Assessing the Solution Shape and Size of Charged Dendronized Polymers Using Double Electron-Electron Resonance

Assessing the Solution Shape and Size of Charged Dendronized Polymers Using Double Electron-Electron Resonance
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DOI:
10.1021/jz200653k
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发表时间:
2011-07-07
影响因子:
5.7
通讯作者:
Hinderberger, Dariush
Hinderberger, Dariush
中科院分区:
化学2区
文献类型:
--
作者:
Kurzbach, Dennis;Kattnig, Daniel R.;Hinderberger, Dariush

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我们提供的双电子电子共振 (DEER) 数据表明,溶液中的高度支化树枝状聚合物 (denpols) 是具有持久形状、明确的包络线和独立于其环境的尺寸的大分子。通过测定圆柱形和阳离子 denpol 表面上自组装双阴离子自旋探针(弗雷米盐双阴离子)的距离分布,我们表明测量的溶液半径与中性 denpol 类似物的固态半径非常一致。为此目的,开发了圆柱体侧面颗粒的解析距离分布,并将其拟合至 DEER 时间轨迹。这样,DEER 与定点自旋探测相结合,提供了一种间接且简单的方法来确定纳米尺度上大分子的溶液形状和尺寸。它还表明,溶液中的至少第四代和第三代denpols可能已经被描述为分子物体。
We present double electron electron resonance (DEER) data that suggest that highly branched dendronized polymers (denpols) in solution are macromolecules with persistent shape, a well-defined envelope, and a size independent of their environment. By determining the distance distribution of self-assembled dianionic spin probes (Fremy's salt dianion) on the surface of the cylindrically shaped and cationic denpols, we show that the measured solution radii are in good agreement with the solid-state radii of the neutral denpol analogues. An analytic distance distribution of particles on the lateral surface of cylinders is developed for this purpose and fitted to DEER time traces. Such, DEER in combination with site-directed spin probing provides an indirect and simple method to determine the solution shape and size of macromolecules on the nanometer scale. It furthermore shows that at least generation four and three denpols in solution may already be described as molecular objects.