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Single-Chain Glycopolymer Folding via Host–Guest Interactions and Its Unprecedented Effect on DC-SIGN Binding
Biomacromolecules ( IF 5.5 ) Pub Date : 2018-06-05 00:00:00 , DOI: 10.1021/acs.biomac.8b00600
Gokhan Yilmaz 1 , Veselina Uzunova 2 , Richard Napier 2 , C. Remzi Becer 1
Affiliation  

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.

中文翻译:

通过主体-来宾相互作用的单链含糖聚合物折叠及其对DC-SIGN结合的空前影响

天然生物大分子的可逆自折叠作用对于自然界中的特定和独特的生物学功能起着至关重要的作用。因此,近年来,单聚合物链的受控折叠引起了极大的关注。在此,产生了在结中具有不同糖部分密度的α-形状的可逆单链折叠糖聚合物结构。研究了结中折叠以及糖密度对与凝集素(例如ConA,DC-SIGN和DC-SIGNR)的结合能力的影响。使用可逆加成-断裂链转移(RAFT)聚合技术,可以合成带有β-CD和金刚烷用于主体-客体相互作用以及甘露糖残基用于凝集素相互作用的三嵌段糖共聚物。糖聚合物的可逆单链折叠在水溶液的高稀释度下实现,并且自组装折叠通过2D核Overhauser增强光谱法(NOESY)NMR和动态光散射进行监测。凝集素结合概况始终如一地提供了单链折叠的空前效果,因为与未折叠的线性结构相比,单链折叠的结构大大增强了结合能力。
更新日期:2018-06-05
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