论文标题
通过浮动催化剂通过原位测量和热力学计算合理地合成SIC纳米线网的超快合成
Ultrafast synthesis of SiC nanowire webs by floating catalysts rationalised through in-situ measurements and thermodynamic calculations
论文作者
论文摘要
这项工作表明,使用催化剂纳米颗粒的气溶胶,通过蒸气液(VLS)机制浮在气流中的SIC纳米线的合成。这些条件在8.5μm/s(最大为50μm/s)时导致超快生长,高于常规底物的化学蒸气沉积高达3个数量级。纳米线的高纵横比(高达2200)有利于它们的纠缠和完全由SICNW组成的独立网络材料的形成。浮动催化剂化学蒸气沉积生长过程通过反应产物的原位采样和来自气相的催化剂气溶胶的原位采样,以及批量三元SI-C-FE相图的热力学计算。该相图提出了对SICNW选择性生长的机械路径的描述,这与观察到没有其他类型的纳米线(SI或C)的观察结果一致。 SICNW的生长发生在1130°C,接近计算出的共晶。根据计算出的相图,添加Si和C后,富含Fe的液体将碳壳分离,然后在Si中富集液体会导致SIC的形成。相对于基于底物的过程的异常快速增长率归因于由于这种新合成模式固有的高碰撞速率,因此将前体的可用性增加了。
This work presents the synthesis of SiC nanowires floating in a gas stream through the vapour-liquid-solid (VLS) mechanism using an aerosol of catalyst nanoparticles. These conditions lead to ultrafast growth at 8.5 μm/s (maximum of 50 μm/s), which is up to 3 orders of magnitude above conventional substrate-based chemical vapour deposition. The high aspect ratio of the nanowires (up to 2200) favours their entanglement and the formation of freestanding network materials consisting entirely of SiCNWs. The floating catalyst chemical vapour deposition growth process is rationalised through in-situ sampling of reaction products and catalyst aerosol from the gas phase, and thermodynamic calculations of the bulk ternary Si-C-Fe phase diagram. The phase diagram suggests a description of the mechanistic path for the selective growth of SiCNWs, consistent with the observation that no other types of nanowires (Si or C) are grown by the catalyst. SiCNW growth occurs at 1130 °C, close to the calculated eutectic. According to the calculated phase diagram, upon addition of Si and C, the Fe-rich liquid segregates a carbon shell, and later enrichment of the liquid in Si leads to the formation of SiC. The exceptionally fast growth rate relative to substrate-based processes is attributed to the increased availability of precursors for incorporation into the catalyst due to the high collision rate inherent to this new synthesis mode.