轮螺旋自组织的非凡加速 通过编码它们的三级结构的链序列
Li Wang1,2, Benjamin E Partridge1, Ning Huang1
1Roy & Diana Vagelos Laboratories, Department of Chemistry, University of Pennsylvania, Philadelphia, Pennsylvania 19104-6323, United States.
Journal of the American Chemical Society
|April 29, 2020
概括
轮模型使二烯基 (PBI) 能够快速自组装成有序的螺旋柱. 一个特定的9r9树突序列极大地加快了这种结晶,创造了已知最快的超分子或共价宏分子.
科学领域:
- 超分子化学
- 材料科学
- 晶体学
背景情况:
- 在创建有序材料的关键是等级的自我组织.
- 烯二氧化物 (PBIs) 与小结合形成晶状螺旋柱状六角阵列,通过轮模型.
- 之前的研究表明组装在缓慢的冷却/加热速度 (1°C/分钟) 和有限的成功与混合树枝.
研究的目的:
- 调查序列定义的树枝对PBI的自组装动力学的影响.
- 探索具有不同链长度 (n=6,7,9,10) 和奇拉/阿奇拉图案的新混合PBI库.
- 了解加速轮组件背后的机制.
主要方法:
- 四个混合二氧化物 (PBIs) 库的合成,具有序列定义的树突.
- 纤维X射线衍射和差分扫描热量计 (DSC) 用于结构和热量分析.
- 固态核磁共振 (NMR) 光谱以阐明分子动力学.
主要成果:
- 9r9序列定义的树突使前所未有的轮组装速度达到50°C/分钟 (加热和冷却).
- 这是迄今为止报告的最快结晶的超分子或共价宏分子.
- 固态NMR显示加速组装是由于最佳的晶体包装和链动态.
结论:
- 序列定义的树枝可以极大地加快PBI系统中的等级自我组织.
- 9r9 PBI系统展示了快速超分子结晶的新基准.
- 这些发现挑战了关于有序系统中性性的假设,并突出了混乱在创造秩序中的作用.
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