Single-wall carbon nanotubes (SWCNTs) are considered ideal electronic and photoelectronic materials in the post-Moore era due to their extremely high carrier mobility, structure-tunable bandgap and nanoscale body [1-2]. However, a slight difference in atomic arrangement between different SWCNTs induces large changes in their optical and electrical properties. Industrial production of single-chirality carbon nanotubes is critical for their applications in high-speed and low-power nanoelectronic devices [2]. In the past, intense efforts have been made to obtain chirality-enriched SWCNTs on a large scale [3, 4], but both their growth and separation have been major challenges.

Most recently, Prof. Huaping Liu's research group from the Institute of Physics (IOP) of the Chinese Academy of Sciences (CAS) reported a simple, yet effective, method to increase the yield of gel chromatography separation of single-chirality carbon nanotubes by enabling significantly higher concentrations of raw nanotubes solution. With this technique, milligram-scale separation of multiple single-chirality SWCNTs have been achieved. This study was mostly recently published in Nature Communications (Preparing high-concentration individualized carbon nanotubes for industrial separation of multiple single-chirality species, Nature Communications, 2023, 14:2491).

The preparation of monodisperse raw SWCNT solution is a critical step in the separation of single-chirality SWCNTs that determines the structural purity of the separated SWCNTs [5]. However, high concentration and high dispersity are difficult to reconcile, which limits the separation efficiency of single-chirality SWCNTs. Huaping Liu and his colleagues developed a strategy for dispersing a highly concentrated individualized SWCNT solution by redispersion, in which the SWCNT solution was first ultrasonically dispersed, followed by ultracentrifugation and reultrasonic dispersion. With this technique, the dispersible initial concentration of SWCNTs increased from 1 to 8 mg/mL, and the corresponding concentration of the resulting individualized SWCNT solution increased from 0.19 to ~1.02 mg/mL. And the separation yields of multiple single-chirality species, including (6, 4), (6, 5), (11, 1), (7, 5), (7, 6), (8, 3), (8, 4) and (9, 1), were increased by approximately six times to the milligram scale in one separation run with gel chromatography.

This dispersion technique was shown to be applicable for the low-cost and commercial hybrid of graphene and SWCNTs (G-SWCNTs) with a wide diameter range of 0.8-2.0 nm. By increasing the initial dispersible concentration of the G-SWCNT raw materials from the typical 1 to 4 mg/mL, the separation yield of single-chirality SWCNTs was increased by more than one order of magnitude. In particular, nine types of single-chirality SWCNTs, namely, (6, 4), (6, 5), (7, 3), (7, 5), (7, 6), (8, 4), (9, 1), (9, 4) and (10, 3), were prepared on the submilligram scale.

The distinct improvement in the separation yield of SWCNTs by increasing the concentration of SWCNT solution is mainly ascribed to the enhanced transfer of SWCNTs from bulk solution to the gel surface and thus their adsorption onto gel, which reduces the proportions of unadsorbed and irreversibly adsorbed SWCNTs. By life techno-economic and life cycle assessments, the mass separation of single-chirality species showed distinct advantages in efficiency, energy consumption and cost compared with the previous methods by increasing the concentration of SWCNTs. This dispersion and separation strategy provide a method for the industrial separation of single-chirality SWCNTs over a wide diameter range.

References

1. Dresselhaus, M. S.; Dresselhaus, G.; Eklund, P. C. Science of Fullerenes and Carbon Nanotubes: Their Properties and Applications. Academic Press, Inc.: New York, 1996.
2. Gaviria Rojas, W. A.; Hersam M. C. Chirality-enriched carbon nanotubes for next-generation computing. Adv. Mater. 2020, 1905654.
3. Wei, X.; Li, S.; Wang, W.; Zhang, X.; Zhou, W.; Xie, S.; Liu, H. Recent advances in structure separation of single-wall carbon nanotubes and their application in optics, electronics, and optoelectronics. Adv. Sci. 2022 9, 220054.
4. Yang, D.; Li, H.; Wei, X.; Wang, Y.; Zhou, W.; Kataura, H.; Xie, S.; Liu, H. Submilligram-scale separation of near-zigzag single-chirality carbon nanotubes by temperature controlling a binary surfactant system. Sci. Adv. 2021, 7, eabe0084.
5. Hersam M. C. Progress towards monodisperse single-walled carbon nanotubes. Nature Nanotechnology 3, 2008, 387-394.