In-Situ Flame-Synthesized Carbon Nanomaterials via an Impinging Swirl Flow with an N-Butanol Pool

Abstract

ABSTRACT This study aims to investigate the impact of flow rotation and oxygen concentration on the synthesis of carbon nanomaterials using n-butanol diffusion flames in a rotating stagnation flow with a liquid pool and a catalytic Ni substrate. With increasing angular velocity (ω), the diffusion flame shifts slightly toward the upper oxidizer nozzle, experiences a lower strain rate, and becomes stronger with a higher maximum flame temperature at a fixed oxygen concentration (ΩO). Meanwhile, the soot layer thickens and gradually turns yellowish. Field Emission Scanning Electron Microscopy (FESEM) analyses confirm that carbon nanotubes (CNTs) can only be fabricated at ω = 2 or 3 rps when ΩO = 21%, highlighting the critical role of flow rotation. Interestingly, the optimal positions for CNT synthesis consistently occur at the same sampling position (1.5 mm below the upper edge of the blue flame) for all values of oxygen concentration (ΩO). The corresponding temperature ranges for ΩO = 19%, 18%, and 17% are approximately 950°C, 820–920°C, and 800–850°C, respectively, which align with existing literature. High-resolution transmission electron microscopy (HRTEM) images reveal both typical straight tubular and bamboo-like CNT structures. Raman spectra indicate superior graphitization at high angular velocities (ω). Notably, at ω = 0 rps, the intensity ratio of the D- and G-bands is greater than 1 (ID/IG >1); however, as ω increases, the opposite holds (ID/IG <1), with its value gradually decreasing. This suggests that the swirl effect enhances graphite layer crystallization. Importantly, the strain rate controlled by flow rotation significantly influences CNT fabrication, considering both residence time and carbon source. The key finding of this study is that swirl flow enhances both the quality and quantity of CNTs synthesized via n-butanol diffusion flames.