Helical Molecular Springs with Varying Spring Constants
Helical Molecular Springs with Varying Spring Constants
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具有不同弹簧常数的螺旋分子弹簧
DOI：
10.1002/anie.202209772
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发表时间：
2022
期刊：
影响因子：
--
通讯作者：
Schneebeli, Severin T.
中科院分区：
文献类型：
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作者：
Murphy, Kyle E.;McKay, Kyle T.;Schenkelberg, Mica;Sharafi, Mona;Vestrheim, Olav;Ivancic, Monika;Li, Jianing;Schneebeli, Severin T.
我们报告了一个通用的合成路线，对螺旋梯形聚合物与不同的弹簧常数，建立与手性辅助合成（CAS）。在拉伸和压缩下，这些形状持久的结构不会展开，而是拉伸和压缩，类似于经典的胡克弹簧。我们的合成适用于不同螺距和直径的螺旋，这使我们能够研究溶液中的分子灵活性如何取决于梯形聚合物的确切几何形状。具体来说，我们用分子动力学模拟和通过测量我们的聚合物在不同拉莫尔频率下的核磁共振弛豫时间（T1）表明，增加螺旋直径会导致灵活性增加。我们的研究结果提出了调整溶液中固有螺旋梯形聚合物机械性能的初步设计规则，这将有助于激发一类新的具有不同机械性能的坚固的弹簧状分子材料。
We report a general synthetic route toward helical ladder polymers with varying spring constants, built with chirality‐assisted synthesis (CAS). Under tension and compression, these shape‐persistent structures do not unfold, but rather stretch and compress akin classical Hookean springs. Our synthesis is adaptable to helices with different pitch and diameter, which allowed us to investigate how molecular flexibility in solution depends on the exact geometry of the ladder polymers. Specifically, we showed with molecular dynamic simulations and by measuring the longitudinal1H NMR relaxation times (T1) for our polymers at different Larmor frequencies, that increasing the helix diameter leads to increased flexibility. Our results present initial design rules for tuning the mechanical properties of intrinsically helical ladder polymers in solution, which will help inspire a new class of robust, spring‐like molecular materials with varying mechanical properties.