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Nacre-Inspired Composite Electrolytes for Load-Bearing Solid-State Lithium-Metal Batteries
Authors:Aijun Li  Xiangbiao Liao  Hanrui Zhang  Lei Shi  Peiyu Wang  Qian Cheng  James Borovilas  Zeyuan Li  Wenlong Huang  Zhenxuan Fu  Martin Dontigny  Karim Zaghib  Kristin Myers  Xiuyun Chuan  Xi Chen  Yuan Yang
Affiliation:1. Program of Materials Science and Engineering, Department of Applied Physics and Applied Mathematics, Columbia University, New York, NY, 10027 USA

Key Laboratory of Orogenic Belts and Crustal Evolution, School of Earth and Space Sciences, Peking University, Beijing, 100871 China;2. Earth Engineering Center, Center for Advanced Materials for Energy and Environment, Department of Earth and Environmental Engineering, Columbia University, New York, NY, 10027 USA;3. Program of Materials Science and Engineering, Department of Applied Physics and Applied Mathematics, Columbia University, New York, NY, 10027 USA;4. Department of Mechanical Engineering, Columbia University, New York, NY, 10027 USA;5. IREQ-Institute Recherche d'Hydro-Québec, Varennes, Québec, J3X 1S1 Canada;6. Key Laboratory of Orogenic Belts and Crustal Evolution, School of Earth and Space Sciences, Peking University, Beijing, 100871 China

Abstract:Solid-state lithium-metal batteries with solid electrolytes are promising for next-generation energy-storage devices. However, it remains challenging to develop solid electrolytes that are both mechanically robust and strong against external mechanical load, due to the brittleness of ceramic electrolytes and the softness of polymer electrolytes. Herein, a nacre-inspired design of ceramic/polymer solid composite electrolytes with a “brick-and-mortar” microstructure is proposed. The nacre-like ceramic/polymer electrolyte (NCPE) simultaneously possesses a much higher fracture strain (1.1%) than pure ceramic electrolytes (0.13%) and a much larger ultimate flexural modulus (7.8 GPa) than pure polymer electrolytes (20 MPa). The electrochemical performance of NCPE is also much better than pure ceramic or polymer electrolytes, especially under mechanical load. A 5 × 5 cm2 pouch cell with LAGP/poly(ether-acrylate) NCPE exhibits stable cycling with a capacity retention of 95.6% over 100 cycles at room temperature, even undergoes a large point load of 10 N. In contrast, cells based on pure ceramic and pure polymer electrolyte show poor cycle life. The NCPE provides a new design for solid composite electrolyte and opens up new possibilities for future solid-state lithium-metal batteries and structural energy storage.
Keywords:composite electrolytes  mechanical load  nacre structure  solid-state batteries
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