High-quality double-walled carbon nanotubes (DWNTs) have been produced by catalyticdecomposition of benzene over Fe-Mo/Al
2O
3 catalyst at 900
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C. The produced carbonmaterials are DWNT bundles free of amorphous carbon covering on the surface. DWNTshave inner tube diameters in the range of 0.69-2.53 nm and outer tube diameters in therange of 1.44-3.30 nm. The interlayer spacing between graphene layers ranges from 0.35to 0.38 nm. Transmission electron microscopy and Raman analysis show that produced carbonmaterials have a low defect level in the atomic carbon structure, indicating the synthesis ofhigh-quality DWNTs. Our results demonstrate that benzene is an ideal carbon feedstock tosynthesize high-purity DWNTs over Fe-Mo/Al
2O
3 catalyst.