期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 19, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202201573
关键词
Chemical Reaction Network; Chemo-Structural Feedback; Colloids; Systems Chemistry; pH-Feedback System
资金
- European Union [812868]
- MPI Minerva ARCHES Program
- Gutenberg Research College
- Projekt DEAL
- Marie Curie Actions (MSCA) [812868] Funding Source: Marie Curie Actions (MSCA)
Biological self-assemblies can self- and cross-regulate each other through chemical reaction networks and feedback. In this study, a rational design approach for chemo-structural feedback was introduced, and a transient colloidal co-assembly system was presented. The formed co-assemblies could autonomously accelerate their destruction. This research introduces versatile mechanisms for chemo-structural feedback.
Biological self-assemblies self- and cross-regulate each other via chemical reaction networks (CRNs) and feedback. Although artificial transient self-assemblies have been realized via activation/deactivation CRNs, the transient structures themselves do mostly not engage in the CRN. We introduce a rational design approach for chemo-structural feedback, and present a transient colloidal co-assembly system, where the formed co-assemblies accelerate their destruction autonomously. We achieve this by immobilizing enzymes of a deactivating acid-producing enzymatic cascade on pH-switchable microgels that can form co-assemblies at high pH. Since the enzyme partners are immobilized on individual microgels, the co-assembled state brings them close enough for enhanced acid generation. The amplified deactivator production (acid) leads to an almost two-fold reduction in the lifetime of the transiently formed pH-state. Our study thus introduces versatile mechanisms for chemo-structural feedback.
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