Li Han, Gordeev Georgy, Garrity Oisin, Peyyety Naga Anirudh, Selvasundaram Pranauv Balaji, Dehm Simone, Krupke Ralph, Cambré Sofie, Wenseleers Wim, Reich Stephanie, Zheng Ming, Fagan Jeffrey A, Flavel Benjamin S
Institute of Nanotechnology , Karlsruhe Institute of Technology , Karlsruhe 76021 , Germany.
Department of Physics , Freie Universität Berlin , Berlin 14195 , Germany.
ACS Nano. 2020 Jan 28;14(1):948-963. doi: 10.1021/acsnano.9b08244. Epub 2020 Jan 14.
The enantiomer-level isolation of single-walled carbon nanotubes (SWCNTs) in high concentration and with high purity for nanotubes greater than 1.1 nm in diameter is demonstrated using a two-stage aqueous two-phase extraction (ATPE) technique. In total, five different nanotube species of ∼1.41 nm diameter are isolated, including both metallics and semiconductors. We characterize these populations by absorbance spectroscopy, circular dichroism spectroscopy, resonance Raman spectroscopy, and photoluminescence mapping, revealing and substantiating mod-dependent optical dependencies. Using knowledge of the competitive adsorption of surfactants to the SWCNTs that controls partitioning within the ATPE separation, we describe an advanced acid addition methodology that enables the fine control of the separation of these select nanotubes. Furthermore, we show that endohedral filling is a previously unrecognized but important factor to ensure a homogeneous starting material and further enhance the separation yield, with the best results for alkane-filled SWCNTs, followed by empty SWCNTs, with the intrinsic inhomogeneity of water-filled SWCNTs causing them to be worse for separations. Lastly, we demonstrate the potential use of these nanotubes in field-effect transistors.
使用两阶段水相双相萃取(ATPE)技术,展示了对直径大于1.1 nm的单壁碳纳米管(SWCNT)进行高浓度、高纯度的对映体水平分离。总共分离出了五种直径约为1.41 nm的不同纳米管种类,包括金属型和半导体型。我们通过吸收光谱、圆二色光谱、共振拉曼光谱和光致发光映射对这些群体进行表征,揭示并证实了与模式相关的光学依赖性。利用表面活性剂对SWCNT的竞争吸附知识来控制ATPE分离中的分配,我们描述了一种先进的酸添加方法,该方法能够精细控制这些特定纳米管的分离。此外,我们表明内包填充是一个以前未被认识到但很重要的因素,可确保起始材料均匀并进一步提高分离产率,对于烷烃填充的SWCNT效果最佳,其次是空的SWCNT,而水填充的SWCNT的固有不均匀性使其在分离方面表现较差。最后,我们展示了这些纳米管在场效应晶体管中的潜在用途。