Engineering the Structural Uniformity of Gel Polymer Electrolytes via Pattern-Guided Alignment for Durable, Safe Solid-State Lithium Metal Batteries

Qi Kang; Zechao Zhuang; Yijie Liu; Zhenhui Liu; Yong Li; Bin Sun; Fei Pei; Han Zhu; Hongfei Li; Pengli Li; Ying Lin; Kunming Shi; Yingke Zhu; Jie Chen; Chaoqun Shi; Yan Zhao; Pingkai Jiang; Yongyao Xia; Dingsheng Wang; Xingyi Huang

doi:10.1002/adma.202303460

Engineering the Structural Uniformity of Gel Polymer Electrolytes via Pattern-Guided Alignment for Durable, Safe Solid-State Lithium Metal Batteries

Adv Mater. 2023 Sep;35(38):e2303460. doi: 10.1002/adma.202303460. Epub 2023 Jul 23.

Authors

Qi Kang¹, Zechao Zhuang^{2

3}, Yijie Liu¹, Zhenhui Liu⁴, Yong Li⁵, Bin Sun^{6

7}, Fei Pei⁸, Han Zhu⁹, Hongfei Li¹, Pengli Li¹, Ying Lin¹, Kunming Shi¹, Yingke Zhu¹, Jie Chen¹, Chaoqun Shi¹⁰, Yan Zhao^{11

12}, Pingkai Jiang¹, Yongyao Xia⁴, Dingsheng Wang², Xingyi Huang¹

Affiliations

¹ Department of Polymer Science and Engineering, Shanghai Key Laboratory of Electrical Insulation and Thermal Ageing, School of Chemistry and Chemical Engineering, State Key Laboratory of Metal Matrix Composites, Shanghai Jiao Tong University, Shanghai, 200240, China.
² Department of Chemistry, Tsinghua University, Beijing, 100084, China.
³ Department of Chemical Engineering, Columbia University, New York, NY, 10027, USA.
⁴ College of Material Science and Engineering, Nanjing University of Aeronautics and Astronautics, Nanjing, 210016, China.
⁵ Institute of Applied and Physical Chemistry and Center for Environmental Research and Sustainable Technology, University of Bremen, 28359, Bremen, Germany.
⁶ College of Electronics and Information, Qingdao University, Qingdao, 266071, China.
⁷ Weihai Innovation Research Institute of Qingdao University, Weihai, 264200, China.
⁸ State Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, 430074, China.
⁹ Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, Jiangnan University, Wuxi, 214122, China.
¹⁰ School of Electrical Engineering, Xi'an Jiaotong University, Xi'an, 710049, China.
¹¹ College of Materials Science and Engineering, Sichuan University, Chengdu, 610065, China.
¹² Institute of Technological Science, Wuhan University, Wuhan, 430070, China.

PMID: 37269455
DOI: 10.1002/adma.202303460

Abstract

Ultrathin and super-toughness gel polymer electrolytes (GPEs) are the key enabling technology for durable, safe, and high-energy density solid-state lithium metal batteries (SSLMBs) but extremely challenging. However, GPEs with limited uniformity and continuity exhibit an uneven Li⁺ flux distribution, leading to nonuniform deposition. Herein, a fiber patterning strategy for developing and engineering ultrathin (16 µm) fibrous GPEs with high ionic conductivity (≈0.4 mS cm^-1 ) and superior mechanical toughness (≈613%) for durable and safe SSLMBs is proposed. The special patterned structure provides fast Li⁺ transport channels and tailoring solvation structure of traditional LiPF₆ -based carbonate electrolyte, enabling rapid ionic transfer kinetics and uniform Li⁺ flux, and boosting stability against Li anodes, thus realizing ultralong Li plating/stripping in the symmetrical cell over 3000 h at 1.0 mA cm^-2 , 1.0 mAh cm^-2 . Moreover, the SSLMBs with high LiFePO₄ loading of 10.58 mg cm^-2 deliver ultralong stable cycling life over 1570 cycles at 1.0 C with 92.5% capacity retention and excellent rate capacity of 129.8 mAh g^-1 at 5.0 C with a cut-off voltage of 4.2 V (100% depth-of-discharge). Patterned GPEs systems are powerful strategies for producing durable and safe SSLMBs.

Keywords: high uniformity; long cycling life; patterned structures; solid-state lithium metal batteries; ultrathin gel polymer electrolytes.

Abstract

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