We present a floating catalyst synthesis route for individual, i.e., non-bundled, small diameter single-walled carbon nanotubes (SWCNTs) with a narrow chiral angle distribution peaking at high chiralities near the armchair species. An ex situ spark discharge generator was used to form iron particles with geometric number mean diameters of 3–4 nm and fed into a laminar flow chemical vapour deposition reactor for the continuous synthesis of long and high-quality SWCNTs from ambient pressure carbon monoxide. The intensity ratio of G/D peaks in Raman spectra up to 48 and mean tube lengths up to 4 μm were observed. The chiral distributions, as directly determined by electron diffraction in the transmission electron microscope, clustered around the (n,m) indices (7,6), (8,6), (8,7), and (9,6), with up to 70% of tubes having chiral angles over 20°. The mean diameter of SWCNTs was reduced from 1.10 to 1.04 nm by decreasing the growth temperature from 880 to 750 °C, which simultaneously increased the fraction of semiconducting tubes from 67% to 80%. Limiting the nanotube gas phase number concentration to ∼105 cm−3 prevented nanotube bundle formation that is due to collisions induced by Brownian diffusion. Up to 80% of 500 as-deposited tubes observed by atomic force and transmission electron microscopy were individual. Transparent conducting films deposited from these SWCNTs exhibited record low sheet resistances of 63 Ω/□ at 90% transparency for 550 nm light.

We use noninvasive atomic force microscopy to probe the spatial electrical conductivity of isolated junctions of pristine and nitric acid treated single-walled carbon nanotube networks (SWCNT-N). By analyzing the local IV curves of SWCNTs and bundles with various diameters, the resistance per unit length and the contact resistance of their junctions are estimated to be 3–16 kΩ/μm and 29–532 kΩ, respectively. We find that the contact resistance decreases with increasing SWCNT or bundle diameter and depends on the contact morphology, reaching a value of 29 kΩ at a diameter of 10 nm. A nitric acid treatment moderately dopes SWCNTs and reduces their average contact resistance by a factor of 3 while the resistance of the nanotubes remains largely unaltered. Remarkably, the same treatment on an SWCNT-N shows similar reduction in the sheet resistance by a factor of 4. These results suggest that the resistance reduction mechanism is related to the contact modulation with no major impact on conductance of SWCNTs.

In floating catalyst chemical vapor deposition (FC-CVD), tuning chirality distribution and obtaining narrow chirality distribution of single-walled carbon nanotubes (SWCNTs) is challenging. Herein, by introducing various amount of CO2 in FC-CVD using CO as a carbon source, we have succeeded in directly synthesizing SWCNT films with tunable chirality distribution as well as tunable colors. In particular, with 0.25 and 0.37 volume percent of CO2, the SWCNT films display green and brown colors, respectively. We ascribed various colors to suitable diameter and narrow chirality distribution of SWCNTs. Additionally, by optimizing reactor temperature, we achieved much narrower (n,m) distribution clustered around (11,9) with extremely narrow diameter range (>98% between 1.2 and 1.5 nm). We propose that CO2 may affect CO disproportionation and nucleation modes of SWCNTs, resulting in SWCNTs’ various diameter ranges. Our work could provide a new route for high-yield and direct synthesis of SWCNTs with narrow chirality distribution and offer potential applications in electronics, such as touch sensors or transistors.

We have developed the floating catalyst chemical vapor deposition (FCCVD) synthesis of single walled carbon nanotubes (SWCNTs) using C2H4 hydrocarbon as a carbon source and iron nanoparticles as the catalyst in an environmentally friendly and economical process. For the first time, ethylene was used as the only carbon source in FCCVD with N2 as the main carrier gas. No sulphur and less than 15% H2 in a N2 carrier gas were used. By varying the ferrocene concentration, the diameter of the SWCNTs was tuned in the range of 1.3-1.5 nm with the optimized control of ferrocene concentration. The process produced SWCNTs with an average length of 13 μm and with a low level of bundling, that is a high proportion (28%) of individual tubes. The electron diffraction (ED) pattern indicated a random chirality distribution of the tubes between armchair and zigzag structures. The ED analysis also revealed that 35-38% of tubes are metallic. As a result of having long SWCNTs with a low level of bundling and a high fraction of metallic tubes, we produced a highly conductive transparent film with a sheet resistance of 51 Ohm per sq. for 90% transmission at 550 nm after HNO3 treatment, this being one of the lowest sheet resistance values reported for SWCNT thin films.

The ultimate performance -ratio of electrical conductivity to optical absorbance -of singlewalled carbon nanotube (SWCNTs) transparent conductive films (TCFs) is an issue of considerable application relevance. Here, we present direct experimental evidence that SWCNT bundling is detrimental for their performance. We combine floating catalyst synthesis of non-bundled, high-quality SWCNTs with an aggregation chamber, in which bundles with mean diameters ranging from 1.38 to 2.90 nm are formed from identical 3 m long SWCNTs. The as-deposited TCFs from 1.38 nm bundles showed sheet resistances of 310 Ω/☐ at 90% transparency, while those from larger bundles of 1.80 and 2.90 nm only reached values of 475 and 670 Ω/☐, respectively. Based on these observations, we elucidate how networks formed by smaller bundles perform better due to their greater interconnectivity at a given optical density. Finally, we present a semi-empirical model for TCF performance as a function of SWCNT mean length and bundle diameter. This gives an estimate for the ultimate performance of non-doped, random network mixed-metallicity SWCNT TCFs at ~80 Ω/☐ and 90% transparency.