science and Technology; Nanotechnology; Nanotechnology and Microengineering; Polyethylene glycol; Room temperature; Solid electrolytes; Solid state; Three dimensional composites; Three dimensional printing
• ISSN: 2311-6706; 2150-5551; 2150-5551
• DOI: 10.1007/s40820-023-01301-4

Highlights This study introduces an innovative 3D-printed electrolyte with vertically aligned ion transport network, which contains well-dispersed nanoscale Ta-doped Li 7 La 3 Zr 2 O 12 in a poly(ethylene glycol) diacrylate matrix. 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. 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. 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.