Chelator-Free Radiolabeling of Nanographene: Breaking the Stereotype of Chelation.
Chelator-Free Radiolabeling of Nanographene: Breaking the Stereotype of Chelation.
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DOI：
10.1002/anie.201610649
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发表时间：
2017-03-06
期刊：
影响因子：
--
通讯作者：
Cai W
中科院分区：
文献类型：
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作者：
Shi S;Xu C;Yang K;Goel S;Valdovinos HF;Luo H;Ehlerding EB;England CG;Cheng L;Chen F;Nickles RJ;Liu Z;Cai W
大环螯合剂已被广泛应用于基于纳米颗粒的正电子发射断层扫描（PET）成像领域，但其准确性仍存在疑问。在这里，我们发现64 Cu可以基于Cu和石墨烯的π电子之间的相互作用内在地标记到纳米石墨烯上，而不需要螯合剂缀合，提供了一种有前途的替代放射性标记方法，其保持纳米颗粒的天然体内药代动力学。由于大量的π键，还原氧化石墨烯（RGO）与氧化石墨烯（GO）相比表现出显著更高的标记效率，并且表现出优异的体内放射稳定性。更重要的是，观察到1，4，7-三氮杂环壬烷-1，4，7-三乙酸（NOTA）在纳米石墨烯上的非特异性附着，这揭示了螯合剂介导的基于纳米颗粒的PET成像具有其固有的缺点，并且可能导致体内错误的成像结果。基于Cu与纳米石墨烯的π电子之间的相互作用的无螯合剂的放射性标记被示出，其可以潜在地替代螯合剂辅助的标记。体内正电子发射断层扫描成像的可靠性得到增强，同时绕过了传统基于螯合剂的标记的固有缺点。
Macrocyclic chelators have been widely employed in the realm of nanoparticle-based positron emission tomography (PET) imaging, whereas its accuracy remains questionable. Here, we found that 64Cu can be intrinsically labeled onto nanographene based on interactions between Cu and the π electrons of graphene without the need of chelator conjugation, providing a promising alternative radiolabeling approach that maintains the native in vivo pharmacokinetics of the nanoparticles. Due to abundant π bonds, reduced graphene oxide (RGO) exhibited significantly higher labeling efficiency in comparison with graphene oxide (GO) and exhibited excellent radiostability in vivo. More importantly, nonspecific attachment of 1,4,7-triazacyclononane-1,4,7-triacetic acid (NOTA) on nanographene was observed, which revealed that chelator-mediated nanoparticle-based PET imaging has its inherent drawbacks and can possibly lead to erroneous imaging results in vivo. Chelator-free radiolabeling based on interactions between Cu and the π electrons of nanographene was shown, which can potentially substitute chelator-assisted labeling. The reliability of in vivo positron emission tomography imaging is enhanced while bypassing the inherent drawbacks of conventional chelator-based labeling.