Defective nano-structure regulating C-F bond for lithium/fluorinated carbon batteries with dual high-performance

材料科学 纳米- 对偶(语法数字) 锂(药物) 化学工程 碳纤维 纳米技术 复合材料 复合数 医学 文学类 工程类 内分泌学 艺术
作者
Lingchen Kong,Yu Li,Cong Peng,Lidong Sun,Kai Wang,Yong Liu,Wei Feng
出处
期刊:Nano Energy [Elsevier]
卷期号:104: 107905-107905 被引量:33
标识
DOI:10.1016/j.nanoen.2022.107905
摘要

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, NH 3 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. 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. • A novel fluorinated honeycomb nitrogen-doped graphene (F-HNG) with both conductive C-F bond and high F/C radio was reported. • The synergistic effects of the structural and heteroatomic defects regulate the C-F bond configuration and thermodynamic parameters, while the unique pore and edge structures provide smooth channels and storage sites for Li + migration. • 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.
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