Department of Chemistry, Korea University, Jochiwon 339-700, Korea.
Phys Chem Chem Phys. 2014 Feb 14;16(6):2411-6. doi: 10.1039/c3cp54039a.
Graphitized nanodiamonds were conveniently prepared by the laser irradiation of colloidal solution using various solvents. The nanodiamonds were converted into a fully graphitized onion-like structure, which became a cage-like mesoporous structure by the degradation of graphitic layers. Alcohols, acetone, and acetonitrile are more efficient solvents for the graphitization compared to water and hydrocarbons. Therefore the number and morphology of the graphitic layers can be simply controlled by the solvent and laser-irradiation duration. We suggest a graphitization model, in which the photocatalytic oxidation of the solvent accelerates the graphitization of nanodiamonds. The graphitized nanodiamonds were easily doped with the nitrogen and sulfur atoms in a controlled manner. In particular, the spherical graphitic layers were preferentially doped with the pyrrolic nitrogen that enhances remarkably electrocatalytic activity for the oxygen reduction reaction.
通过使用各种溶剂对胶体溶液进行激光辐照,方便地制备了石墨化纳米金刚石。纳米金刚石被转化为完全石墨化的洋葱状结构,通过石墨层的降解,形成了笼状介孔结构。与水和碳氢化合物相比,醇、丙酮和乙腈是更有效的石墨化溶剂。因此,通过溶剂和激光辐照时间可以简单地控制石墨层的数量和形态。我们提出了一种石墨化模型,其中溶剂的光催化氧化加速了纳米金刚石的石墨化。石墨化纳米金刚石很容易以可控的方式掺杂氮和硫原子。特别是,球形石墨层优先掺杂吡咯氮,显著提高了氧还原反应的电催化活性。