Modifying the Molecular Structure of Carbon Nanotubes through Gas-Phase Reactants

IF 4.8 Q2 NANOSCIENCE & NANOTECHNOLOGY ACS Nanoscience Au Pub Date : 2023-02-06 DOI:10.1021/acsnanoscienceau.2c00052
Michael J. Giannetto, Eric P. Johnson, Adam Watson, Edgar Dimitrov, Andrew Kurth, Wenbo Shi, Francesco Fornasiero, Eric R. Meshot and Desiree L. Plata*, 
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引用次数: 2

Abstract

Current approaches to carbon nanotube (CNT) synthesis are limited in their ability to control the placement of atoms on the surface of nanotubes. Some of this limitation stems from a lack of understanding of the chemical bond-building mechanisms at play in CNT growth. Here, we provide experimental evidence that supports an alkyne polymerization pathway in which short-chained alkynes directly incorporate into the CNT lattice during growth, partially retaining their side groups and influencing CNT morphology. Using acetylene, methyl acetylene, and vinyl acetylene as feedstock gases, unique morphological differences were observed. Interwall spacing, a highly conserved value in natural graphitic materials, varied to accommodate side groups, increasing systematically from acetylene to methyl acetylene to vinyl acetylene. Furthermore, attenuated total reflectance Fourier-transfer infrared spectroscopy (ATR-FTIR) illustrated the existence of intact methyl groups in the multiwalled CNTs derived from methyl acetylene. Finally, the nanoscale alignment of the CNTs grown in vertically aligned forests differed systematically. Methyl acetylene induced the most tortuous growth while CNTs from acetylene and vinyl-acetylene were more aligned, presumably due to the presence of polymerizable unsaturated bonds in the structure. These results demonstrate that feedstock hydrocarbons can alter the atomic-scale structure of CNTs, which in turn can affect properties on larger scales. This information could be leveraged to create more chemically and structurally complex CNT structures, enable more sustainable chemical pathways by avoiding the need for solvents and postreaction modifications, and potentially unlock experimental routes to a host of higher-order carbonaceous nanomaterials.

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用气相反应物修饰碳纳米管的分子结构
目前的碳纳米管(CNT)合成方法在控制原子在纳米管表面的放置的能力方面受到限制。其中一些限制源于对CNT生长中的化学键构建机制缺乏了解。在这里,我们提供了支持炔烃聚合途径的实验证据,在该途径中,短链炔烃在生长过程中直接结合到CNT晶格中,部分保留其侧基并影响CNT形态。使用乙炔、甲基乙炔和乙烯基乙炔作为原料气体,观察到独特的形态差异。壁间距是天然石墨材料中的一个高度保守值,它随着侧基的变化而变化,从乙炔到甲基乙炔再到乙烯基乙炔都在系统地增加。此外,衰减全反射傅立叶转移红外光谱(ATR-FTIR)表明,在源自甲基乙炔的多壁CNT中存在完整的甲基。最后,生长在垂直排列的森林中的CNT的纳米级排列存在系统性差异。甲基乙炔诱导了最曲折的生长,而乙炔和乙烯基乙炔的CNT排列更整齐,这可能是由于结构中存在可聚合的不饱和键。这些结果表明,原料碳氢化合物可以改变碳纳米管的原子级结构,进而影响更大规模的性能。这些信息可以用来创造更复杂的化学和结构CNT结构,通过避免溶剂和反应后修饰的需要,实现更可持续的化学途径,并有可能开启通往大量高阶碳质纳米材料的实验路线。
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来源期刊
ACS Nanoscience Au
ACS Nanoscience Au 材料科学、纳米科学-
CiteScore
4.20
自引率
0.00%
发文量
0
期刊介绍: ACS Nanoscience Au is an open access journal that publishes original fundamental and applied research on nanoscience and nanotechnology research at the interfaces of chemistry biology medicine materials science physics and engineering.The journal publishes short letters comprehensive articles reviews and perspectives on all aspects of nanoscience and nanotechnology:synthesis assembly characterization theory modeling and simulation of nanostructures nanomaterials and nanoscale devicesdesign fabrication and applications of organic inorganic polymer hybrid and biological nanostructuresexperimental and theoretical studies of nanoscale chemical physical and biological phenomenamethods and tools for nanoscience and nanotechnologyself- and directed-assemblyzero- one- and two-dimensional materialsnanostructures and nano-engineered devices with advanced performancenanobiotechnologynanomedicine and nanotoxicologyACS Nanoscience Au also publishes original experimental and theoretical research of an applied nature that integrates knowledge in the areas of materials engineering physics bioscience and chemistry into important applications of nanomaterials.
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