Please use this identifier to cite or link to this item:
http://doi.org/10.25358/openscience-9153
Authors: | Sittel, Steven Sell, Arne Christian Hofmann, Kamil Wiedemann, Christina Nau, Jan Philipp Kerzig, Christoph Manolikakes, Georg Heinze, Katja |
Title: | Visible-light induced fixation of SO2 into organic molecules with polypyridine chromium(III) complexes |
Online publication date: | 7-Jun-2023 |
Year of first publication: | 2023 |
Language: | english |
Abstract: | Incorporation of sulfur dioxide into organic compounds is achieved by a photocatalytic approach using sensitizers made from earth-abundant chromium(III) ions and visible light leading to sulfones and sulfonamides. We employed three different chromium(III) sensitizers [Cr(ddpd)2]3+, [Cr(bpmp)2]3+ and [Cr(tpe)2]3+ with long excited state lifetimes and different ground and excited state redox potentials as well as varying stability under the reaction conditions (ddpd=N,N’-dimethyl-N,N’-dipyridin-2-yl-pyridine-2,6-diamine; bpmp=2,6-bis(2-pyridylmethyl)pyridine; tpe=1,1,1-tris(pyrid-2-yl)ethane). Key reaction steps of the catalytic cycles are identified by electrochemical, luminescence quenching, photolysis, laser flash photolysis and catalytic experiments delivering a detailed picture of the challenges in these transformations. The reactivity of the reduced chromium complex was identified as a key property to explain the reaction outcomes. Initial cage escape yield determinations with [Cr(tpe)2]3+ revealed that desired photoreactions occur with unusually high quantum efficiencies, whereas side reactions are almost unproductive. |
DDC: | 540 Chemie 540 Chemistry and allied sciences |
Institution: | Johannes Gutenberg-Universität Mainz |
Department: | FB 09 Chemie, Pharmazie u. Geowissensch. |
Place: | Mainz |
ROR: | https://ror.org/023b0x485 |
DOI: | http://doi.org/10.25358/openscience-9153 |
Version: | Published version |
Publication type: | Zeitschriftenaufsatz |
License: | CC BY-NC |
Information on rights of use: | https://creativecommons.org/licenses/by-nc/4.0/ |
Journal: | ChemCatChem 15 6 |
Pages or article number: | e202201562 |
Publisher: | Wiley-VCH |
Publisher place: | Weinheim |
Issue date: | 2023 |
ISSN: | 1867-3899 |
Publisher DOI: | 10.1002/cctc.202201562 |
Appears in collections: | DFG-491381577-H |
Files in This Item:
File | Description | Size | Format | ||
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visiblelight_induced_fixation-20230605215506683.pdf | 358.95 kB | Adobe PDF | View/Open |