Selective Surface Charge Sign Reversal on Metallic Carbon Nanotubes for Facile Ultrahigh Purity Nanotube Sorting

Semiconducting (semi-) single-walled carbon nanotubes (SWNTs) must be purified of their metallic (met-) counterparts for most applications including nanoelectronics, solar cells, chemical sensors, and artificial skins. Previous bulk sorting techniques are based on subtle contrasts between properties of different nanotube/dispersing agent complexes. We report here a method which directly exploits the nanotube band structure differences. For the heterogeneous redox reaction of SWNTs with oxygen/water couple, the aqueous pH can be tuned so that the redox kinetics is determined by the availability of nanotube electrons only at/near the Fermi level, as predicted quantitatively by the Marcus–Gerischer (MG) theory. Consequently, met-SWNTs oxidize much faster than semi-SWNTs and only met-SWNTs selectively reverse the sign of their measured surface zeta potential from negative to positive at the optimized acidic pH when suspended with nonionic surfactants. By passing the redox-reacted nanotubes through anionic hyd...