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首页> 外文期刊>Chemistry: A European journal >A top-down synthesis route to ultrasmall multifunctional Gd-based silica nanoparticles for theranostic applications
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A top-down synthesis route to ultrasmall multifunctional Gd-based silica nanoparticles for theranostic applications

机译：自上而下的合成方法，用于超小多功能基于Gd的二氧化硅纳米颗粒，用于治疗学应用

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摘要

New, ultrasmall nanoparticles with sizes below 5 nm have been obtained. These small rigid platforms (SRP) are composed of a polysiloxane matrix with DOTAGA (1,4,7,10-tetraazacyclododecane-1-glutaric anhydride-4,7,10-triacetic acid)-Gd~(3+) chelates on their surface. They have been synthesised by an original top-down process: 1) formation of a gadolinium oxide Gd _2O_3 core, 2) encapsulation in a polysiloxane shell grafted with DOTAGA ligands, 3) dissolution of the gadolinium oxide core due to chelation of Gd~(3+) by DOTAGA ligands and 4) polysiloxane fragmentation. These nanoparticles have been fully characterised using photon correlation spectroscopy (PCS), transmission electron microscopy (TEM), a superconducting quantum interference device (SQUID) and electron paramagnetic resonance (EPR) to demonstrate the dissolution of the oxide core and by inductively coupled plasma mass spectrometry (ICP-MS), mass spectrometry, fluorescence spectroscopy, ~(29)Si solid-state NMR, 1H NMR and diffusion ordered spectroscopy (DOSY) to determine the nanoparticle composition. Relaxivity measurements gave a longitudinal relaxivity r _1 of 11.9 s~(-1) mM~(-1) per Gd at 60 MHz. Finally, potentiometric titrations showed that Gd~(3+) is strongly chelated to DOTAGA (complexation constant logβ_(110)=24.78) and cellular tests confirmed the that nanoconstructs had a very low toxicity. Moreover, SRPs are excreted from the body by renal clearance. Their efficiency as contrast agents for MRI has been proved and they are promising candidates as sensitising agents for image-guided radiotherapy.
机译：已经获得了尺寸小于5nm的新的超小纳米颗粒。这些小的刚性平台（SRP）由聚硅氧烷基质组成，在它们的表面上带有DOTAGA（1,4,7,10-四氮杂环十二烷-1-戊二酸酐-4,7,10-三乙酸）-Gd〜（3+）螯合物表面。它们是通过原始的自上而下的过程合成的：1）氧化oxide Gd _2O_3核的形成，2）封装在接有DOTAGA配体的聚硅氧烷壳中，3）由于Gd〜（）的螯合而使氧化lin核溶解。 3+）通过DOTAGA配体和4）聚硅氧烷断裂。这些纳米粒子已使用光子相关光谱（PCS），透射电子显微镜（TEM），超导量子干涉装置（SQUID）和电子顺磁共振（EPR）进行了全面表征，以证明氧化物核的溶解以及通过电感耦合的等离子体质量光谱法（ICP-MS），质谱法，荧光光谱法，〜（29）Si固态NMR，1H NMR和扩散有序光谱法（DOSY）确定纳米颗粒的组成。弛豫度测量结果表明，在60 MHz时，纵向弛豫度r _1为每Gd 11.9 s〜（-1）mM〜（-1）。最后，电位滴定表明Gd〜（3+）与DOTAGA螯合度很强（络合常数logβ_（110）= 24.78），细胞测试证实纳米结构的毒性很低。而且，SRP通过肾脏清除而从体内排出。已经证明了它们作为MRI造影剂的效率，它们有望成为图像引导放射治疗的敏化剂。

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