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首页> 外文期刊>Chemistry: A European journal >Modification of Carbon Nanofibres for the Immobilization of Metal Complexes: A Case Study with Rhodium and Anthranilic Acid
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Modification of Carbon Nanofibres for the Immobilization of Metal Complexes: A Case Study with Rhodium and Anthranilic Acid

机译：碳纳米纤维的修饰，用于固定金属配合物：以铑和邻氨基苯甲酸为例

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摘要

The immobilisation of the rhodium/anthranilic acid complex onto fishbone carbon nanofibres (CNFs) was executed by means of the following steps: 1) surface oxidation of the fibres, 2) conversion of the oxygen-containing surface groups into acid chloride groups, 3) attachment of anthranilic acid and 4) complexation of rhodium by the at-tached anthranilic acid. The immobilisation process was followed and the resulting surface species were characterised by IR, X-ray absorption fine structure (XAFS) and X-ray photoelectron spectroscopy (XPS), and by molecular modelling. An thranilic acid bonds to the CNFs by an amide linkage to the carboxyl groups that are present after surface oxidation of the fibres. The immobilised anthranilic acid coordinates to rhodium through the nitrogen atom and the carboxyl group. The as-synthesised Rh~III complex itself is not active in the liquid-phase hydrogenation of cyclohexene. Reduction with sodium borohydride yields small particles (d=1.5-2 nm) of rhodium metal that are highly active. The results indicate that different activation procedures for the immobilised Rh/anthranilic acid system should be applied, such as reduction with a milder reducing agent or direct complexation of the rhodium in the Rh~I state.
机译：通过以下步骤将铑/邻氨基苯甲酸络合物固定在鱼骨碳纳米纤维（CNF）上：1）纤维的表面氧化; 2）含氧表面基团转化为酰氯基团; 3）邻氨基苯甲酸的附着和4）附位的邻氨基苯甲酸络合铑。随后进行固定化过程，并通过IR，X射线吸收精细结构（XAFS）和X射线光电子能谱（XPS）以及分子建模对所得表面物种进行表征。邻氨基苯甲酸通过与纤维表面氧化后存在的羧基的酰胺键与CNF结合。固定的邻氨基苯甲酸通过氮原子和羧基与铑配位。合成后的Rh〜III配合物本身在环己烯的液相加氢中没有活性。用硼氢化钠还原可得到高活性的金属铑小颗粒（d = 1.5-2 nm）。结果表明，对于固定化的Rh /邻氨基苯甲酸体系，应采用不同的活化程序，例如用较温和的还原剂还原或以Rh〜I态直接络合铑。

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