Single-walled carbon nanotubes (SWCNTs) with a narrow diameter distribution and high areal density hold great promise for a variety of applications, particularly in advanced electronics and biomedical devices. This study utilizes Mn ion doping as a strategic approach both to stabilize the ZrO2-supported Fe catalyst and regulate lattice oxygen release, thereby facilitating the growth of SWCNTs with high areal density and a narrow diameter distribution. The ZrO2-supported Fe catalyst was meticulously dispersed on Si/SiO2 (300 nm) substrates through the optimization of spin-coating speed and solvent viscosity, aiming to enhance the dispersion and uniformity. Investigation into the precise control over the Mn ion content was conducted to regulate the structure and stability of the Mn-doped ZrO2-supported Fe catalyst. Mn ions perform a dual role: they maintain a higher proportion of ZrO2 in the monoclinic phase, which in turn alleviates the monoclinic-tetragonal phase transition during chemical vapor deposition (CVD) growth. Concurrently, the conversion of Mn3+ to Mn4+ ions captures the lattice oxygen released during the formation of zirconium transition oxides. Additionally, first-principles simulations have confirmed the stabilizing impact of Mn ions on the catalyst, which reduces aggregation and maturation, ultimately resulting in a more concentrated diameter distribution of as-grown SWCNTs. This approach has successfully achieved the controlled growth of high areal density SWCNTs with a diameter distribution of 1.73 ± 0.08 nm.
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