Optimal Reactivity and Improved Self-Healing Capability of Structurally-Dynamic Polymers Grafted on Janus Nanoparticles Governed by Chain Stiffness and Spatial Organization
Optimal Reactivity and Improved Self-Healing Capability of Structurally-Dynamic Polymers Grafted on Janus Nanoparticles Governed by Chain Stiffness and Spatial Organization
复制标题
由链刚度和空间组织控制的 Janus 纳米粒子上接枝的结构动态聚合物的最佳反应性和改进的自愈能力
作者：
Guoxi Xu;Zihan Huang;Pengyu Chen;Tianqi Cui;张兴华;苗兵;燕立唐
结构动态聚合物被认为是一个关键的潜力，革命性的技术，从设计的自我修复材料，以众多的生物医学应用。尽管在这一领域进行了大量的研究，但优化反应性，从而在最基本的水平上提高自修复能力，这对这些新兴材料的更广泛应用提出了紧迫的问题。在这里，作者报告了通过结合大规模计算机模拟，理论分析和实验讨论，对反应性和自修复能力对动态聚合物固有性质的依赖性的基本原理的第一次机械研究。结果允许揭示链刚度和空间组织如何调节接枝在Janus纳米颗粒上的动态聚合物的反应性以及在其反向化学中的机械介导反应，特别是确定半柔性动态聚合物具有最佳反应性和自修复能力。作者还开发了一个分析模型的大滴理论的聚合物链，以补充模拟结果，并揭示最佳反应性的基本标度律。这些发现为涉及反向/动态化学的各种系统的物理机制提供了新的见解。这些研究突出了聚合物结构和固有特性的分子工程作为控制具有优化自修复能力的新兴材料的结构响应和功能的通用策略。
Structurally dynamic polymers are recognized as a key potential to revolutionize technologies ranging from design of self‐healing materials to numerous biomedical applications. Despite intense research in this area, optimizing reactivity and thereby improving self‐healing ability at the most fundamental level pose urgent issue for wider applications of such emerging materials. Here, the authors report the first mechanistic investigation of the fundamental principle for the dependence of reactivity and self‐healing capabilities on the properties inherent to dynamic polymers by combining large‐scale computer simulation, theoretical analysis, and experimental discussion. The results allow to reveal how chain stiffness and spatial organization regulate reactivity of dynamic polymers grafted on Janus nanoparticles and mechanically mediated reaction in their reverse chemistry, and, particularly, identify that semiflexible dynamic polymers possess the optimal reactivity and self‐healing ability. The authors also develop an analytical model of blob theory of polymer chains to complement the simulation results and reveal essential scaling laws for optimal reactivity. The findings offer new insights into the physical mechanism in various systems involving reverse/dynamic chemistry. These studies highlight molecular engineering of polymer architecture and intrinsic property as a versatile strategy in control over the structural responses and functionalities of emerging materials with optimized self‐healing capabilities.