Continuous intercalation compound fibers of bromine wires and aligned CNTs for high-performance conductors

This work presents macroscopic fibers of aligned double-walled carbon nanotubes (DWCNTs) intercalated with long-range ordered bromine, with a stoichiometry close to C17Br. Tribromide ions lie inside interstitial sites between hexagonally-packed DWCNTs and extend parallel to their axis as ordered supramolecular “wires”. First-principles simulations confirm this structure and a transfer of 0.13 electrons per Br atom. The structure of nested bundles of CNTs with a homogeneous distribution of bromine species in the interstitial sites of the superlattice is directly imaged by cross-sectional HRTEM, showing full intercalation of highly dense and aligned fibers. The presence of Br2 and Br3– is confirmed by Raman spectroscopy, and their supramolecular organization is resolved by 2D wide-angle X-ray scattering. Intercalation increases room-temperature longitudinal electrical conductivity by a factor of 8.4. Through low-temperature transport measurements in the longitudinal and transverse directions, we show that the intercalate reduces the tunneling-dominated resistance associated with transport between adjacent CNTs, rather than exclusively acting as a dopant that increases conductance of individual CNTs. By preserving the separation between CNTs, the exceptional mechanical properties of the CNT fiber host are retained. The combined tensile strength above 2.46 GPa and conductivity of 10.68 MS/m makes intercalated CNT fibers attractive lightweight conductors with combined properties superior to metals and graphite intercalation compounds.