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Fast Ion Transport in Li-Rich Alloy Anode for High-Energy-Density All Solid-State Lithium Metal Batteries
Authors:Xuejie Gao  Xiaofei Yang  Ming Jiang  Matthew Zheng  Yang Zhao  Ruying Li  Wenfeng Ren  Huan Huang  Runcang Sun  Jiantao Wang  Chandra Veer Singh  Xueliang Sun
Affiliation:1. Department of Mechanical and Materials Engineering, University of Western Ontario, London, Ontario, N6A 5B9 Canada

Liaoning Key Laboratory of Lignocellulosic Chemistry and Biomaterials, College of Light Industry and Chemical Engineering, Dalian Polytechnic University, Dalian, 116034 China;2. Department of Mechanical and Materials Engineering, University of Western Ontario, London, Ontario, N6A 5B9 Canada;3. Institute of Physical Science and Information Technology, Anhui University, Hefei, 230601 China

Department of Materials Science and Engineering, University of Toronto, 184 College Street, Suite 140, Toronto, Ontario, M5S 3E4 Canada;4. Liaoning Key Laboratory of Lignocellulosic Chemistry and Biomaterials, College of Light Industry and Chemical Engineering, Dalian Polytechnic University, Dalian, 116034 China;5. Glabat Solid-State Battery Inc., 700 Collip Circle, London, Ontario, N6G 4X8 Canada;6. Department of Materials Science and Engineering, University of Toronto, 184 College Street, Suite 140, Toronto, Ontario, M5S 3E4 Canada

Abstract:All-solid-state Li batteries (ASSLBs) with solid-polymer electrolytes are considered promising battery systems to achieve improved safety and high energy density. However, Li dendrite formation at the Li anode under high charging current density/capacity has limited their development. To tackle the issue, Li-metal alloying has been proposed as an alternative strategy to suppress Li dendrite growth in ASSLBs. One drawback of alloying is the relatively lower operating cell voltages, which will inevitably lower energy density compared to cells with pure Li anode. Herein, a Li-rich Li13In3 alloy electrode (LiRLIA) is proposed, where the Li13In3 alloy scaffold guides Li nucleation and hinders Li dendrite formation. Meanwhile, the free Li can recover Li's potential and facilitate fast charge transfer kinetics to realize high-energy-density ASSLBs. Benefitting from the stronger adsorption energy and lower diffusion energy barrier of Li on a Li13In3 substrate, Li prefers to deposit in the 3D Li13In3 scaffold selectively. Therefore, the Li–Li symmetric cell constructed with LiRLIA can operate at a high current density/capacity of 5 mA cm?2/5 mAh cm?2 for almost 1000 h.
Keywords:density functional theory calculations  high-energy-density solid-state batteries  Li dendrite suppression  Li-rich Li13In3 alloys  Li's potential levels
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