Departments of Chemistry, Computer Science, Mechanical Engineering and Materials Science, and the Smalley Institute for Nanoscale Science and Technology, Rice University, MS 222, 6100 Main Street, Houston, Texas 77005, USA.
ACS Nano. 2010 Jun 22;4(6):3095-102. doi: 10.1021/nn100306r.
Sheets of chemically converted graphene (CCG) on the surface of Si/SiO(2) substrates exhibit nanoscopic corrugation. This corrugation has been assumed to be caused by a combination of factors including (a) thermal treatments in the device preparation, (b) different oxygen-containing addends on the CCG, and (c) the substrate roughness. In this paper, we study the interplay of these factors in the corrugation behavior of monolayer CCG flakes, prepared by reduction of graphene oxide (GO) synthesized by Hummers method, and CCG nanoribbons, produced by chemical unzipping of carbon nanotubes, followed by the reduction by hydrazine at 95 degrees C. We have studied the morphology, composition, and electrical properties of the flakes and nanoribbons before and after annealing in Ar/H(2) at 300 degrees C. Our experiments demonstrate that, despite the temperature treatment and the associated removal of the oxygen-containing addends from the basal plane of the CCG, the corrugation pattern of the CCG exhibits almost no change upon annealing. This suggests that the substrate roughness, not the chemical addends nor the thermal cycling, is the predominant determinant in the graphene corrugation. This conclusion is supported by depositing GO flakes on freshly cleaved mica. Such flakes were shown to have extremely low corrugation (rms approximately 70 pm), as dictated by the atomically flat surface of mica. Our experimental observations are in accord with the results of our molecular dynamics simulations, which show that interaction with the substrate greatly suppresses the intrinsic corrugation of graphene materials.
在 Si/SiO2 衬底表面的化学转化石墨烯 (CCG) 片上表现出纳米级波纹。这种波纹被认为是由多种因素共同作用的结果,包括(a)器件制备过程中的热处理,(b)CCG 上不同含氧添加剂,以及(c)衬底粗糙度。在本文中,我们研究了这些因素在单层 CCG 薄片波纹行为中的相互作用,这些薄片是通过还原 Hummers 法合成的氧化石墨烯 (GO) 制备的,以及通过化学解缠的碳纳米管制备的 CCG 纳米带,然后通过肼在 95 度还原。我们研究了在 300 度的 Ar/H2 中退火前后薄片和纳米带的形貌、组成和电性能。我们的实验表明,尽管进行了温度处理以及与含氧添加剂从 CCG 的基面去除相关的处理,但 CCG 的波纹图案在退火后几乎没有变化。这表明基底粗糙度是 CCG 波纹的主要决定因素,而不是化学添加剂或热循环。这一结论得到了在新鲜剥离云母上沉积 GO 薄片的实验支持。事实证明,这些薄片的波纹非常低(均方根约 70pm),这是由云母原子级平坦的表面决定的。我们的实验观察结果与分子动力学模拟的结果一致,这些结果表明与基底的相互作用极大地抑制了石墨烯材料的固有波纹。