Lin Yuehe, Cui Xiaoli, Yen Clive, Wai Chien M
Pacific Northwest National Laboratory, 902 Battelle Boulevard, P.O. Box 999, Richland, Washington 99352, USA.
J Phys Chem B. 2005 Aug 4;109(30):14410-5. doi: 10.1021/jp0514675.
Carbon nanotube (CNT)-supported Pt nanoparticle catalysts have been synthesized in supercritical carbon dioxide (scCO(2)) using platinum(II) acetylacetonate as metal precursor. The structure of the catalysts has been characterized with transmission electron micrograph (TEM) and X-ray photoelectron spectroscopy (XPS). TEM images show that the platinum particles' size is in the range of 5-10 nm. XPS analysis indicates the presence of zero-valence platinum. The Pt-CNT exhibited high catalytic activity both for methanol oxidation and oxygen reduction reaction. The higher catalytic activity has been attributed to the large surface area of carbon nanotubes and the decrease in the overpotential for methanol oxidation and oxygen reduction reaction. Cyclic voltammetric measurements at different scan rates showed that the oxygen reduction reaction at the Pt-CNT electrode is a diffusion-controlled process. Analysis of the electrode kinetics using Tafel plot suggests that Pt-CNT from scCO(2) provides a strong electrocatalytic activity for oxygen reduction reaction. For the methanol oxidation reaction, a high ratio of forward anodic peak current to reverse anodic peak current was observed at room temperature, which implies good oxidation of methanol to carbon dioxide on the Pt-CNT electrode. This work demonstrates that Pt-CNT nanocomposites synthesized in supercritical carbon dioxide are effective electrocatalysts for low-temperature fuel cells.
以乙酰丙酮铂(II)作为金属前驱体,在超临界二氧化碳(scCO₂)中合成了碳纳米管(CNT)负载的铂纳米颗粒催化剂。采用透射电子显微镜(TEM)和X射线光电子能谱(XPS)对催化剂的结构进行了表征。TEM图像显示铂颗粒尺寸在5 - 10 nm范围内。XPS分析表明存在零价铂。Pt-CNT对甲醇氧化和氧还原反应均表现出高催化活性。较高的催化活性归因于碳纳米管的大表面积以及甲醇氧化和氧还原反应过电位的降低。在不同扫描速率下进行的循环伏安测量表明,Pt-CNT电极上的氧还原反应是一个扩散控制过程。使用塔菲尔曲线对电极动力学进行分析表明,由scCO₂制备的Pt-CNT对氧还原反应具有很强的电催化活性。对于甲醇氧化反应,在室温下观察到正向阳极峰电流与反向阳极峰电流的高比值,这意味着在Pt-CNT电极上甲醇能很好地氧化为二氧化碳。这项工作表明,在超临界二氧化碳中合成的Pt-CNT纳米复合材料是低温燃料电池的有效电催化剂。