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基于树枝状大分子的主客体相互作用的顺磁 NMR 研究。

Paramagnetic NMR investigation of dendrimer-based host-guest interactions.

机构信息

Shanghai Key Laboratory of Regulatory Biology, School of Life Sciences, East China Normal University, Shanghai, People's Republic of China.

出版信息

PLoS One. 2013 Jun 10;8(6):e64722. doi: 10.1371/journal.pone.0064722. Print 2013.

DOI:10.1371/journal.pone.0064722
PMID:23762249
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC3677888/
Abstract

In this study, the host-guest behavior of poly(amidoamine) (PAMAM) dendrimers bearing amine, hydroxyl, or carboxylate surface functionalities were investigated by paramagnetic NMR studies. 2,2,6,6-Tetramethylpiperidinyloxy (TEMPO) derivatives were used as paramagnetic guest molecules. The results showed that TEMPO-COOH significantly broaden the ¹H NMR peaks of amine- and hydroxyl-terminated PAMAM dendrimers. In comparison, no paramagnetic relaxation enhancement (PRE) was observed between TEMPO-NH₂, TEMPO-OH and the three types of PAMAM dendrimers. The PRE phenomenon observed is correlated with the encapsulation of TEMPO-COOH within dendrimer pockets. Protonation of the tertiary amine groups within PAMAM dendrimers plays an important role during this process. Interestingly, the absence of TEMPO-COOH encapsulation within carboxylate-terminated PAMAM dendrimer is observed due to the repulsion of TEMPO-COO- anion and anionic dendrimer surface. The combination of paramagnetic probes and ¹H NMR linewidth analysis can be used as a powerful tool in the analysis of dendrimer-based host-guest systems.

摘要

在这项研究中，通过顺磁 NMR 研究了具有胺、羟基或羧酸盐表面官能团的聚（酰胺-胺）（PAMAM）树枝状大分子的主客体行为。使用 2,2,6,6-四甲基哌啶氧基（TEMPO）衍生物作为顺磁客体分子。结果表明，TEMPO-COOH 显著展宽了胺和羟基末端 PAMAM 树枝状大分子的 ¹H NMR 峰。相比之下，TEMPO-NH₂、TEMPO-OH 与三种 PAMAM 树枝状大分子之间未观察到顺磁弛豫增强（PRE）现象。观察到的 PRE 现象与 TEMPO-COOH 在树枝状大分子口袋内的包合有关。在这个过程中，PAMAM 树枝状大分子中叔胺基团的质子化起着重要作用。有趣的是，由于 TEMPO-COO-阴离子和阴离子树枝状大分子表面的排斥，未观察到 TEMPO-COOH 在羧酸盐末端 PAMAM 树枝状大分子内的包合。顺磁探针和 ¹H NMR 线宽分析的结合可作为分析基于树枝状大分子的主客体体系的有力工具。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/427f/3677888/fea530cb0ca1/pone.0064722.g008.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/427f/3677888/da7636ab0df1/pone.0064722.g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/427f/3677888/cd17c26c6748/pone.0064722.g007.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/427f/3677888/595031ac1117/pone.0064722.g001.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/427f/3677888/d1701e2ba5cf/pone.0064722.g003.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/427f/3677888/fea530cb0ca1/pone.0064722.g008.jpg

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