Towards dual light control of a catalytically-driven chemical reaction cycle

31 January 2024, Version 2
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

Chemically-fueled chemical reaction networks (CRNs) are key in controlling dissipative self-assembly. Having catalysts gating fuel consumption for both the activation and deactivation chemistry of (assembly-prone) monomers and controlling the catalytic activity with an external stimulus would provide better control over where, when, and how long self-assembled structures can form. Here we achieve light control over monomer activation and subsequent assembly into supramolecular fibers, and partial light control over deactivation and fiber disassembly. Activation proceeds via photoredox catalysis under visible light, whereas deactivation is achieved by organometallic catalysis that relies on a photocaged pre-fuel activated by ultraviolet light. Overall, we show how supramolecular fibers can be formed by visible light and how their destruction is accelerated by ultraviolet light.

Keywords

Dissipative self-assembly
out-of-equilibrium
chemical reaction cycle
photoredox catalysis
chemical fuels

Supplementary materials

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Description
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Supporting Information
Description
1. Materials and Methods 2. Synthetic details and characterization 3. Supporting Figures
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Supporting Video 1
Description
Activation/Assembly followed by Deactivation/Dis-assembly both by light.
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