Generic Concept to Program the Time Domain of Self-Assemblies with a Self-Regulation Mechanism
Generic Concept to Program the Time Domain of Self-Assemblies with a Self-Regulation Mechanism
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DOI：
10.1021/nl5039506
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发表时间：
2015-04-01
期刊：
影响因子：
10.8
通讯作者：
Walther, Andreas
中科院分区：
文献类型：
--
作者：
Heuser, Thomas;Steppert, Ann-Kathrin;Walther, Andreas
大自然通过反馈循环、动力学控制的转化以及能量耗散来调节空间和时间中的复杂结构，以允许非平衡过程。虽然人造的静态自组装通过分子编程实现了对层次结构的良好控制，但通过自我调节来管理它们的时间命运在很大程度上是一个未解决的挑战。在这里，我们介绍了一个通用的概念，通过编程的寿命在封闭系统中的可切换的自组装控制的时域。我们设想休眠的失活剂，与快速启动子相结合，使一个独特的动力学平衡，建立一个自主自我调节，瞬时pH值状态，其持续时间可以编程的数量级，从几分钟到几天。将这种非平衡状态与pH可切换的自组装体相结合，可以及时预测它们的组装/分解命运，类似于精确的自毁机制。我们展示了一个平台的方法，通过编程的自组装寿命的嵌段共聚物，纳米粒子和肽，使动态材料的自我调节功能。
Nature regulates complex structures in space and time via feedback loops, kinetically controlled transformations, and under energy dissipation to allow non-equilibrium processes. Although man-made static self-assemblies realize excellent control over hierarchical structures via molecular programming, managing their temporal destiny by self-regulation is a largely unsolved challenge. Herein, we introduce a generic concept to control the time domain by programming the lifetimes of switchable self-assemblies in closed systems. We conceive dormant deactivators that, in combination with fast promoters, enable a unique kinetic balance to establish an autonomously self-regulating, transient pH-state, whose duration can be programmed over orders of magnitude-from minutes to days. Coupling this non-equilibrium state to pH-switchable self-assemblies allows predicting their assembly/disassembly fate in time, similar to a precise self-destruction mechanism. We demonstrate a platform approach by programming self-assembly lifetimes of block copolymers, nanoparticles, and peptides, enabling dynamic materials with a self-regulation functionality.