Tsuji Takashi, Kim Jaeho, Sakakita Hajime, Shimizu Yoshiki, Chen Guohai, Hata Kenji, Futaba Don N, Sakurai Shunsuke
CNT-Application Research Center, National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba Central 5, 1-1-1 Higashi, Tsukuba, Ibaraki 305-8565, Japan.
Innovative Plasma Processing Group, Research Institute for Advanced Electronics and Photonics, National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba Central 2, 1-1-1 Umezono, Tsukuba, Ibaraki 305-8568, Japan.
ACS Omega. 2021 Jul 14;6(29):18763-18769. doi: 10.1021/acsomega.1c01822. eCollection 2021 Jul 27.
The importance of hydrogen in carbon nanotube (CNT) synthesis has been known as it supports the critical processes necessary for CNT growth, such as catalyst reduction. However, within the scope of our mini microplasma CNT synthesis reactor, we found that hydrogen was critical for unexpected reasons. Without hydrogen, CNT growth was inhibited and characterized by amorphous carbon particles. Optical emission spectroscopy of the microplasma revealed that without hydrogen, the high-energy electrons induced the immediate decomposition of carbon feedstock simultaneously with the catalyst feedstock, thus suppressing the formation of catalyst nanoparticles and inducing catalyst deactivation. In contrast, the inclusion of hydrogen induced less-immediate decomposition of reactant gases, through the conversion of electron energy of the plasma to thermal energy, which provided the appropriate conditions for catalyst nanoparticle formation and subsequent CNT nucleation. A simple reaction pathway model was proposed to explain these observed results and underlying mechanisms.
氢在碳纳米管(CNT)合成中的重要性已为人所知,因为它支持CNT生长所需的关键过程,如催化剂还原。然而,在我们的微型微等离子体CNT合成反应器范围内,我们发现氢之所以至关重要,原因出人意料。没有氢,CNT生长受到抑制,其特征是出现无定形碳颗粒。微等离子体的发射光谱显示,没有氢时,高能电子会同时导致碳原料和催化剂原料立即分解,从而抑制催化剂纳米颗粒的形成并导致催化剂失活。相比之下,加入氢通过将等离子体的电子能量转化为热能,诱导反应气体不那么迅速地分解,这为催化剂纳米颗粒的形成和随后的CNT成核提供了合适的条件。我们提出了一个简单的反应途径模型来解释这些观察结果和潜在机制。