Visible-Light-Induced Homolysis of Earth-Abundant Metal-Substrate Complexes: A Complementary Activation Strategy in Photoredox Catalysis.
Durch sichtbares Licht induzierte Homolyse unedler, gut verfügbarer Metallsubstratkomplexe: Eine komplementäre Aktivierungsstrategie in der Photoredoxkatalyse

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urn:nbn:de:bvb:355-epub-525496 Copy

Abderrazak, Youssef ; Bhattacharyya, Aditya ; Reiser, Oliver

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Date of publication of this fulltext: 01 Jul 2022 08:42

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Details

Item type:	Article
Journal or Publication Title:	Angew.Chem.Int. Ed.
Publisher:	Wiley
Volume:	60
Page Range:	pp. 21100-21115
Date:	18 February 2021
Institutions:	Chemistry and Pharmacy > Institut für Organische Chemie > Lehrstuhl Prof. Dr. Oliver Reiser
Projects:	DFG RE 948/18-1, H2020 Marie Skłodowska-Curie Actions. Grant Number: 795161
Identification Number:	Value Type 10.1002/anie.202100270 DOI
Keywords:	3d transition metals, dissociative ligand-to-metal charge transfer, inner-sphere electron transfer, photoredox catalysis, visible-light-induced homolysis
Dewey Decimal Classification:	500 Science > 540 Chemistry & allied sciences
Status:	Published
Refereed:	Yes, this version has been refereed
Created at the University of Regensburg:	Yes
Item ID:	52549

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Abstract

The mainstream applications of visible-light photoredox catalysis predominately involve outer-sphere single-electron transfer (SET) or energy transfer (EnT) processes of precious metal RuII or IrIII complexes or of organic dyes with low photostability. Earth-abundant metal-based MnLn-type (M=metal, Ln=polydentate ligands) complexes are rapidly evolving as alternative photocatalysts as they offer ...

Abstract

The mainstream applications of visible-light photoredox catalysis predominately involve outer-sphere single-electron transfer (SET) or energy transfer (EnT) processes of precious metal RuII or IrIII complexes or of organic dyes with low photostability. Earth-abundant metal-based MnLn-type (M=metal, Ln=polydentate ligands) complexes are rapidly evolving as alternative photocatalysts as they offer not only economic and ecological advantages but also access to the complementary inner-sphere mechanistic modes, thereby transcending their inherent limitations of ultrashort excited-state lifetimes for use as effective photocatalysts. The generic process, termed visible-light-induced homolysis (VLIH), entails the formation of suitable light-absorbing ligated metal–substrate complexes (MnLn-Z; Z=substrate) that can undergo homolytic cleavage to generate Mn−1Ln and Z. for further transformations.
Die Hauptanwendungen der Photoredoxkatalyse mit sichtbarem Licht umfassen vorwiegend in der äußeren Sphäre des Katalysators stattfindende SET- oder EnT-Prozesse, ausgelöst durch Edelmetall-RuII- oder -IrIII-Komplexe oder durch organische Farbstoffe mit geringer Photostabilität. Gut verfügbare MnLn-Metallkomplexe entwickeln sich schnell als alternative Photokatalysatoren, denn sie bieten wirtschaftliche und ökologische Vorteile und eröffnen den Zugang zu mechanistisch komplementären Innersphären-Modi; damit lassen sich die inhärenten Einschränkungen, die aufgrund von ultrakurzen Lebensdauern im angeregten Zustand ihrer Anwendung entgegenstehen, überwinden. Das allgemeine Verfahren, das als durch sichtbares Licht induzierte Homolyse (VLIH) bezeichnet wird, umfasst die Bildung geeigneter lichtabsorbierender Metall-Substrat-Komplexe (MnLn-Z; Z=Substrat), die eine homolytische Spaltung zu Mn−1Ln und Z. als Startpunkt für weitere Transformationen eingehen.

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