Journal
ACS NANO
Volume 12, Issue 1, Pages 884-893Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.7b08708
Keywords
boron nitride nanotubes; scalable manufacturing; hydrogen-catalyzed; induction thermal plasma; thermofluid simulation; optical emission spectroscopy; density functional theory
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Funding
- NRC-Security Materials Technology Program
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We recently demonstrated scalable manufacturing of boron nitride nanotubes (BNNTs) directly from hexagonal BN (hBN) powder by using induction thermal plasma, with a high-yield rate approaching 20 g/h. The main finding was that the presence of hydrogen is crucial for the high yield growth of BNNTs. Here we investigate the detailed role of hydrogen by numerical modeling and in situ optical emission spectroscopy (OES) and reveal that both the thermofluidic fields and chemical pathways are significantly altered by hydrogen in favor of rapid growth of BNNTs. The numerical simulation indicated improved particle heating and quenching rates (similar to 10(5) K/s) due to the high thermal conductivity of hydrogen over the temperature range of 3500-4000 K. These are crucial for the complete vaporization of the hBN feedstock and rapid formation of nanosized B droplets for the subsequent BNNT growth. Hydrogen is also found to extend the active BNNT growth zone toward the reactor downstream, maintaining the gas temperature above the B solidification limit (similar to 2300 K) by releasing the recombination heat of H atoms, which starts at 3800 K. The OES study revealed that H radicals also stabilize B or N radicals from dissociation of the feedstock as BH and NH radicals while suppressing the formation of N-2 or N-2(+) species. Our density functional theory calculations showed that such radicals can provide faster chemical pathways for the formation of BN compared with relatively inert N-2.
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