Load-collapse-release cascades of amphiphilic guest molecules in charged dendronized polymers through spatial separation of noncovalent forces.
Load-collapse-release cascades of amphiphilic guest molecules in charged dendronized polymers through spatial separation of noncovalent forces.
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通过非共价力的空间分离，带电树枝状聚合物中两亲性客体分子的负载-塌缩-释放级联
DOI：
10.1002/chem.201204060
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发表时间：
2013
期刊：
影响因子：
--
通讯作者：
D. Hinderberger
中科院分区：
文献类型：
--
作者：
D. Kurzbach;X. Zhang;B. Zhang;P. Arnold;D. Hinderberger
描述了将客体分子包装到带电树枝化聚合物（denpol）中的能力，以及在负载-塌陷-释放级联中从随后密集聚集的 denpol 中释放这些客体分子的可能性。带电的 denpols 构成具有持久、明确的包膜和内部的分子物体，能够结合大量的两亲性客体分子。同时，多价离子可以与带电 denpol 表面配位，导致反离子诱导已经负载客体的主体结构发生聚集。因此，尽管基于denpol的分子运输中的局部客体浓度最初可能已经很高，因为树突denpol支架内的客体密集堆积，但“局部”客体浓度仍然可以通过主客体复合物本身的堆积（通过聚集）进一步增加。随后可以从致密聚集的树枝化聚合物中释放客体化合物（例如，通过增加咪唑基离子的溶液浓度）。增强了这种释放可能性，客体双重包装的概念，首先通过宿主本身，其次通过宿主的聚集，产生了负载-崩溃-释放级联，这惊人地展示了树枝化大分子在未来分子运输应用中的巨大潜力。
The ability to pack guest molecules into charged dendronized polymers (denpols) and the possibility to release these guest molecules from subsequently densely aggregated denpols in a load–collapse–release cascade is described. Charged denpols, which constitute molecular objects with a persistent, well‐defined envelope and interior, are capable of incorporating large amounts of amphiphilic guest molecules. Simultaneously, multivalent ions can coordinate to the surfaces of charged denpols, leading to counterion‐induced aggregation of the already guest‐loaded host structures. Thus, although the local guest concentration in denpol‐based molecular transport might already be initially high due to the dense guest packing inside the dendritic denpol scaffolding, the “local” guest concentration can nonetheless be further increased by packing (through aggregation) of the host–guest complexes themselves. Subsequent release of guest compounds from densely aggregated dendronized polymers is then possible (e.g., through increasing the solution concentration of imidazolium‐based ions). Augmented with this release possibility, the concept of twofold packing of guests, firstly through hosting itself and secondly through aggregation of the hosts, gives rise to a load–collapse–release cascade that strikingly displays the high potential of dendronized macromolecules for future molecular transport applications.
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