ArticleChemistry (Weinheim an der Bergstrasse, Germany)2021
Controlling Spin-Correlated Radical Pairs with Donor-Acceptor Dyads: A New Concept to Generate Reduced Metal Complexes for More Efficient Photocatalysis.
Article in Chemistry (Weinheim an der Bergstrasse, Germany), 2021. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 12 papers.
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12 citing papers in PubMed, 35 citations in OpenAlex.
- When less is more: harnessing optimal quencher concentrations to maximize quantum yields in TADF photoredox reactions.Chemical science · 2026Article
- Thermally activated delayed fluorescence photocatalysts: a kinetic model to predict time-resolved spectroscopic experiments and photoreactions under continuous irradiation.Photochemical & photobiological sciences : Official journal of the European Photochemistry Association and the European Society for Photobiology · 2026Article
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- Efficient Red Light-Driven Singlet Oxygen Photocatalysis with an Osmium-Based Coulombic Dyad.Angewandte Chemie (International ed. in English) · 2025Article
- Bichromophoric Ruthenium Complexes for Photocatalyzed Late-Stage Synthesis of Trifluoromethylated Indolizines.The Journal of organic chemistry · 2025Article
- Exploring the Photophysics and Photocatalytic Activity of Heteroleptic Rh(III) Transition-Metal Complexes Using High-Throughput Experimentation.Inorganic chemistry · 2024Article
- Mechanistic investigations of polyaza[7]helicene in photoredox and energy transfer catalysis.Beilstein journal of organic chemistry · 2024Article
- Triplet quenching pathway control with molecular dyads enables the identification of a highly oxidizing annihilator class.Chemical science · 2023Article
- Shedding Light on the Oxidizing Properties of Spin-Flip Excited States in a CrJournal of the American Chemical Society · 2022Article
- Cobalt(III) Carbene Complex with an Electronic Excited-State Structure Similar to Cyclometalated Iridium(III) Compounds.Journal of the American Chemical Society · 2022Article
- Luminescent First-Row Transition Metal Complexes.JACS Au · 2021Review
- Controlling Spin-Correlated Radical Pairs with Donor-Acceptor Dyads: A New Concept to Generate Reduced Metal Complexes for More Efficient Photocatalysis.Chemistry (Weinheim an der Bergstrasse, Germany) · 2021Article
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Authors and funding
3 authors at 1 institution in 2 countries.
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Abstract
One-electron reduced metal complexes derived from photoactive ruthenium or iridium complexes are important intermediates for substrate activation steps in photoredox catalysis and for the photocatalytic generation of solar fuels. However, owing to the heavy atom effect, direct photochemical pathways to these key intermediates suffer from intrinsic efficiency problems resulting from rapid geminate recombination of radical pairs within the so-called solvent cage. In this study, we prepared and investigated molecular dyads capable of producing reduced metal complexes via an indirect pathway relying on a sequence of energy and electron transfer processes between a Ru complex and a covalently connected anthracene moiety. Our test reaction to establish the proof-of-concept is the photochemical reduction of ruthenium(tris)bipyridine by the ascorbate dianion as sacrificial donor in aqueous solution. The photochemical key step in the Ru-anthracene dyads is the reduction of a purely organic (anthracene) triplet excited state by the ascorbate dianion, yielding a spin-correlated radical pair whose (unproductive) recombination is strongly spin-forbidden. By carrying out detailed laser flash photolysis investigations, we provide clear evidence for the indirect reduced metal complex generation mechanism and show that this pathway can outperform the conventional direct metal complex photoreduction. The further optimization of our approach involving relatively simple molecular dyads might result in novel photocatalysts that convert substrates with unprecedented quantum yields.
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