Segura Rodrigo A, Hevia Samuel, Häberle Patricio
Departamento de Química y Bioquímica, Facultad de Ciencias, Universidad de Valparaíso, Valparaíso 2340000, Chile.
J Nanosci Nanotechnol. 2011 Nov;11(11):10036-46. doi: 10.1166/jnn.2011.4998.
Carbon nanostructures were synthesized by decomposition of different carbon sources over an alumina supported palladium catalyst via Chemical Vapor Deposition (CVD). Several experimental conditions were varied to verify their influence in the synthesis products: temperature ramping rate, pre-annealing conditions, hydrogen pre-treatment, synthesis temperature and time, together with the use of different carbon sources. Depending on the experimental conditions carbon nanotubes and nanofibers with different shapes and structural characteristics were obtained. Straight, coiled and branched morphologies are the most common. Among our findings, the addition of hydrogen plays a significant role in the structure of the carbonaceous products. For example, the decomposition of acetylene on palladium catalysts at 800 degrees C in the absence of hydrogen produces only carbon micro- spheres as synthesis products. The incorporation of increasing amounts of hydrogen modifies the outcome, from thick fibers to carbon nanotubes. To verify the level of graphitization of the synthesis products we have used high resolution transmission electron microscopy (HRTEM) in addition to Raman spectroscopy. Our results, based on these complementary techniques, indicate the decomposition of acetylene on a palladium based catalyst, produces the best degree of graphitization in carbon nanotubes for a temperature of 800 degrees C and 100 cc/min of hydrogen flow. Similar hydrogen flows on the same catalyst, produced highly graphitized nanofibers by the decomposition of methane at 850 degrees C.
通过化学气相沉积(CVD)法,在氧化铝负载的钯催化剂上分解不同的碳源来合成碳纳米结构。改变了几个实验条件以验证它们对合成产物的影响:升温速率、预退火条件、氢气预处理、合成温度和时间,以及使用不同的碳源。根据实验条件,获得了具有不同形状和结构特征的碳纳米管和纳米纤维。直的、卷曲的和分支的形态最为常见。在我们的研究结果中,氢气的添加对含碳产物的结构起着重要作用。例如,在800℃下,乙炔在钯催化剂上分解,在没有氢气的情况下,仅产生碳微球作为合成产物。增加氢气的加入量会改变产物,从粗纤维变为碳纳米管。为了验证合成产物的石墨化程度,除了拉曼光谱外,我们还使用了高分辨率透射电子显微镜(HRTEM)。基于这些互补技术的结果表明,在800℃和100 cc/min氢气流的条件下,乙炔在钯基催化剂上分解,可在碳纳米管中产生最佳程度的石墨化。在相同催化剂上,类似的氢气流在850℃下通过甲烷分解产生了高度石墨化的纳米纤维。