The unique electrical properties of carbon nanotubes (CNTs) are highly desired in many technological applications. Unfortunately, in practice, the electrical conductivity of most CNTs and their assemblies has fallen short of expectations. One reason for this poor performance is that electrical resistance develops at the interface between carbon nanomaterials and metal surfaces when traditional metal-metal type contacts are employed. Here, a method for overcoming this resistance using covalent bond formation between open-ended CNTs and Cu surfaces is investigated experimentally and supported by theoretical calculations. The open-ended CNTs are vertically oriented compared to the substrate and have carboxylic functional groups that react with aminophenyl groups (linkers) grafted on metal surfaces. The covalent bond formation, crosslinking carboxylic and amine, via amide bond formation occurs at 120 °C. The covalent bonding nature of the aminophenyl linker is demonstrated theoretically using (100), (110), and (111) Cu surfaces, and bridge-like bond formation between carbon and two adjacent Cu atoms is revealed. The electrical conductivity calculated for a single intramolecular-type junction supports covalent bond formation between Cu and CNTs. Experimentally, the robustness of the covalent bonding between vertically oriented CNTs is tested by exposing CNTs on Cu to sonication, which reveals that CNTs remain fixed to the Cu supports. Since bonding CNTs to metals was performed at low temperatures, the reported method of covalent bond formation is expected to facilitate the application of CNTs in multiple fields, including electronics.
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