Single-Chain Glycopolymer Folding via Host-Guest Interactions and Its Unprecedented Effect on DC-SIGN Binding.
Single-Chain Glycopolymer Folding via Host-Guest Interactions and Its Unprecedented Effect on DC-SIGN Binding.
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DOI：
10.1021/acs.biomac.8b00600
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发表时间：
2018-06
影响因子：
6.2
通讯作者：
G. Yilmaz;V. Uzunova;R. Napier;C. Becer
中科院分区：
文献类型：
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作者：
G. Yilmaz;V. Uzunova;R. Napier;C. Becer
天然生物大分子的可逆自折叠作用对于自然界中特定和独特的生物功能起着至关重要的作用。因此，单聚合物链的受控折叠近年来引起了人们的广泛关注。在此，创建了α型可逆单链折叠糖聚合物结构，结中糖部分的密度不同。研究了折叠以及结中糖密度对与凝集素（例如ConA、DC-SIGN 和DC-SIGNR）结合能力的影响。使用可逆加成-断裂链转移（RAFT）聚合技术合成了带有用于主客体相互作用的β-CD和金刚烷以及用于凝集素相互作用的甘露糖残基的三嵌段糖共聚物。糖聚合物的可逆单链折叠是在水溶液的高度稀释下实现的，并且通过二维核欧沃豪瑟增强光谱（NOESY）NMR和动态光散射监测自组装折叠。凝集素结合谱始终提供前所未有的单链折叠效果，因为与未折叠的线性结构相比，单链折叠结构大大增强了结合能力。
Reversible self-folding actions of natural biomacromolecules play crucial roles for specific and unique biological functions in Nature. Hence, controlled folding of single polymer chains has attracted significant attention in recent years. Herein, reversible single-chain folded glycopolymer structures in α-shape with different density of sugar moieties in the knot were created. The influence of folding as well as the sugar density in the knot was investigated on the binding capability with lectins, such as ConA, DC-SIGN, and DC-SIGNR. The synthesis of triblock glycocopolymers bearing β-CD and adamantane for the host-guest interaction and also mannose residues for the lectin interaction was achieved using the reversible addition-fragmentation chain transfer (RAFT) polymerization technique. The reversible single-chain folding of glycopolymers was achieved under a high dilution of an aqueous solution and the self-assembled folding was monitored by 2D nuclear overhauser enhancement spectroscopy (NOESY) NMR and dynamic light scattering. The lectin binding profiles consistently provided an unprecedented effect of single chain folding as the single-chain folded structures enhanced greatly the binding ability in comparison to the unfolded linear structures.