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Introduction of CO2 is a facile way to tune the growth of vertically aligned double- or single-walled carbon nanotube (CNT) forests on wafers. In the absence of CO2, a double-walled CNT convexity was obtained. With increasing concentration of CO2, the morphologies of the forests transformed first into radial blocks, and finally into bowl-shaped forests. Furthermore, the wall number and diameter distribution of the CNTs were also modulated by varying the amount of CO2. With increasing CO2 concentration, CNTs with fewer wall number and smaller diameter were obtained. The addition of CO2 is speculated to generate water and serve as a weak oxidant for high quality CNT growth. It can tune the growth rate and the morphologies of the forests, prevent the formation of amorphous carbon, and reduce the wall number of the CNTs.
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