School of Chemical and Biomedical Engineering, Nanyang Technological University, Singapore 637459.
J Am Chem Soc. 2010 Dec 1;132(47):16747-9. doi: 10.1021/ja106937y. Epub 2010 Nov 4.
Selective synthesis of single walled carbon nanotubes (SWCNTs) with specific (n,m) structures is desired for many potential applications. Current chirality control growth has only achieved at small diameter (6,5) and (7,5) nanotubes. Each (n,m) species is a distinct molecule with structure-dependent properties; therefore it is essential to extend chirality control to various (n,m) species. In this communication, we demonstrate the highly selective synthesis of (9,8) nanotubes on a cobalt incorporated TUD-1 catalyst are (Co-TUD-1). When catalysts were prereduced in H(2) at the optimized temperature of 500 °C, 59.1% of semiconducting nanotubes have the (9,8) structure. The uniqueness of Co-TUD-1 relies on its low reduction temperature (483 °C), large surface area, and strong metal-support interaction, which stabilizes Co clusters responsible for the growth of (9,8) nanotubes. SWCNT thin film field effect transistors fabricated using (9,8) nanotubes from our synthesis process have higher average device mobility and a higher fraction of semiconducting devices than those using (6,5) nanotubes. Combining with further postsynthetic sorting techniques, our selective synthesis method brings us closer to the ultimate goal of producing (n,m) specific nanotube materials.
对于许多潜在的应用来说,具有特定(n,m)结构的单壁碳纳米管(SWCNTs)的选择性合成是很有必要的。目前的手性控制生长仅在小直径(6,5)和(7,5)纳米管上实现。每个(n,m)物种都是具有结构依赖性的特性的独特分子;因此,将手性控制扩展到各种(n,m)物种是至关重要的。在本通讯中,我们展示了在钴掺入的 TUD-1 催化剂(Co-TUD-1)上高度选择性地合成(9,8)纳米管。当催化剂在优化温度 500°C 的 H(2)中预还原时,有 59.1%的半导体纳米管具有(9,8)结构。Co-TUD-1 的独特之处在于其还原温度低(483°C)、比表面积大以及金属-载体相互作用强,这些特性稳定了负责生长(9,8)纳米管的 Co 簇。使用我们的合成工艺从(9,8)纳米管制备的 SWCNT 薄膜场效应晶体管具有比使用(6,5)纳米管更高的平均器件迁移率和更高比例的半导体器件。结合进一步的后合成分类技术,我们的选择性合成方法使我们更接近生产(n,m)特定纳米管材料的最终目标。