Crystal Facet‐Engineered Anion Regulation Enables Fast‐Charging Stability in Lithium Metal Batteries
Abstract
AbstractLithium metal batteries (LMBs) offer exceptional energy density and output voltage. However, their practical application remains hindered by sluggish ion transport and uncontrolled lithium dendrite formation, particularly under fast‐charging conditions. Here, we report a facet‐engineered anion‐regulating separator based on zeolitic imidazolate framework‐8 (ZIF‐8) with preferentially crystal‐exposed (110) facets. The coordinatively unsaturated Zn centers on this surface serve as Lewis acid sites that selectively anchor bis(trifluoromethanesulfonyl)imide anions (TFSI−), inducing directional Li+ flux and suppressing dendritic growth. Concurrently, the microporous framework facilitates spatial lithium confinement, mitigating local current density and enhancing interfacial stability. As a result, the engineered separator enables ultra‐stable cycling of Li||Cu cells for over 1400 cycles at 2 mA cm−2 and 1 mAh cm−2, delivering an average Coulombic efficiency of 98.7%. In full‐cell configurations, LiFePO4 (LFP) cells exhibit 99.9% Coulombic efficiency over 3000 cycles at 5 C, while high‐loading Li||LiNi0.8Co0.1Mn0.1O2 (NCM811, 12.30 mg cm−2) cell retains 84.4% of its capacity after 135 cycles. Furthermore, a Li||LFP pouch cell with a high cathode loading of 19.92 mg cm−2 demonstrates robust cycling over 170 cycles. These findings establish facet‐engineered separators based on framework materials as a versatile and scalable strategy for advancing stable and fast‐charging metal batteries.
Article Details
Authors (15)
Chunli Liu
Xi’an Key Laboratory of Sustainable Energy Materials Chemistry, Department of Applied Chemistry, School of Chemistry
Weiping Li
Beijing National Laboratory for Condensed Matter Physics
Zheng Wang
Zhengqian Jin
School of Chemistry, Engineering Research Center of Energy Storage Materials and Devices, Ministry of Education, National Innovation Platform (Center) for Industry‐Education Integration of Energy Storage Technology, State Key Laboratory of Electrical Insulation and Power Equipment, Engineering Research Center of Energy Storage Material and Chemistry Universities of Shaanxi Province, Xi'an Jiaotong University Xi'an 710049 China
Teng Deng
School of Earth Sciences, East China University of Technology
Zhuo Yang
Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry
Diandian Han
Department Center for Advanced Materials Research Zhongyuan University of Technology Henan P. R. China
Yaqiong Su
Engineering Research Center of Energy Storage Materials and Devices, Ministry of Education School of Chemistry
Yuankun Wang
Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry
Zhenjiang Cao
Yangyang Liu
State Key Laboratory for Mechanical Behavior of Materials, School of Instrument Science and Technology
R. Vasant Kumar
Department of Materials Science and Metallurgy University of Cambridge Cambridge UK
Wei Tang
Shujiang Ding
Engineering Research Center of Energy Storage Materials and Devices, Ministry of Education, School of Chemistry
Kai Xi
Xi’an Key Laboratory of Sustainable Energy Materials Chemistry, Department of Applied Chemistry, School of Chemistry