Dai Kun, Tena-Solsona Marta, Rodon Fores Jennifer, Bergmann Alexander M, Boekhoven Job
Department of Chemistry, Technical University of Munich, Lichtenbergstrasse 4, 85748 Garching, Germany.
Institute for Advanced Study, Technical University of Munich, Lichtenbergstrasse 2a, 85748 Garching, Germany.
Nanoscale. 2021 Dec 13;13(47):19864-19869. doi: 10.1039/d1nr04954b.
In chemically fueled self-assembly, a reaction cycle activates and deactivates molecules for self-assembly. The resulting assembly is dynamic and should be endowed with unique behavior in this kinetically controlled regime. Recent works have mainly focused on design rules for the activation of molecules for self-assembly, thereby assuming that disassembly upon deactivation inherently follows. However, that is not always the case. This work shows a family of peptides that assemble into colloids regulated through a chemical reaction cycle. Despite their similarity in assembly, we find that they follow a different disassembly pathway upon deactivation. The colloids from several peptides completely disassemble as fuel depletes while others transition into fibers. Our findings demonstrate that assembly and disassembly should be taken into account in chemically fueled self-assembly.
在化学驱动的自组装中,一个反应循环激活并失活用于自组装的分子。由此产生的组装体是动态的,并且在这种动力学控制的体系中应具有独特的行为。最近的研究主要集中在用于自组装的分子激活的设计规则上,从而假定失活时的解组装是固有的后续过程。然而,情况并非总是如此。这项工作展示了一类通过化学反应循环调控组装成胶体的肽。尽管它们在组装上相似,但我们发现它们在失活时遵循不同的解组装途径。随着燃料耗尽,几种肽形成的胶体完全解组装,而其他的则转变为纤维。我们的研究结果表明,在化学驱动的自组装中应同时考虑组装和解组装。