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Theoretical and experimental studies on the carbon-nanotube surface oxidation by nitric acid: Interplay between functionalization and vacancy enlargement

机译:硝酸对碳纳米管表面氧化的理论和实验研究:功能化与空位扩大之间的相互作用

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摘要

The nitric acid oxidation of multiwalled carbon nanotubes leading to surface carboxylic groups has been investigated both experimentally and theoretically. The experimental results show that such a reaction involves the initial rapid formation of carbonyl groups, which are then transformed into phenol or carboxylic groups. At room temperature, this reaction takes place on the most reactive carbon atoms. At higher temperatures a different mechanism would operate, as evidenced by the difference in activation energies. Experimental data can be partially related to first-principles calculations, showing a multistep functionalization mechanism. The theoretical aspects of the present article have led us to propose the most efficient pathway leading to carboxylic acid functional groups on the surface. Starting from mono-vacancies, it ends up with the synergistic formation of dangling -COOH groups and the enlargement of the vacancies.
机译:已经通过实验和理论研究了多壁碳纳米管的硝酸氧化产生表面羧基。实验结果表明,这种反应涉及羰基的初始快速形成,然后将其转化为酚或羧基。在室温下,该反应在反应性最高的碳原子上发生。在较高的温度下,会产生不同的机理,这由活化能的差异证明。实验数据可能与第一性原理计算部分相关,从而显示了多步功能化机制。本文的理论方面使我们提出了最有效的途径,可在表面上生成羧酸官能团。从单空位开始,它以悬挂的-COOH基团的协同形成和空位的扩大而结束。

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