One-Pot, Large-Scale Synthesis of Organic Color Center-Tailored Semiconducting Carbon Nanotubes
One-Pot, Large-Scale Synthesis of Organic Color Center-Tailored Semiconducting Carbon Nanotubes
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DOI：
10.1021/acsnano.9b04087
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发表时间：
2019-07-01
期刊：
影响因子：
17.1
通讯作者：
Wang, YuHuang
中科院分区：
文献类型：
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作者：
Luo, Hong-Bin;Wang, Peng;Wang, YuHuang
有机色心定制半导体单壁碳纳米管是一个新兴的合成量子发射器家族，其显示明亮的缺陷光致发光，可用于成像，传感和量子信息处理。这一领域的一个重大进展将是开发一种高产率的合成路线，该路线能够生产远远超过目前μ g/mL规模的这些材料。在这里，我们证明，加入氯磺酸溶液的原料碳纳米管，亚硝酸钠，和苯胺衍生物到水中容易导致有机色心定制的纳米管的合成。这种出乎意料的简单一锅反应是高度可扩展的（在一次运行中产生数百毫克的材料），高效的（反应在几秒钟内完成）和通用的（实现了以前无法实现的有机色心的合成）。植入的有机色心可以通过从超过40种市售的苯胺衍生物（包括许多氟苯胺和氨基苯甲酸衍生物，并且难以转化为重氮盐）中选择来容易地定制。我们发现这种化学方法适用于所有研究的纳米管手性。合成的材料是纯净的固体，根据具体应用，可以通过表面活性剂或聚合物直接分散在水或有机溶剂中。纳米管产物还可以进一步分选成具有缺陷特异性光致发光的单一手性富集部分，所述缺陷特异性光致发光在近似1100至近似1550 nm范围内可调。因此，这种一锅法化学为许多需要大量材料的潜在应用提供了高度可扩展的有机色心合成。
Organic color center-tailored semiconducting single walled carbon nanotubes are a rising family of synthetic quantum emitters that display bright defect photoluminescence molecularly tunable for imaging, sensing, and quantum information processing. A major advance in this area would be the development of a high-yield synthetic route that is capable of producing these materials well exceeding the current mu g/mL scale. Here, we demonstrate that adding a chlorosulfonic acid solution of raw carbon nanotubes, sodium nitrite, and an aniline derivative into water readily leads to the synthesis of organic color center-tailored nanotubes. This unexpectedly simple one-pot reaction is highly scalable (yielding hundreds of milligrams of materials in a single run), efficient (reaction completes in seconds), and versatile (achieved the synthesis of organic color centers previously unattainable). The implanted organic color centers can be easily tailored by choosing from the more than 40 aniline derivatives that are commercially available, including many fluoroaniline and aminobenzoic acid derivatives, and that are difficult to convert into diazonium salts. We found this chemistry works for all the nanotube chiralities investigated. The synthesized materials are neat solids that can be directly dispersed in either water or an organic solvent by a surfactant or polymer depending on the specific application. The nanotube products can also be further sorted into single chirality-enriched fractions with defect-specific photoluminescence that is tunable over similar to 1100 to similar to 1550 nm. This one-pot chemistry thus provides a highly scalable synthesis of organic color centers for many potential applications that require large quantities of materials.