High‐Yield Aerosol CVD Synthesis of High‐Quality Single‐Walled Carbon Nanotubes via Control of Nanotube Structure

ABSTRACT Aerosol chemical vapor deposition (CVD), a variant of floating catalyst CVD, enables one‐step, solvent‐free, and scalable production of high‐quality single‐walled carbon nanotube (SWCNT) films for next‐generation electronics, photonics, and optoelectronics. However, simultaneously achieving high production yield and superior film conductivity remains an unsolved challenge, as conventional approaches to boost yield inevitably promote nanotube bundling and degrade performance. Here, the mechanistic origin of this yield‐performance trade‐off is investigated through precise control of nanotube structural parameters during synthesis. Systematic investigation identifies nanotube diameter as the most influential structural parameter for balancing production yield and film conductivity within the broad parameter space explored: large‐diameter SWCNTs not only form lower‐resistance junctions but also tend to suppress bundling during aerosol‐state growth, thereby indirectly enhancing film conductivity while simultaneously facilitating higher yield. Bundle length and crystallinity also contribute positively, although their influence is less pronounced. Consequently, SWCNT‐predominant films (>55%) comprising large‐diameter nanotubes (∼2.4 nm) are synthesized, achieving an unprecedented yield‐to‐sheet‐resistance ratio at 90% transparency of 4.7 mm 2 L −1 (Ω □ −1 ) −1 after doping—an order of magnitude higher than previously reported values for SWCNT films. This work establishes fundamental structure‐property‐yield relationships and provides a rational design strategy for scalable production of high‐performance SWCNT films.