Photoinitiated Transient Self‐Assembly in a Catalytically Driven Chemical Reaction Cycle

Abstract: Chemically fueled chemical reaction networks (CRNs) are essential in controlling dissipative self‐assembly. A key challenge in the field is to store chemical fuel‐precursors or “pre‐fuels” in the system that are converted into activating or deactivating fuels in a catalytically controlled CRN. In addition, real‐time control over catalysis in a CRN by light is highly desirable, but so far not yet achieved. Here we show a catalytically driven CRN that is photoinitiated with 450 nm light, producing activated monomers that go on to perform transient self‐assembly. Monomer activation proceeds via photoredox catalysis, converting the monomer alcohol groups into the corresponding aldehydes that self‐assemble into large supramolecular fibers. Monomer deactivation is achieved by organometallic catalysis that relies on pre‐fuel hydrolysis to release formate (i.e. the deactivating fuel). Additionally, irradiation with 305 nm light accelerates the release of formate by photo‐uncaging the pre‐fuel, leading to a factor of ca. 2 faster deactivation of the monomer. Overall, we show transient self‐assembly upon visible light photoactivation, and tunable life‐times by ultraviolet light.

Location
Deutsche Nationalbibliothek Frankfurt am Main
Extent
Online-Ressource
Language
Englisch

Bibliographic citation
Photoinitiated Transient Self‐Assembly in a Catalytically Driven Chemical Reaction Cycle ; day:30 ; month:06 ; year:2024 ; extent:6
Angewandte Chemie / International edition. International edition ; (30.06.2024) (gesamt 6)

Creator
Valera, Jorge S.
López‐Acosta, Álvaro
Hermans, Thomas M.

DOI
10.1002/anie.202406931
URN
urn:nbn:de:101:1-2407011407131.384312327096
Rights
Open Access; Der Zugriff auf das Objekt ist unbeschränkt möglich.
Last update
14.08.2025, 10:54 AM CEST

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Associated

  • Valera, Jorge S.
  • López‐Acosta, Álvaro
  • Hermans, Thomas M.

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