Abstract
Fluorinated graphene has a promising application prospect in lithium primary batteries (LPBs) and sodium primary batteries (SPBs). Herein, five fluorinated graphene materials with different fluorine contents (FG-x) are prepared by a large-scale gas fluorination process. It is found that the structural characteristics of FG-x strongly depend on the fluorination temperature: the fluorine content (i.e., F/C ratio) gradually increases with the fluorination temperature rising, resulting in the enlargement of interlayer spacing and the increase of average bonding strength between C and F. FG-0.75 sample with the intermediate degree of fluorination achieves the maximum energy densities in LPBs (2239.8 Wh·kg−1) and SPBs (1939.2 Wh·kg−1). The interlayer distance is critical to the rate capability of FG-x, and FG-0.95 with the largest lattice spacing exhibits the best rate performance in both Li/CFx and Na/CFx batteries. The electrochemical reaction mechanism and the structural evolution of FG material revealed by ex situ X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD) characterization, and in situ Raman spectra further confirm the effect of interlayer distance.
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摘要
氟化石墨烯在锂、钠一次电池中具有广阔的应用前景。 本文采用大规模气体氟化法制备了5 种不同氟含量的氟 化石墨烯材料(FG-x)。结果表明,FG-x 的结构特征与氟化温度密切相关:随着氟化温度的升高,氟含量(即F/C 比)逐渐增大,导致了层间距的增大以及C–F 键结合能的增加。中间样品FG-0.75 在LPBs (2239.8 Wh·kg−1)和 SPBs (1939.2 Wh·kg−1)中均表现出最大的能量密度。层间距对FG-x 的倍率性能至关重要,晶格间距最大的FG- 0.95 在Li/CFx 和Na/CFx 电池中均表现出最佳的倍率性能。通过非原位XPS、XRD 和原位拉曼光谱揭示了FG 材 料的电化学反应机理和结构演变,进一步证实了层间距离的影响。
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Acknowledgements
This study was financially supported by the National Natural Science Foundation of China (No. 22078179) and Taishan Scholar Foundation (No. tsqn201812063). We are particularly grateful to Shandong Zhongshan Photoelectric Materials Co., Ltd. for the help on the fluorination process.
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Li, YY., Liu, C., Chen, L. et al. Multi-layered fluorinated graphene cathode materials for lithium and sodium primary batteries. Rare Met. 42, 940–953 (2023). https://doi.org/10.1007/s12598-022-02155-2
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DOI: https://doi.org/10.1007/s12598-022-02155-2