Sheikh Idris Samahir, Wang Hucheng, Gao Yuliang, Cai Peiwen, Wang Yiming, Zhao Shicheng
State Key Laboratory of Chemical Engineering, Shanghai Key Laboratory of Multiphase Materials Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China.
Gels. 2025 Apr 14;11(4):289. doi: 10.3390/gels11040289.
Spatial control over molecular self-assembly at the nano scale offers great potential for many high-tech applications, yet remains a challenging task. Here, we report a polymer brush-mediated strategy to confine the self-assembly of hydrazone-based hydrogelators exclusively at nanoparticle surfaces. The surfaces of these nanoparticles are grafted with negatively charged polyacrylic acid, which enrich protons that can catalyze the in situ formation and self-assembly of hydrazone-based gelators. We found that, with respect to the polymer lengths, the concentration of the nanoparticles presents more significant effects on the self-assembly process and the properties of the resultant hydrogels, including gelation time, stiffness, and network morphology. More interestingly, the hydrogel fibers are found to be formed specifically around the nanoparticles, demonstrating the directed nanoscale molecular self-assembly. This work demonstrates that triggering molecular self-assembly using catalysis can serve as an effective way to realize directed molecular self-assembly at the nano scale, which may serve as a powerful approach to improve many material properties, such as the mechanical properties of supramolecular materials as we found in this work.
在纳米尺度上对分子自组装进行空间控制在许多高科技应用中具有巨大潜力，但仍然是一项具有挑战性的任务。在此，我们报告一种聚合物刷介导的策略，将基于腙的水凝胶剂的自组装限制在纳米颗粒表面。这些纳米颗粒的表面接枝有带负电荷的聚丙烯酸，其富集可催化基于腙的凝胶剂原位形成和自组装的质子。我们发现，相对于聚合物长度，纳米颗粒的浓度对自组装过程和所得水凝胶的性质（包括凝胶化时间、硬度和网络形态）具有更显著的影响。更有趣的是，发现水凝胶纤维专门在纳米颗粒周围形成，展示了定向纳米尺度分子自组装。这项工作表明，利用催化触发分子自组装可作为在纳米尺度上实现定向分子自组装的有效方法，这可能是改善许多材料性质（如我们在这项工作中发现的超分子材料的机械性质）的有力途径。
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