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In this study, Si-doped graphene nanoflakes (Si-GNFs) were synthesized by the pyrolysis of the hexane+tetramethylsilane mixtures over a MgO template using a tubular quartz reactor. To prepare the electrodes, 80 wt.% active materials, 10 wt.% super-P, and 10 wt.% polyacrylic acid binder were mixed homogeneously in an N-methylpyrrolidinone solvent to form a uniform slurry. The slurry was coated on the copper foils and then dried at 100 °C under vacuum for 16 h. Galvanostatic charge/discharge measurements were carried out at a potential range of 0.01–3.0 V using a Landt Instr. CT2001A battery tester.