This study investigates the carbon products generated by melamine under various heat-treatment temperatures with the catalysis of calcium carbonate. We discovered that the cost-effective precursor melamine readily self-assembles and curls into graphene tubes when catalyzed by the alkaline earth salt CaCO3 at elevated temperatures. Under heat-treatment conditions of 1100 °C and 1200 °C, the growth morphology of graphene tubes with open structures and exceptionally large diameters was observed, and the diameters reached the micron level. These products exhibit a high degree of carbonization and an extremely low nitrogen content, as low as 1.7%. Further, the intensity ratio (ID/IG) of the D band and the G band is as low as 0.79 in Raman characterization. The results show that the products have a certain graphite structure, which proves the catalytic activity of CaCO3. This is attributed to the incorporation of CaCO3 into the raw material system, which impedes the complete thermal decomposition of melamine. On the other hand, the resulting CaO particles are evenly distributed along the tubular products, providing certain support for their self-assembly and growth, thereby achieving the efficient growth of graphene tubes.
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