Self‐Regulating Colloidal Co‐Assemblies That Accelerate Their Own Destruction via 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 ra...

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Bibliographic Details
Published in:Angewandte Chemie International Edition 2022-05, Vol.61 (19), p.e202201573-n/a
Main Authors: Sharma, Charu, Walther, Andreas
Format: Article
Language:English
Subjects:
Assemblies
Chemical Reaction Network
Chemical reactions
Chemo-Structural Feedback
Colloids
Communication
Communications
Deactivation
Destruction
Feedback
Microgels
pH effects
pH-Feedback System
Systems Chemistry
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Summary: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. A chemo‐structural feedback mechanism is introduced in co‐assembling microgels (MGs), whereby the co‐assemblies promote their own destruction. The key concept uses co‐assembly‐triggered proximity effects of enzymes immobilized on individual MGs so that the co‐assembly enhances an enzymatic cascade for deactivator production.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202201573