Charge-transfer interactions induce surface dependent conformational changes in apolipoprotein biocorona.
Charge-transfer interactions induce surface dependent conformational changes in apolipoprotein biocorona.
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DOI：
10.1116/1.4977064
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发表时间：
2017-03
期刊：
影响因子：
2.1
通讯作者：
Achyut J. Raghavendra;Nasser B Alsaleh;Jared M Brown;R. Podila
中科院分区：
文献类型：
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作者：
Achyut J. Raghavendra;Nasser B Alsaleh;Jared M Brown;R. Podila
在引入生物系统后，工程纳米材料（ENM）迅速与各种生物分子（如蛋白质和脂质）结合，形成生物冠。“生物冠”的存在会显著影响纳米生物相互作用，并最终导致生物反应的改变。载脂蛋白A-I（ApoA-I）是高密度脂蛋白（HDL）的主要成分，是在ENM生物冠中发现的最普遍的蛋白质之一，与ENM的性质、大小和形状无关。鉴于ApoA-I在HDL和胆固醇转运中的重要性，有必要了解ApoA-I吸附的机制和相关的结构变化，以评估ENM暴露的后果。在这里，作者使用了一系列全面的显微镜和光谱工具来阐明ApoA-I和具有四种不同表面官能团的100 nm Ag纳米颗粒（AgNPs）之间的相互作用。作者发现，蛋白质的吸附和二级结构的变化高度依赖于表面功能。我们的电化学研究为电荷转移相互作用影响ApoA-I展开提供了新的证据。虽然ApoA-I在AgNP上的解折叠没有显著改变它们的摄取和短期细胞毒性，但作者观察到它强烈改变了仅一些AgNP产生活性氧的能力。我们的研究结果揭示了生物冠形成的表面功能和电荷转移相互作用的重要性。
Upon introduction into a biological system, engineered nanomaterials (ENMs) rapidly associate with a variety of biomolecules such as proteins and lipids to form a biocorona. The presence of "biocorona" influences nano-bio interactions considerably, and could ultimately result in altered biological responses. Apolipoprotein A-I (ApoA-I), the major constituent of high-density lipoprotein (HDL), is one of the most prevalent proteins found in ENM-biocorona irrespective of ENM nature, size, and shape. Given the importance of ApoA-I in HDL and cholesterol transport, it is necessary to understand the mechanisms of ApoA-I adsorption and the associated structural changes for assessing consequences of ENM exposure. Here, the authors used a comprehensive array of microscopic and spectroscopic tools to elucidate the interactions between ApoA-I and 100 nm Ag nanoparticles (AgNPs) with four different surface functional groups. The authors found that the protein adsorption and secondary structural changes are highly dependent on the surface functionality. Our electrochemical studies provided new evidence for charge transfer interactions that influence ApoA-I unfolding. While the unfolding of ApoA-I on AgNPs did not significantly change their uptake and short-term cytotoxicity, the authors observed that it strongly altered the ability of only some AgNPs to generate of reactive oxygen species. Our results shed new light on the importance of surface functionality and charge transfer interactions in biocorona formation.