Optimized Lithium Ion Coordination via Chlorine Substitution to Enhance Ionic Conductivity of Garnet-Based Solid Electrolytes
Shuhan Wang
College of Materials and Chemistry & Chemical Engineering, Chengdu University of Technology, 1#, Dongsanlu, Erxianqiao, Chengdu, Sichuan, 610059 P. R. China
Search for more papers by this authorTing Zeng
College of Materials and Chemistry & Chemical Engineering, Chengdu University of Technology, 1#, Dongsanlu, Erxianqiao, Chengdu, Sichuan, 610059 P. R. China
Search for more papers by this authorXiaojuan Wen
College of Materials and Chemistry & Chemical Engineering, Chengdu University of Technology, 1#, Dongsanlu, Erxianqiao, Chengdu, Sichuan, 610059 P. R. China
Search for more papers by this authorHaoyang Xu
College of Materials and Chemistry & Chemical Engineering, Chengdu University of Technology, 1#, Dongsanlu, Erxianqiao, Chengdu, Sichuan, 610059 P. R. China
Search for more papers by this authorFengxia Fan
College of Materials and Chemistry & Chemical Engineering, Chengdu University of Technology, 1#, Dongsanlu, Erxianqiao, Chengdu, Sichuan, 610059 P. R. China
Search for more papers by this authorXinxiang Wang
College of Materials and Chemistry & Chemical Engineering, Chengdu University of Technology, 1#, Dongsanlu, Erxianqiao, Chengdu, Sichuan, 610059 P. R. China
Search for more papers by this authorGuilei Tian
College of Materials and Chemistry & Chemical Engineering, Chengdu University of Technology, 1#, Dongsanlu, Erxianqiao, Chengdu, Sichuan, 610059 P. R. China
Search for more papers by this authorSheng Liu
College of Materials and Chemistry & Chemical Engineering, Chengdu University of Technology, 1#, Dongsanlu, Erxianqiao, Chengdu, Sichuan, 610059 P. R. China
Search for more papers by this authorPengfei Liu
College of Materials and Chemistry & Chemical Engineering, Chengdu University of Technology, 1#, Dongsanlu, Erxianqiao, Chengdu, Sichuan, 610059 P. R. China
Search for more papers by this authorChuan Wang
College of Materials and Chemistry & Chemical Engineering, Chengdu University of Technology, 1#, Dongsanlu, Erxianqiao, Chengdu, Sichuan, 610059 P. R. China
Search for more papers by this authorChenrui Zeng
College of Materials and Chemistry & Chemical Engineering, Chengdu University of Technology, 1#, Dongsanlu, Erxianqiao, Chengdu, Sichuan, 610059 P. R. China
Search for more papers by this authorCorresponding Author
Chaozhu Shu
College of Materials and Chemistry & Chemical Engineering, Chengdu University of Technology, 1#, Dongsanlu, Erxianqiao, Chengdu, Sichuan, 610059 P. R. China
E-mail: [email protected]
Search for more papers by this authorShuhan Wang
College of Materials and Chemistry & Chemical Engineering, Chengdu University of Technology, 1#, Dongsanlu, Erxianqiao, Chengdu, Sichuan, 610059 P. R. China
Search for more papers by this authorTing Zeng
College of Materials and Chemistry & Chemical Engineering, Chengdu University of Technology, 1#, Dongsanlu, Erxianqiao, Chengdu, Sichuan, 610059 P. R. China
Search for more papers by this authorXiaojuan Wen
College of Materials and Chemistry & Chemical Engineering, Chengdu University of Technology, 1#, Dongsanlu, Erxianqiao, Chengdu, Sichuan, 610059 P. R. China
Search for more papers by this authorHaoyang Xu
College of Materials and Chemistry & Chemical Engineering, Chengdu University of Technology, 1#, Dongsanlu, Erxianqiao, Chengdu, Sichuan, 610059 P. R. China
Search for more papers by this authorFengxia Fan
College of Materials and Chemistry & Chemical Engineering, Chengdu University of Technology, 1#, Dongsanlu, Erxianqiao, Chengdu, Sichuan, 610059 P. R. China
Search for more papers by this authorXinxiang Wang
College of Materials and Chemistry & Chemical Engineering, Chengdu University of Technology, 1#, Dongsanlu, Erxianqiao, Chengdu, Sichuan, 610059 P. R. China
Search for more papers by this authorGuilei Tian
College of Materials and Chemistry & Chemical Engineering, Chengdu University of Technology, 1#, Dongsanlu, Erxianqiao, Chengdu, Sichuan, 610059 P. R. China
Search for more papers by this authorSheng Liu
College of Materials and Chemistry & Chemical Engineering, Chengdu University of Technology, 1#, Dongsanlu, Erxianqiao, Chengdu, Sichuan, 610059 P. R. China
Search for more papers by this authorPengfei Liu
College of Materials and Chemistry & Chemical Engineering, Chengdu University of Technology, 1#, Dongsanlu, Erxianqiao, Chengdu, Sichuan, 610059 P. R. China
Search for more papers by this authorChuan Wang
College of Materials and Chemistry & Chemical Engineering, Chengdu University of Technology, 1#, Dongsanlu, Erxianqiao, Chengdu, Sichuan, 610059 P. R. China
Search for more papers by this authorChenrui Zeng
College of Materials and Chemistry & Chemical Engineering, Chengdu University of Technology, 1#, Dongsanlu, Erxianqiao, Chengdu, Sichuan, 610059 P. R. China
Search for more papers by this authorCorresponding Author
Chaozhu Shu
College of Materials and Chemistry & Chemical Engineering, Chengdu University of Technology, 1#, Dongsanlu, Erxianqiao, Chengdu, Sichuan, 610059 P. R. China
E-mail: [email protected]
Search for more papers by this authorAbstract
Garnet-type solid-state electrolytes attract abundant attentions due to the broad electrochemical window and remarkable thermal stability while their poor ionic conductivity obstructs their widespread application in all-solid-state batteries. Herein, the enhanced ionic conductivity of garnet-type solid electrolytes is achieved by partially substituting O2− sites with Cl− anions, which effectively reduce Li+ migration barriers while preserving the highly conductive cubic phase of garnet-type solid-state electrolytes. This substitution not only weakens the anchoring effect of anions on Li+ to widen the size of Li+ diffusion channel but also optimizes the occupancy of Li+ at different sites, resulting in a substantial reduction of the Li+ migration barrier and a notable improvement in ionic conductivity. Leveraging these advantageous properties, the developed Li6.35La3Zr1.4Ta0.6O11.85-Cl0.15 (LLZTO-0.15Cl) electrolyte demonstrates high Li+ conductivity of 4.21×10−6 S cm−1. When integrated with LiFePO4 (LFP) cathode and metallic lithium anode, the LLZTO-0.15Cl electrolyte enables the solid-state battery to operate for more than 100 cycles with a high capacity retention of 76.61% and superior Coulombic efficiency of 99.48%. This work shows a new strategy for modulating anionic framework to enhance the conductivity of garnet-type solid-state electrolytes.
Conflict of Interest
The authors declare no conflict of interest.
Open Research
Data Availability Statement
Research data are not shared.
Supporting Information
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