The poor dispersibility, strong interlayer interaction, and inferior crack resistance ability restrict the employment of graphene as a lubricant additive. Herein, we prepared fluorinated graphene with different F/C ratios by direct fluorination of multilayer graphene utilizing F. Among them, highly fluorinated graphene (HFG) with an F/C ratio of about 1.0 presented prominent thermal stability and excellent tribological performance as an oil-based lubricant additive, whose friction coefficient and wear rate had a 51.4 and 90.9% decrease compared to that of pristine graphene, respectively. It was confirmed that C-F bonds perpendicular to the graphene plane contributed to increasing the interlayer distance and tribological performance of fluorinated graphene, while the randomly oriented CF and CF groups did not count as influential, as demonstrated via X-ray diffraction, X-ray photoelectron spectroscopy, and polarized attenuated total reflection-Fourier transform infrared spectroscopy. Meanwhile, Raman measurements traced the formation process of integrated and stable HFG tribofilm during friction process, and the corresponding stability was attributed to the physical and chemical interactions between HFG and friction pairs. More interestingly, the outstanding crack resistance ability of HFG preserved the sheet structure from destruction due to decreased in-plane stiffness and out-plane stress, thus constructing the tough tribofilm. The simple and feasible preparation makes HFG a promising candidate as advanced lubricant in industrial fabrication.

By employing honeycomb GO with large surface area as the starting materials and using elemental fluorine, we developed a novel, straightforward topotactic route toward highly fluorinated graphene in really large quantities at low temperature. The value of F/C molar ratio approaches to 1.02. Few-layer fluorinated graphene sheets are obtained, among which the yield of monolayered FG sheet is about 10% and the number of layers is mainly in the range of 2-5. Variations in morphology and chemical structure of fluorinated graphene were explored, and some physical properties were reported.

Figure 1. Timeline showing synthetic methods for FG in the past decade. Image for "Direct gas fluorination": Reproduced with permission.

Sufficient amounts of fluorographene sheets with different sheet-size and fluorine/carbon ratio were synthesized for preparing of fluorographene/polyimide hybrids in order to explore the effect of fluorographene on the dielectric properties of hybrid materials. It is found that the fluorine/carbon ratio, width of band gap, and sheet-size of fluorographene play the important roles in determining the final dielectric properties of hybrids. The fluorographene with high fluorine/carbon ratio (F/C ≈ 1) presents broaden band gap, enhanced hydrophobicity, good dispersity and thermal stability, etc. Even at a very low filling, only 1 wt %, its polyimide hybrids exhibited drastically reduced dielectric constants as low as 2.1 without sacrificing thermal stability, improved mechanical properties obviously and decreased water absorption by about 120% to 1.0 wt %. This provides a novel route for improving the dielectric properties of materials and a new thought to carry out the application of fluorographene as an advanced material.

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