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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Hydrogen-bonded metallo-supramolecular polymers based on ruthenium or iron complexes for the selective extraction of single-walled carbon nanotubes
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Hydrogen-bonded metallo-supramolecular polymers based on ruthenium or iron complexes for the selective extraction of single-walled carbon nanotubes

机译：基于钌或铁络合物的氢键金属 - 超分子聚合物，用于选择性萃取单壁碳纳米管

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The chemical functionalization of nano-carbon materials such as single-walled carbon nanotubes (SWNTs) and graphene by metal complexes has attracted much attention due to the multitude of potential applications in efficient energy-conversion and -storage devices. The solubilization and single-chirality separation of SWNTs by surface modifications is a useful approach to manipulate SWNTs in the liquid phase. In this study, several Ru and Fe complexes containing two terminal quadruple hydrogen-bonded (H-bonded) ureidopyrimidinedione (UPy) groups were synthesized (Ru-1, Ru-UPy, and Fe-UPy) to form H-bonded supramolecular polymers by self-association. In order to control the solubility of these complexes in nonpolar solvents, Ru-UPy and Fe-UPy were endowed with long alkyl side chain groups in the coordinated 2,6-bis(benzimidazol-2-yl) pyridine ligand, while Ru-1 and Ru-2 do not contain such long alkyl chain groups. AFM measurements revealed that Ru-1, Ru-UPy, and Fe-UPy form a fiber-like network morphology on HOPG surfaces, arising from the H-bonded aggregation. However, only Ru-UPy and Fe-UPy are able to solubilize SWNTs effectively upon simple sonication in chlorobenzene. After the solubilization of a CoMoCAT (R) SWNT in chlorobenzene using Ru-UPy or Fe-UPy, UV-Vis-NIR spectra showed sharp peaks at 996 and 1150 nm, which were attributed to (6, 5) and (7, 6)-SWNTs. The Raman spectra of the solubilized SWNTs revealed peaks that were attributed to the radial breathing mode (RBM), which suggests an enrichment of semiconducting SWNTs, i. e., Ru-UPy and Fe-UPy are able to selectively solubilize semiconducting SWNTs. Cyclic voltammograms of films of SWNTs covered with Ru-UPy or Fe-UPy on ITO electrodes showed a well-defined adsorbed Ru(II/III) or Fe(II/III) wave. Upon addition of acid, the redox response from the adsorbed H-bonded Ru-UPy and Fe-UPy disappeared and only SWNTs were left on the ITO electrode. Moreover, the Ru-UPy/SWNT and Fe-UPy/SWNT hybrids exhibited non-linear I-V characteristics.
机译：由于在有效的能量转换和-Storage装置中，金属配合物的纳米碳材料如单壁碳纳米管（SWNT）和石墨烯的纳米碳材料和石墨烯的化学官能化引起了很多潜在应用。通过表面修饰的SWNT的溶解和单手性分离是一种有用的方法来操纵液相中的SWNT。在该研究中，合成了含有两个末端四氢键合（H键合）ureidopyOpylimidoIche（Umy）基团的几种Ru和Fe络合物（Ru-1，Ru-Upy和Fe-Upy），通过自我关联。为了控制这些配合物在非极性溶剂中的溶解性，Ru-Upy和Fe-Upy在配位的2,6-双（Benzimidazol-2-基）吡啶配体中赋予长的烷基侧链基团，而RU-1并且Ru-2不含这种长的烷基链基团。 AFM测量显示Ru-1，Ru-Upy和Fe-Upy在跳跃表面上形成纤维样网络形态，由H键合的聚集产生。然而，只有Ru-Upy和Fe-Upy能够在氯苯中简单的超声处理时有效地溶解漩涡。在使用Ru-Upy或Fe-Upy的氯苯中溶解氯苯（R）SWNT后，UV-Vis-Nir光谱在996和1150nm处显示出尖锐的峰，其归因于（6,5）和（7,6 - ）。溶解的SWNT的拉曼光谱显示出归因于径向呼吸模式（RBM）的峰，这表明富集半导体SWNT，I。即，Ru-Upy和Fe-Upy能够选择性地溶解半导体SWNT。 ITO电极上覆盖的Ru-Upy或Fe-Upy覆盖的SWNT薄膜的循环伏安图显示了明确定义的吸附Ru（II / III）或Fe（II / III）波。加入酸后，来自吸附的H键合Ru-Upy和Fe-Upy的氧化还原反应消失，并且仅在ITO电极上留下SWNT。此外，Ru-Upy / SWNT和Fe-Upy / SWNT杂种呈非线性I-V特性。

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