期刊
NANO LETTERS
卷 15, 期 4, 页码 2213-2219出版社
AMER CHEMICAL SOC
DOI: 10.1021/nl5039506
关键词
Non-Equilibrium Self-Assembly; Self-Regulation; Programmable Materials; Time Domain; Switchable Materials; Dynamic Properties
类别
资金
- DFG [WA3084/4-1]
- [SFB 985]
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.
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