The high-temperature plasma process has demonstrated great potential in growing high-quality boron nitride nanotubes (BNNTs) with small diameters (∼5 nm) and few walls (3-4 walls) and led to successful commercialization with a high production rate approaching 20 g/h. However, the process is still accompanied by the production of BN impurities (e.g., a-BN, BN shell, BN flakes) whose physicochemical properties are similar to those of BNNTs. This renders the post-purification process very challenging and thus hampers the development of their practical applications. In this study, we have employed both experimental and numerical approaches for a mechanistic understanding of BN impurity formation in the high-temperature plasma process. This study suggests that the flow structure of the plasma jet (e.g., laminar or turbulent) plays a key role in the formation of BN impurities by dictating the transport phenomena of BNNT seeds (e.g., B droplets), which play an important role in BNNT nucleation. We discussed that the turbulence enhances the radial diffusion of B droplets as well as their interparticle coagulation, which leads to a significant reduction in the population of effective BNNT seeds in the BNNT growth zone (T < 4000 K). This results in the generation of unreacted BN precursors (e.g., B-N-H species) in the BNNT growth zone that eventually self-assemble into BN impurities. Our numerical simulation also suggests that a higher thermal energy input makes the flow more turbulent in the BNNT growth zone due to the elevated velocity difference between the plasma jet and ambient cold gas. This finding provides critical insight into the process design that can suppress the BN impurity formation in the high-temperature plasma process.
© 2021 The Authors. Published by American Chemical Society.