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Structure-Function Relationship of PAMAM Dendrimers as Robust Oil Dispersants

机译:PAMAM树枝状聚合物作为稳健油分散剂的结构-功能关系

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摘要

PAMAM dendrimers have recently been investigated as efficient and biocompatible oil dispersants utilizing their encapsulation capacity; however, their high cationic charge density has been shown to be cytotoxic. It is therefore imperative to mitigate cationic charge-induced toxicity and understand the effects of such changes. Presented here is a synergistic experimental and computational approach to examine the effects of varying terminal surface charge on the capacity of dendrimers to disperse model liner, polycyclic aromatic, and hybrid hydrocarbons. Uncharged dendrimers collapse by forming intramolecular hydrogen bonds, which reduce the hosting capability. On the other hand, changing the surface charges from positive to negative greatly shifts the pK, of tertiary amines of the PAMAM dendrimer interior. As a result, the negatively charged dendrimers have a significant percentage of tertiary amines protonated, ~30%. This unexpected change in the interior protonation state causes electrostatic interactions with the anionic terminal groups, leading to contraction and a marked decrease in hydrocarbon hosting capacity. The present work highlights the robust nature of dendrimer oil dispersion and also illuminates potentially unintended or unanticipated effects of varying dendrimer surface chemistry on their encapsulation or hosting efficacy, which is important for their environmental, industrial, and biomedical applications.
机译:最近,利用PAMAM树状大分子的包封能力,已将其作为有效且生物相容的油分散剂进行了研究。然而,它们的高阳离子电荷密度已被证明具有细胞毒性。因此,必须减轻阳离子电荷引起的毒性并了解这种变化的影响。这里介绍的是一种协同实验和计算方法,以检查变化的末端表面电荷对树枝状聚合物分散模型衬里,多环芳族化合物和杂化烃的能力的影响。不带电的树枝状大分子通过形成分子内氢键而崩溃,从而降低了宿主能力。另一方面,将表面电荷从正电荷变为负电荷会极大地改变PAMAM树状聚合物内部的叔胺的pK。结果,带负电荷的树状聚合物的叔胺质子化比例很高,约为30%。内部质子化状态的这种意外变化会引起与阴离子端基的静电相互作用,从而导致收缩并显着降低烃的吸收能力。本工作突出了树枝状聚合物油分散体的稳健性,并阐明了树枝状聚合物表面化学变化对它们的封装或寄主功效的潜在意想不到或无法预期的影响,这对于其环境,工业和生物医学应用至关重要。

著录项

  • 来源
    《Environmental Science & Technology》 |2014年第21期|12868-12875|共8页
  • 作者单位

    Department of Physics and Astronomy, Clemson University, Clemson, South Carolina 29634, United States;

    Department of Physics and Astronomy, Clemson University, Clemson, South Carolina 29634, United States;

    Department of Physics and Astronomy, Clemson University, Clemson, South Carolina 29634, United States;

    Department of Environmental Engineering and Earth Sciences, Clemson University, Clemson, South Carolina 29634, United States;

    Department of Physics and Astronomy, Clemson University, Clemson, South Carolina 29634, United States;

    Department of Physics and Astronomy, Clemson University, Clemson, South Carolina 29634, United States;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
  • 原文格式 PDF
  • 正文语种 eng
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