通过类Fenton反应轻松获得生物相容性单壁碳纳米管中的高亮度氧缺陷
Easy Access to Bright Oxygen Defects in Biocompatible Single-Walled Carbon Nanotubes via a Fenton-Like Reaction
AI总结：
本文提出一种基于类Fenton反应、无需光照的温和方法，在单壁碳纳米管中高效引入高亮度氧缺陷，显著提升NIR-II荧光性能并适用于体内成像与多巴胺传感。
摘要：
单壁碳纳米管（SWNTs）与发光氧缺陷的共价功能化可提高其亮度，并使其能够作为光学生物传感器或荧光探针应用于第二生物窗口（NIR-II）的体内成像。然而，由于反应条件窗口受限或需要受控紫外光照射，当前功能化方法难以获得高亮度的发光缺陷。本文报道了一种通过类Fenton反应引入发光氧缺陷的方法，该方法使用良性且廉价的化学品，无需光照射。采用该方法功能化的水分散体中的(6,5) SWNTs显示出明亮的$E_{11}$*发射（1105 nm），其峰值强度比原始$E_{11}$发射高3.2倍，并且具有可重复的3%光致发光量子产率。该功能化可在宽泛的反应参数范围内进行，甚至可使用未分选的纳米管原料在高浓度（100 mg/L）下进行，从而可大量获得高亮度发光SWNTs。我们进一步发现，所引入的氧缺陷在光照射下会发生重排，这为氧缺陷的结构和动力学提供了额外的见解。最后，超短SWNTs的氧缺陷功能化也能实现高光致发光量子产率，并且在与生物相容性聚乙二醇化磷脂或单链DNA进行表面活性剂交换后，其优异的发射性能得以保留，使其适用于体内NIR-II成像和多巴胺传感。
英文摘要：
The covalent functionalization of single-walled carbon nanotubes (SWNTs) with luminescent oxygen defects increases their brightness and enables their application as optical biosensors or fluorescent probes for in-vivo imaging in the second-biological window (NIR-II). However, obtaining luminescent defects with high brightness is challenging with the current functionalization methods due to a restricted window of reaction conditions or the necessity for controlled irradiation with ultraviolet light. Here we report a method for introducing luminescent oxygen defects via a Fenton-like reaction that uses benign and inexpensive chemicals without light irradiation. (6,5) SWNTs in aqueous dispersion functionalized with this method show bright $E_{11}$* emission (1105 nm) with 3.2-times higher peak intensities than the pristine $E_{11}$ emission and a reproducible photoluminescence quantum yield of 3%. The functionalization can be performed within a wide range of reaction parameters and even with unsorted nanotube raw material at high concentrations (100 mg/L), giving access to large amounts of brightly luminescent SWNTs. We further find that the introduced oxygen defects rearrange under light irradiation, which gives additional insights into the structure and dynamics of oxygen defects. Finally, the functionalization of ultra-short SWNTs with oxygen defects also enables high photoluminescence quantum yields and their excellent emission properties are retained after surfactant exchange with biocompatible pegylated phospholipids or single-stranded DNA to make them suitable for in-vivo NIR-II imaging and dopamine sensing.
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