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Angew. Chem. Int. Ed.发表课题组首次合成同位素标记一维碳链的工作
发布时间:2021-02-18

        同位素可用于追踪物质的运行和变化规律。同位素标记的材料往往可以保持相同的化学性质,但是其物理性质会发生改变。

        近期,我们关于合成同位素标记的一维碳链的论文被Angew. Chem. Int. Ed.接收发表,这是世界首次合成同位素标记的一维碳链样品,后续将继续针对样品进行光学和热学方面的深入研究,探究其物理性能的变化。

        论文由崔玮丽同学实验完成,乌尔姆大学的曹克诚教授(现上海科技大学)和Ute Kaiser教授进行的电镜表征工作,日本产业综合研究所的Takeshi Saito研究员提供的单壁碳纳米管样品,维也纳大学的Paola Ayala教授对写作和数据分析有贡献,中山大学石磊和维也纳大学Thomas Pichler教授为共同通讯作者。

        恭喜玮丽!感谢她在这一课题中的努力,做出了漂亮的工作!

        论文链接:https://doi.org/10.1002/anie.202017356

        免费下载:https://onlinelibrary.wiley.com/share/author/PQ3VEZCSGCYG8MSTWMXB?target=10.1002/anie.202017356



    Carbyne, as a new truly one-dimensional carbon allotrope is one of the most interesting existing one-dimensional materials because of its predicted outstanding mechanical, thermal and electronic properties but synthesizing it has remained challenging for more than 125 years because of its instability. In our previous studies since 2016, we showed a pathway to overcome this issue by confining very long carbon chains, i.e., carbyne, inside the hollow core of double walled carbon nanotubes by high temperature and high vacuum annealing (Nature Mater. 201615, 634-639). Last year we have proven that this material has at least a factor of 100 stronger resonance cross section as any other known material for Raman scattering (Nano Lett. 202020, 6750-6755). This paves the way of the application of confined carbyne as tracers or contact free temperature sensor. However, gaining control on the growth and functionality of confined carbyne remained challenging. A recent study (Nano Lett. 202121, 1096-1101) showed a novel pathway by stepwise growth of confined carbyne with single walled carbon nanotubes transformed to double walled carbon nanotubes first.

    The present study led by Lei Shi at Sun Yat-Sen University in China and Thomas Pichler at Vienna University, which has been just published in Angewandte Chemie-International Edition, reports a breakthrough in the controlled growth carbyne in double walled carbon nanotubes with greatly enhanced yield using nanotubes filled with liquid precursors as starting material. This method uniquely facilitates also to tailor the functionality of confined carbyne by isotope labelling. As shown in the sketch below, we used isotopic labelled liquid precursors and encapsulated them inside carbon nanotubes as carbon source for further synthesis. This allowed us to obtain pioneering results on isotope engineered carbyne with around 11.9% of 13C-labelling using 13C-methanol as precursor.

 

    This method of isotope engineering of carbyne brings unprecedented capability to tune the properties of these confined long linear carbon chains. So far, only the interaction with nanotubes that host and protect them from the environment has been found to offer a possibility to control carbyne´s properties. 

 

    “Isotope engineering keeps the same chemical structure but implies identifying nuclei of different sizes with tremendous implications in the physical performance of the material itself, for instance regarding its thermal conductivity. Hence, the method reported here opens a new opportunity for the design of advanced heterostructured nanomaterials and paves the way to applications in quantum spin transport, nanoelectronics, nuclear magnetic resonance and others, with a huge enforcement potential within short reach.” said lead author Weili Cui.

 

    The work was supported by the National Natural Science Foundation of China and FWF.

 

Publication in "Angew. Chem. Int. Ed. ":

“Isotopic labelling of confined carbyne” Weili Cui, Lei Shi, Kecheng Cao, Ute Kaiser, Takeshi Saito, Paola Ayala, Thomas Pichler

Angewandte Chemie-International Edition, DOI: 10.1002/anie.202017356