Synthesis and Solution-Phase Characterization of Sulfonated Oligothioetheramides,Macromolecules

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Synthesis and Solution-Phase Characterization of Sulfonated Oligothioetheramides
Macromolecules ( IF 5.1 ) Pub Date : 2017-11-01 00:00:00 , DOI: 10.1021/acs.macromol.7b01915
Joseph S Brown ₁ , Yaset M Acevedo ₁ , Grace D He ₁ , Jack H Freed ₂ , Paulette Clancy ₁ , Christopher A Alabi _{1,

2}

Affiliation

Nature has long demonstrated the importance of chemical sequence to induce structure and tune physical interactions. Investigating macromolecular structure and dynamics is paramount to understand macromolecular binding and target recognition. To that end, we have synthesized and characterized flexible sulfonated oligothioetheramides (oligoTEAs) by variable temperature pulse field gradient (PFG) NMR, double electron–electron resonance (DEER), and molecular dynamics (MD) simulations to capture their room temperature structure and dynamics in water. We have examined the contributions of synthetic length (2–12mer), pendant group charge, and backbone hydrophobicity. We observe significant entropic collapse, driven in part by backbone hydrophobicity. Analysis of individual monomer contributions revealed larger changes due to the backbone compared to pendant groups. We also observe screening of intramolecular electrostatic repulsions. Finally, we comment on the combination of DEER and PFG NMR measurements via Stokes–Einstein–Sutherland diffusion theory. Overall, this sensitive characterization holds promise to enable de novo development of macromolecular structure and sequence–structure–function relationships with flexible, but biologically functional macromolecules.

中文翻译：

磺化低聚硫醚酰胺的合成和溶液相表征

大自然早已证明了化学序列对于诱导结构和调整物理相互作用的重要性。研究大分子结构和动力学对于理解大分子结合和目标识别至关重要。为此，我们通过变温脉冲场梯度 (PFG) NMR、双电子-电子共振 (DEER) 和分子动力学 (MD) 模拟合成并表征了柔性磺化低聚硫醚酰胺 (oligoTEA)，以捕获其室温结构和动力学在水中。我们研究了合成长度（2-12mer）、侧基电荷和主链疏水性的贡献。我们观察到显着的熵崩溃，部分是由主链疏水性驱动的。对单个单体贡献的分析显示，与侧链基团相比，主链造成的变化更大。我们还观察了分子内静电斥力的筛选。最后，我们通过 Stokes-Einstein-Sutherland 扩散理论对 DEER 和 PFG NMR 测量的组合进行评论。总体而言，这种敏感的表征有望使大分子结构和序列-结构-功能关系与灵活但具有生物功能的大分子从头开发。

更新日期：2017-11-01

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