1 μm-Thick Robust Gel Polymer Electrolyte with Excellent Interfacial Stability for High-Performance Li Metal Batteries

Feng, Jianwen1,2; Wang, Jiayi1,2; Gu, Qiao1; Li, Pingting2; Xu, Hongli3; Deng, Yonghong3; Gao, Ping1,2

2024-08-01

10.1002/adfm.202412287

ADVANCED FUNCTIONAL MATERIALS   影响因子和分区

1616-301X

1616-3028

["Gel polymer electrolytes (GPEs) hold great promise for lithium (Li) metal batteries (LMBs). Nevertheless, a critical challenge lies in reducing the thickness of GPEs while maintaining their mechanical integrity to achieve high-energy-density LMBs. Additionally, protecting the Li metal anode via electrolyte engineering in GPEs remains demanding. Herein, an innovative ultrathin (1 mu m-thick) yet robust GPE developed using an in situ curing technique, featuring a nanofibrous, exceptionally strong polyethylene separator is presented. The unique microstructure, interfacial conformability, and ultrahigh mechanical robustness of the ultrathin polyethylene separator are thoroughly verified. Enhanced ionic association within the GPE is achieved due to the strong affinity of electrolyte solvent with the fluorinated polymer network, as confirmed by large-scale molecular dynamics simulations. The optimized solvation structure with high contact ion pairs and aggregate fractions contributes to forming an anion-derived inorganic-rich solid electrolyte interphase (SEI), thereby protecting the lithium anode. Benefiting from the ultrahigh robustness of GPE and the excellent interfacial stability, the Li metal full cell with a high mass loading LiNi0.8Co0.1Mn0.1O2 cathode (approximate to 17.3 mg cm-2) and thin Li foil anode (50 mu m) demonstrates 91% capacity retention after 200 cycles. This design demonstrates a feasible approach toward the practical quasi-solid-state LMBs.","An innovative ultrathin (1 mu m) and robust gel polymer electrolyte (GPE) for lithium metal batteries is successfully prepared using an in situ curing technique. The ultrahigh robustness of the polyethylene separator and the optimized solvation structure within the GPE contribute to the construction of durable and stable interfacial layers, leading to extraordinary cycling stability in practical quasi-solid-state Li metal batteries. image"]

interfacial stability lithium metal batteries ultrathin gel polymer electrolytes ultrathin polyethylene membrane

SCI ; EI

英语

通讯

Guangzhou Municipal Government and Shenzhen Science and Technology Program[JCYJ20220818100407016]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter

WOS:001292131800001

WILEY-V C H VERLAG GMBH

MATERIALS SCIENCE

Web of Science

1.Hong Kong Univ Sci & Technol, Dept Chem & Biol Engn, Adv Mat Thrust, Interdisciplinary Off,Clear Water Bay, Hong Kong 999077, Peoples R China
2.Hong Kong Univ Sci & Technol Guangzhou, Adv Mat Thrust, Funct Hub, Multifunct Polymer Membranes Res Facil, Guangzhou 511453, Peoples R China
3.Southern Univ Sci & Technol, Sch Innovat & Entrepreneurship, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China

Feng, Jianwen,Wang, Jiayi,Gu, Qiao,et al. 1 μm-Thick Robust Gel Polymer Electrolyte with Excellent Interfacial Stability for High-Performance Li Metal Batteries[J]. ADVANCED FUNCTIONAL MATERIALS,2024.

Feng, Jianwen.,Wang, Jiayi.,Gu, Qiao.,Li, Pingting.,Xu, Hongli.,...&Gao, Ping.(2024).1 μm-Thick Robust Gel Polymer Electrolyte with Excellent Interfacial Stability for High-Performance Li Metal Batteries.ADVANCED FUNCTIONAL MATERIALS.

Feng, Jianwen,et al."1 μm-Thick Robust Gel Polymer Electrolyte with Excellent Interfacial Stability for High-Performance Li Metal Batteries".ADVANCED FUNCTIONAL MATERIALS (2024).