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Plasmon-Induced Optical Control over Dithionite-Mediated Chemical Redox Reactions

Abstract

External-stimuli controlled reversible formation of radical species is of great interest for synthetic and supramolecular chemistry, molecular machinery, as well as emerging technologies ranging from (photo)catalysis and photovoltaics to nanomedicine. Here, we show a novel hybrid colloidal system for light-driven reversible reduction of chemical species that, on their own, do not respond to light. This is achieved by the unique combination of photo-sensitive plasmonic aggregates and temperature-responsive inorganic species generating radicals that can be finally accepted and stabilised by non photo-responsive organic molecules. In this system Au nanoparticles (NPs) self-assembled via sub-nm precise molecular spacers (cucurbin[n]urils) interact strongly with visible light to locally accelerate the decomposition of dithionite species (S2O42-) close to the NP interfaces. This light-driven process leads to the generation of inorganic radicals whose electrons can then be reversibly picked up by small organic acceptors, such as the methylviologen molecules (MV2+) used here. During light-triggered plasmon- and heat-assisted generation of radicals, the S2O42- species work as a chemical ‘fuel’ linking photo-induced processes at the NP interfaces with redox chemistry in the surrounding water environment. By incorporating MV2+ as a Raman-active reporter molecule, the resulting optically-controlled redox processes can be followed in real-time.

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Publication details

The article was received on 16 Oct 2018, accepted on 08 Nov 2018 and first published on 27 Nov 2018


Article type: Paper
DOI: 10.1039/C8FD00155C
Citation: Faraday Discuss., 2018, Accepted Manuscript
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    Plasmon-Induced Optical Control over Dithionite-Mediated Chemical Redox Reactions

    J. Huang, B. de Nijs, S. Cormier, K. Sokolowski, D. Grys, C. A. Readman, S. J. Barrow, O. A. Scherman and J. J. Baumberg, Faraday Discuss., 2018, Accepted Manuscript , DOI: 10.1039/C8FD00155C

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