Selective Breakdown of Metallic Pathways in Double‐Walled Carbon Nanotube Networks

Covalently functionalized, semiconducting double‐walled carbon nanotubes exhibit remarkable properties and can outperform their single‐walled carbon nanotube counterparts. In order to harness their potential for electronic applications, metallic double‐walled carbon nanotubes must be separated from the semiconductors. However, the inner wall is inaccessible to current separation techniques which rely on the surface properties. Here, the first approach to address this challenge through electrical breakdown of metallic double‐walled carbon nanotubes, both inner and outer walls, within networks of mixed electronic types is described. The intact semiconductors demonstrate a ∼62% retention of the ON‐state conductance in thin film transistors in response to covalent functionalization. The selective elimination of the metallic pathways improves the ON/OFF ratio, by more than 360 times, to as high as 40 700, while simultaneously retaining high ON‐state conductance.