Zhu Anquan, Yang Xusheng, Zhang Lei, Wang Kun, Liu Tianhui, Zhao Xin, Zhang Luyao, Wang Lei, Yang Feng
Department of Chemistry, Guangdong Provincial Key Laboratory of Catalytic Chemistry, Southern University of Science and Technology, Shenzhen, 518055, China.
Nanoscale. 2022 Jan 20;14(3):953-961. doi: 10.1039/d1nr04019g.
The selective separation of soluble and individual single-walled carbon nanotubes (SWCNTs) in aqueous solution is a key step for harnessing the extraordinary properties of these materials. Manipulating the strong van der Waals intertube interactions between the SWCNT bundles is very important in selective separation, which is a long-standing challenge. Here we reported the ability of redox polyoxometalate clusters to modulate the intertube π-π stacking interaction through electron transfer and achieved the diameter-selective separation of SWCNTs in a surfactant aqueous solution. The large-diameter SWCNTs concentrated at ∼1.3-1.4 nm were selectively separated when ∼1 nm clusters encapsulated within the tube cavity, and the dispersion of subnanometer ∼0.7-0.9 nm SWCNTs was boosted when clusters were adsorbed on the outer surface of small-diameter nanotubes. The mechanism of diameter-selective separation of SWCNTs associated with the size-dependent interaction between cluster-tubes and the steric hindrance effect of clusters was revealed by optical absorption and Raman spectroscopy. This simple method thus enables the selective separation of individual high-quality SWCNTs in aqueous solutions without harsh sonication with the potential for other separation applications.
在水溶液中选择性分离可溶性和单个单壁碳纳米管(SWCNT)是利用这些材料非凡特性的关键步骤。控制SWCNT管束之间强大的范德华管间相互作用在选择性分离中非常重要,这是一个长期存在的挑战。在此,我们报道了氧化还原多金属氧酸盐簇通过电子转移调节管间π-π堆积相互作用的能力,并在表面活性剂水溶液中实现了SWCNT的直径选择性分离。当直径约1nm的簇包封在管腔内时,直径集中在约1.3 - 1.4nm的大直径SWCNT被选择性分离;当簇吸附在小直径纳米管的外表面时,亚纳米级约0.7 - 0.9nm的SWCNT的分散性得到增强。通过光吸收和拉曼光谱揭示了与簇 - 管之间尺寸依赖性相互作用以及簇的空间位阻效应相关的SWCNT直径选择性分离机制。因此,这种简单方法能够在不进行苛刻超声处理的情况下在水溶液中选择性分离单个高质量SWCNT,并具有用于其他分离应用的潜力。