Defective nano-structure regulating C-F bond for lithium/fluorinated carbon batteries with dual high-performance. (15th December 2022)

• Record Type: Journal Article
• Authors: Kong, Lingchen; Li, Yu; Peng, Cong; Sun, Lidong; Wang, Kai; Liu, Yong; Feng, Wei
• Is Part Of: Nano energy. Volume 104(2022)Part A
• Publication Date: 2022-12-15
• Subjects: Regulating C-F bond -- Nano defect engineering -- Heteroatomic doping -- Dual ultrahigh performance -- Li-CFx battery; Nanoscience -- Periodicals; Nanotechnology -- Periodicals; Nanostructured materials -- Periodicals; Power resources -- Technological innovations -- Periodicals; Nanoscience; Nanostructured materials; Nanotechnology; Power resources -- Technological innovations; Periodicals; 621.042
• DOI: 10.1016/j.nanoen.2022.107905
• Languages: English
• ISSNs: 2211-2855

Abstract

Abstract: Lithium/fluorinated carbon (Li/CF x ) batteries show significant potential owing to high energy density and long-term storage performance. Restricted to the mutual restriction of F/C ratio and conductivity, the high energy density and power density cannot be achieved simultaneously. Herein, fluorinated honeycomb N-doped graphene (F-HNG) with conductive C-F bond was regulated by structural and heteroatomic defects, which was fabricated by nanoscale etching, NH3 treatment and gas phase fluorination. The unique pore provided smooth channels and storage sites for Li + migration, while N atom with more electronegativity further regulated the charge distribution of the carbon skeleton. F-HNG delivered dual excellent electrochemical performance of a maximum energy density of 2595.47 Wh kg -1, associated with the unprecedented power density of 73.203 kW kg -1 at an ultrahigh rate of 50 C. Li/F-HNG pouch cell achieved an energy density of 707.52 Wh kg -1 with a mass loading of 10–15 mg cm -2 and reduced the heat release and battery swelling. In-depth density functional theory (DFT) calculations revealed that synergistic effect of porosity and N-doping regulated its C-F bond configuration, thermodynamic parameters, and ion diffusion pathway. This work indicates that nano-defect engineering and heteroatomic doping provide innovative possible directions for the design of CF x cathodes with dual superior performance. Graphical Abstract: Honeycomb N-doped graphene was first proposed as precursor of CF x, delivering ultrahigh energy density and power density. The synergistic effects of porosity and N-doping directly affected charge distribution and reactivity of carbon skeleton, yielding semi-ionic C-F bonds with high electrochemical activity, while the pore structure provided a smooth channel and storage place for Li + migration. ga1 Highlights: A novel fluorinated honeycomb nitrogen-doped graphene (F-HNG) with conductive C-F bond and high F/C ratio was reported. The synergistic effects of the structural and heteroatomic defects regulate the C-F bond configuration and thermodynamic parameters. The obtained Li/F-HNG coin cell deliver dual high-performance with a maximum energy density of 2595.47 Wh kg -1 and the unprecedented power density of 73.203 kW kg -1 at an ultrahigh rate of 50 C. The Li/F-HNG pouch cell exhibited an energy density of 707.52 Wh kg -1 at 0.01 C.