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Engineered Nanomaterial Transformation Under Oxidative Environmental Conditions: Development Of An In Vitro Biomimetic Assay

机译:氧化环境条件下的工程纳米材料转化:体外仿生分析技术的发展

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Once released into the environment, engineered nanomaterials may be transformed by microbially mediated redox processes altering their toxicity and fate. Little information currently exists on engineered nanomaterial transformation under environmentally relevant conditions. Here, we report the development of an in vitro biomimetic assay for investigation of nanomaterial transformation under simulated oxidative environmental conditions. The assay is based on the extracellular hydroquinone-driven Fenton's reaction used by lignolytic fungi. We demonstrate the utility of the assay using CdSe_(core)/ZnS_(shell) quantum dots (QDs) functionalized with polyethylene glycol). QD transformation was assessed by UV-visible spectroscopy, inductively coupled plasma-optical emission spectroscopy, dynamic light scattering, transmission electron microscopy (TEM), and energy dispersive X-ray spectroscopy (EDX). QDs were readily degraded under simulated oxidative environmental conditions: the ZnS shell eroded and cadmium was released from the QD core. TEM, electron diffraction analysis, and EDX of transformed QDs revealed formation of amorphous Se aggregates. The biomimetic hydroquinone-driven Fenton's reaction degraded QDs to a larger extent than did H_2O_2 and classical Fenton's reagent (H_2O_2 + Fe~(2+)). This assay provides a new method to characterize transformations of nanoscale materials expected to occur under oxidative environmental conditions.
机译:一旦释放到环境中,工程纳米材料可以通过微生物介导的氧化还原过程进行转化,从而改变其毒性和命运。目前在环境相关的条件下关于工程纳米材料转化的信息很少。在这里,我们报告了体外仿生测定法的发展,用于在模拟氧化环境条件下研究纳米材料的转化。该测定基于木质素分解真菌使用的细胞外对苯二酚驱动的Fenton反应。我们展示了使用CdSe_(core)/ ZnS_(shell)量子点(QDs)(用聚乙二醇官能化)进行测定的实用性。通过紫外可见光谱,电感耦合等离子体-光发射光谱,动态光散射,透射电子显微镜(TEM)和能量色散X射线光谱(EDX)评估了QD转换。在模拟的氧化环境条件下,量子点很容易降解:ZnS壳腐蚀,镉从量子点的核心中释放出来。 TEM,电子衍射分析和转化的QD的EDX揭示了非晶硒聚集体的形成。仿生对苯二酚驱动的Fenton反应的降解QDs比H_2O_2和经典Fenton试剂(H_2O_2 + Fe〜(2+))降解的程度更大。该测定法提供了一种表征预期在氧化环境条件下发生的纳米级材料转化的新方法。

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