Tuning nanostructure dimensions with supramolecular twisting.
Tuning nanostructure dimensions with supramolecular twisting.
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DOI：
10.1021/jp3087978
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发表时间：
2013-04-25
影响因子：
3.3
通讯作者：
Stupp, Samuel I.
中科院分区：
文献类型：
--
作者：
Moyer, Tyson J.;Cui, Honggang;Stupp, Samuel I.
肽两亲物是含有共价键合到疏水尾部的肽段的分子，已知在水中自组装成超分子纳米结构，其形状多种多样，从球形到圆柱形、扭曲带、带和管。了解控制纳米结构尺寸和形状的自组装机制仍然是一个巨大的挑战。我们在此报告了对含有缬氨酸-谷氨酸二聚重复序列的肽两亲物的系统研究，已知该两亲物可促进自组装成带状扁平组装体。我们发现，随着二聚体重复次数从 2 个增加到 6 个，组装体的横向生长可以控制在 100 nm 至 10 nm 的范围内。利用圆二色性，发现超分子组装体内 β-片层扭曲的程度与 PA 分子中二聚体重复的数量成正比。有趣的是，随着扭曲的增加，达到了一个阈值，其中圆柱体而不是扁平组件成为主要形态。我们还表明，在带状区域中，可以通过提高 pH 值来增加电荷密度，从而增加谷氨酸残基之间的静电排斥力，从而减小纳米结构的宽度。这些纳米结构的尺寸和形状的控制应该会影响它们在生物信号传导和药物输送中的功能。
Peptide amphiphiles are molecules containing a peptide segment covalently bonded to a hydrophobic tail and are known to self-assemble in water into supramolecular nanostructures with shape diversity ranging from spheres to cylinders, twisted ribbons, belts, and tubes. Understanding the self-assembly mechanisms to control dimensions and shapes of the nanostructures remains a grand challenge. We report here on a systematic study of peptide amphiphiles containing valine-glutamic acid dimeric repeats known to promote self-assembly into belt-like flat assemblies. We find that lateral growth of the assemblies can be controlled in the range of 100 nm down to 10 nm as the number of dimeric repeats is increased from two to six. Using circular dichroism, the degree of β-sheet twisting within the supramolecular assemblies was found to be directly proportional to the number of dimeric repeats in the PA molecule. Interestingly, as twisting increased a threshold is reached where cylinders rather than flat assemblies become the dominant morphology. We also show that in the belt regime, the width of the nanostructures can be decreased by raising the pH to increase charge density and therefore electrostatic repulsion among glutamic acid residues. The control of size and shape of these nanostructures should affect their functions in biological signaling and drug delivery.
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影响因子：
3.9
作者：
Capes, Jacqueline S.;Kiley, Patrick J.;Windle, Alan H.
通讯作者：
Windle, Alan H.
影响因子：
10.8
作者：
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通讯作者：
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影响因子：
38.3
作者：
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影响因子：
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作者：
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通讯作者：
Stupp, Samuel I.
DOI：
10.1073/pnas.0801763105
发表时间：
2008-08-19
影响因子：
11.1
作者：
Gratton, Stephanie E. A.;Ropp, Patricia A.;DeSimone, Joseph M.
通讯作者：
DeSimone, Joseph M.