Impact of dynamic sub-populations within grafted chains on the protein binding and colloidal stability of PEGylated nanoparticles,Nanoscale

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Impact of dynamic sub-populations within grafted chains on the protein binding and colloidal stability of PEGylated nanoparticles
Nanoscale ( IF 5.8 ) Pub Date : 2021-2-22 , DOI: 10.1039/d0nr08294e
Delyan R. Hristov _{1,

2,

3,

4,

5} , Hender Lopez _{5,

6,

7,

8} , Yannick Ortin _{2,

3,

5,

9} , Kate O'Sullivan _{2,

3,

5,

9} , Kenneth A. Dawson _{1,

2,

3,

4,

5} , Dermot F. Brougham _{2,

3,

5,

9}

Affiliation

Polyethylene glycol grafting has played a central role in preparing the surfaces of nano-probes for biological interaction, to extend blood circulation times and to modulate protein recognition and cellular uptake. However, the role of PEG graft dynamics and conformation in determining surface recognition processes is poorly understood primarily due to the absence of a microscopic picture of the surface presentation of the polymer. Here a detailed NMR analysis reveals three types of dynamic ethylene glycol units on PEG-grafted SiO₂ nanoparticles (NPs) of the type commonly evaluated as long-circulating theranostic nano-probes; a narrow fraction with fast dynamics associated with the chain ends; a broadened fraction spectrally overlapped with the former arising from those parts of the chain experiencing some dynamic restriction; and a fraction too broad to be observed in the spectrum arising from units closer to the surface/graft which undergo slow motion on the NMR timescale. We demonstrate that ethylene glycol units transition between fractions as a function of temperature, core size, PEG chain length and surface coverage and demonstrate how this distribution affects colloidal stability and protein uptake. The implications of the findings for biological application of grafted nanoparticles are discussed in the context of accepted models for surface ligand conformation.

中文翻译：

嫁接链中动态亚群对聚乙二醇化纳米颗粒蛋白质结合和胶体稳定性的影响

聚乙二醇接枝在准备用于生物相互作用的纳米探针表面，延长血液循环时间以及调节蛋白质识别和细胞摄取方面起着核心作用。然而，人们对PEG接枝动力学和构象在确定表面识别过程中的作用知之甚少，这主要是由于缺乏聚合物表面表现的显微照片。在这里，详细的NMR分析揭示了PEG接枝的SiO ₂上的三种动态乙二醇单元通常被认为是长循环的诊断纳米探针的类型的纳米颗粒；链段末端具有快速动力学的狭窄部分；链上那些受到动态限制的部分，在光谱上与前者光谱重叠；以及由于在NMR时标上经历缓慢运动的更靠近表面/接枝的单元而导致的光谱中太宽以至于无法在光谱中观察到的分数。我们证明乙二醇单元在各部分之间的转变是温度，核心尺寸，PEG链长和表面覆盖率的函数，并证明这种分布如何影响胶体稳定性和蛋白质摄取。在表面配体构象的公认模型的背景下讨论了发现的结果对于生物学应用接枝纳米颗粒的意义。

更新日期：2021-03-04

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