Unzipping Carbon Nanotube Bundles through NH-π Stacking for Enhanced Electrical and Thermal Transport

Bundling of single-walled carbon nanotubes (SWCNTs) significantly undermines their superior thermal and electrical properties. Realizing stable, homogeneous, and surfactant-free dispersion of SWCNTs in solvents and composites has long been regarded as a key challenge. Here, we report amine-containing aromatic and cyclohexane molecules, which are common chain extenders (CEs) for epoxy curing in industry, can be used to effectively disperse CNTs. We achieve single-tube-level dispersion of SWCNTs in CE solvents, as demonstrated by the strong chirality-dependent absorption and photoluminescence emission. The SWCNT-CE dispersion remains stable under ambient conditions for months. The excellent dispersibility and stability are attributed to the formation of an n-type charge-transfer complex through the NH-π interaction between the amine group of CEs and the delocalized π bond of SWCNTs, which is confirmed by the negative Seebeck coefficient of the CE-functionalized SWCNT films, the red shift of the G band in the Raman spectra, and the NH-π peak in X-ray photoelectron spectroscopy. The high dispersibility of CEs significantly improves the electrical and thermal transport of macroscale CNT assemblies. The sheet resistance of the CE-dispersed SWCNT thin films reaches 161 Ω sq^-1 at 80.8% optical transmittance after functional modification by HNO₃. Moreover, the CEs cross-link CNTs and epoxy molecules, forming a pathway for phonon transport in CNT/epoxy nanocomposites. The thermal conductivity of the CE-CNT-epoxy composite is enhanced by 1850% compared with the original epoxy, which is the highest enhancement reported to date for CNT/epoxy nanocomposites. The CE-based NH-π interaction provides a new paradigm for the effective and stable dispersion of SWCNTs in a facile and scalable process.