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CO2 Stimuli-Responsive, Injectable Block Copolymer Hydrogels Cross-Linked by Discrete Organoplatinum(II) Metallacycles via Stepwise Post-Assembly Polymerization
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2017-09-20 00:00:00 , DOI: 10.1021/jacs.7b07303
Wei Zheng 1 , Guang Yang 2 , Nannan Shao 3 , Li-Jun Chen 1 , Bo Ou 1 , Shu-Ting Jiang 1 , Guosong Chen 2 , Hai-Bo Yang 1
Affiliation  

Supramolecular polymeric gels cross-linked by well-defined, discrete metal–organic macrocycles (MOMs) or metal–organic cages have become a prevailing topic within the field of supramolecular self-assembly. However, the realization of supramolecular polymeric hydrogels cross-linked by discrete organometallic architectures with good biocompatibility is still a great challenge. Herein, we present the successful preparation of CO2 stimuli-responsive, injectable block copolymer hydrogels cross-linked by discrete organoplatinum(II) metallacycles. Through the combination of coordination-driven self-assembly and stepwise post-assembly polymerization, star block copolymers (SBCPs) containing well-defined hexagonal metallacycles as cores were successfully prepared, which featured CO2 stimuli-responsive properties including CO2-triggered morphology transition and CO2-induced thermoresponsive behavior. Interestingly, the resultant SBCPs were capable of forming supramolecular hydrogels with MOMs as junctions near physiological temperature, which allowed the realization of a reversible gel-to-sol transformation through the removal and addition of CO2. More importantly, the resultant supramolecular hydrogels presented good cytocompatibility in vitro. Therefore, this study provides a new strategy for the construction of new “smart” supramolecular hydrogels with promising applications as biological materials.

中文翻译:

离散有机铂(II)金属环通过逐步组装后聚合作用交联的CO 2刺激响应性,可注射嵌段共聚物水凝胶。

通过定义明确的,离散的金属有机大环(MOM)或金属有机笼子交联的超分子聚合凝胶已成为超分子自组装领域的一个主要话题。然而,通过具有良好生物相容性的离散有机金属结构交联的超分子聚合物水凝胶的实现仍然是巨大的挑战。在这里,我们目前成功地制备了由离散的有机铂(II)金属环交联的CO 2刺激响应,可注射的嵌段共聚物水凝胶。通过配位驱动的自组装与逐步的后组装聚合相结合,成功制备了以明确的六角形金属环为核的星型嵌段共聚物(SBCP)。2种刺激响应特性,包括CO 2触发的形态转变和CO 2诱导的热响应行为。有趣的是,所得的SBCPs能够与MOMs形成超分子水凝胶,并在生理温度附近成为连接点,从而通过去除和添加CO 2实现了可逆的凝胶-溶胶转化。更重要的是,所得的超分子水凝胶在体外具有良好的细胞相容性。因此,这项研究为构建新型的“智能”超分子水凝胶提供了新的策略,并有望作为生物材料应用。
更新日期:2017-09-20
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