Luan Jiabin, Wang Danni, Zhang Shaohua, Miyazaki Yusuke, Shinoda Wataru, Wilson Daniela A
Institute for Molecules and Materials, Radboud University Nijmegen, Heyendaalseweg 135, 6525 AJ Nijmegen, The Netherlands.
Research Institute for Interdisciplinary Science, Okayama University, Okayama 700-8530, Japan.
J Am Chem Soc. 2023 Jul 19;145(28):15496-15506. doi: 10.1021/jacs.3c04285. Epub 2023 Jul 10.
The field of supramolecular chemistry has witnessed tremendous progress in bringing the system away from equilibrium for traditionally inaccessible structures and functions. Vesicular assemblies with complex energy landscapes and pathways, which are reminiscent of diverse cellular vesicles like exosomes, remain exceedingly rare. Here, relying on the activation of oligo(ethylene glycol) (OEG) interdigitation and the encoded conformational freedom in monodisperse Janus dendrimers, we reveal a rich landscape and a pathway selection of distinct vesicles. The interdigitation can be selectively switched on and off using temperature ramps, and the critical temperatures can be further determined by molecular design. Our findings suggest that synthetic vesicles, with different energy states and unexpected transition pathways, emulate dynamic cellular vesicles in nature. We anticipate that vesicles with an activated OEG corona conformation will open new routes for nanomedicine and advanced materials.
超分子化学领域在使系统远离平衡态以实现传统上难以获得的结构和功能方面取得了巨大进展。具有复杂能量景观和途径的囊泡组装体，类似于外泌体等多种细胞囊泡，仍然极为罕见。在这里，依靠寡聚乙二醇（OEG）交叉排列的激活以及单分散Janus树枝状大分子中编码的构象自由度，我们揭示了丰富的景观和不同囊泡的途径选择。交叉排列可以通过温度梯度选择性地开启和关闭，并且临界温度可以通过分子设计进一步确定。我们的研究结果表明，具有不同能量状态和意外转变途径的合成囊泡模拟了自然界中的动态细胞囊泡。我们预计，具有激活的OEG冠层构象的囊泡将为纳米医学和先进材料开辟新途径。
