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钌联吡啶配合物负载富勒烯或碳纳米管:不同碳基配体对产物的影响。

Ruthenium-bipyridine complexes bearing fullerene or carbon nanotubes: synthesis and impact of different carbon-based ligands on the resulting products.

机构信息

State Key Lab for Physical Chemistry of Solid Surfaces, Department of Chemistry and College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, PR China.

出版信息

Dalton Trans. 2011 Sep 7;40(33):8353-60. doi: 10.1039/c1dt10417a. Epub 2011 Jul 18.

Abstract

This paper discusses the synthesis of two carbon-based pyridine ligands of fullerene pyrrolidine pyridine (C(60)-py) and multi-walled carbon nanotube pyrrolidine pyridine (MWCNT-py) via 1,3-dipolar cycloaddition. The two complexes, C(60)-Ru and MWCNT-Ru, were synthesized by ligand substitution in the presence of NH(4)PF(6), and Ru(II)(bpy)(2)Cl(2) was used as a reaction precursor. Both complexes were characterized by mass spectroscopy (MS), elemental analysis, nuclear magnetic resonance (NMR) spectroscopy, infrared spectroscopy (IR), ultraviolet/visible spectroscopy (UV-VIS) spectrometry, Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), thermogravimetric analysis (TGA), and cyclic voltammetry (CV). The results showed that the substitution way of C(60)-py is different from that of MWCNT-py. The C(60)-py and a NH(3) replaced a Cl(-) and a bipyridine in Ru(II)(bpy)(2)Cl(2) to produce a five-coordinate complex of [Ru(bpy)(NH(3))(C(60)-py)Cl]PF(6), whereas MWCNT-py replaced a Cl(-) to generate a six-coordinate complex of [Ru(bpy)(2)(MWCNT-py)Cl]PF(6). The cyclic voltammetry study showed that the electron-withdrawing ability was different for C(60) and MWCNT. The C(60) showed a relatively stronger electron-withdrawing effect with respect to MWCNT.

摘要

本文讨论了通过 1,3-偶极环加成反应合成富勒烯吡咯吡啶(C(60)-py)和多壁碳纳米管吡咯吡啶(MWCNT-py)这两种基于碳的吡啶配体。在 NH(4)PF(6)存在下,通过配体取代反应合成了两种配合物 C(60)-Ru 和 MWCNT-Ru,反应前体为 Ru(II)(bpy)(2)Cl(2)。通过质谱(MS)、元素分析、核磁共振(NMR)光谱、红外光谱(IR)、紫外/可见光谱(UV-VIS)、拉曼光谱、X 射线光电子能谱(XPS)、热重分析(TGA)和循环伏安法(CV)对两种配合物进行了表征。结果表明,C(60)-py 的取代方式与 MWCNT-py 不同。C(60)-py 和一个 NH(3)取代了 Ru(II)(bpy)(2)Cl(2)中的一个 Cl(-)和一个联吡啶,生成了一个五配位的配合物[Ru(bpy)(NH(3))(C(60)-py)Cl]PF(6),而 MWCNT-py 取代了一个 Cl(-),生成了一个六配位的配合物[Ru(bpy)(2)(MWCNT-py)Cl]PF(6)。循环伏安法研究表明,C(60)和 MWCNT 的电子受主能力不同。C(60)相对于 MWCNT 具有更强的电子受主效应。

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