Lithium-fluorinated carbon (Li-CFx) batteries have become one of the most widely applied power sources for high energy density applications because of the advantages provided by the CFx cathode. Moreover, the large gap between the practical and theoretical potentials alongside the stoichiometric limit of commercial graphite fluorides indicates the potential for further energy improvement. Herein, monolayer fluorinated graphene nanoribbons (F-GNRs) were fabricated by unzipping single-walled carbon nanotubes (SWCNTs) using pure F2 gas at high temperature, which delivered an unprecedented energy density of 2738.45 W h kg−1 due to the combined effect of a high fluorination degree and discharge plateau, realized by the abundant edges and destroyed periodic structure, respectively. Furthermore, at a high fluorination temperature, the theoretical calculation confirmed a zigzag pathway of fluorine atoms that were adsorbed outside of the SWCNTs and hence initiated the spontaneous process of unzipping SWCNTs to form the monolayer F-GNRs. The controllable fluorination of SWCNTs provided a feasible approach for preparing CFx compounds for different applications, especially for ultrahigh energy density cathodes.
由于CFx正极材料的优势, 锂-氟化碳(Li-CFx)电池已成为一 种应用广泛、能提供巨大能量密度的电源之一. 但其实际放电电 压与理论放电电压之间的较大差距, 以及商用氟化石墨的化学计 量极限, 使得进一步提高其能量密度面临挑战. 本文采用纯F2气体 直接在高温下对单壁碳纳米管(SWCNTs)进行切割, 制备出单层氟 化石墨烯纳米带(F-GNRs). 丰富的边缘结构和碳骨架周期性结构 的破坏使其具有高的氟化程度和放电平台, 从而使其能量密度高 达2738.45 W h kg−1. 理论计算表明在高氟化温度下, 氟原子在碳纳 米管外以zigzag路径吸附, 进一步证实了切割单壁碳纳米管形成单 层F-GNRs为自发过程. 单壁碳纳米管的可控氟化为制备具有不同 用途的CFx, 特别是具有超高能量密度正极材料提供了一条可行途 径.
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This work was financially supported by the National Key R&D Program of China (2016YFA0202302), the State Key Program of National Natural Science Foundation of China (51633007), and the National Natural Science Foundation of China (51773147, 51803149 and 51973151).
The manuscript was written through contributions of all authors. All authors have given approval to the final version of the manuscript.
Conflict of interest
The authors declare no conflict of interest.
Cong Peng obtained his MSc degree from Hubei University in 2016. He is currently working on his PhD in Professor Feng’s group at the School of Materials Science and Engineering in Tianjin University. His research interests include the synthesis, assemblies, and application of fluorinated carbon materials.
Yu Li is a lecturer at the School of Materials Science and Engineering, Tianjin University. He obtained his PhD degree from Tianjin University in 2011 and had worked as a postdoctoral research fellow at Tianjin University from 2011 to 2014. His current research is focused on conductive polymers and nano energy storage materials.
Wei Feng received his PhD in 2000 from Xi’an Jiaotong University focusing on photoelectric properties and device applications of novel conducting polymers. Then he worked at Osaka University and Tsinghua University as a JSPS fellow and postdoctoral researcher, respectively. In 2004, he became a full professor at Tianjin University. His research interest is the functional nanocarbon materials.
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Peng, C., Kong, L., Li, Y. et al. Fluorinated graphene nanoribbons from unzipped single-walled carbon nanotubes for ultrahigh energy density lithium-fluorinated carbon batteries. Sci. China Mater. (2021). https://doi.org/10.1007/s40843-020-1551-x
- fluorinated graphene nanoribbons
- single-walled carbon nanotubes
- ultrahigh energy density
- lithium-fluorinated carbon batteries