Gezielte Optimierung von molekularen Photokatalysatoren zur Wasserstoffproduktion mit sichtbarem Licht

Pfeffer, Michael; Kowacs, Tanja; Wächtler, Maria; Guthmuller, Julien; Dietzek, Benjamin; Vos, Johannes G.; Rau, Sven

doi:10.1002/ange.201409442

Cited by 26 publications

(1 citation statement)

References 47 publications

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“…A different approach was taken by Rau and his coworkers. They developed photochemical molecular devices (PMDs) and used them for various reduction reactions [ 125 , 126 , 127 , 128 , 129 , 130 , 131 , 132 , 133 ]. These PMDs consist of three structural units ( Figure 7 ): a photoactive Ru II complex fragment that acts as a light absorber, a catalytic center (in the chosen example, a [Rh III Cp*Cl] moiety, Cp* = C 5 Me 5 ), and a bridging unit that connects the two metals via a conjugated reducible π-electron system [ 129 , 133 ].…”

Section: Heterobimetallic Complexes In Homogeneous Catalysismentioning

confidence: 99%

Added Complexity!—Mechanistic Aspects of Heterobimetallic Complexes for Application in Homogeneous Catalysis

Fickenscher

Hey‐Hawkins

2023

Molecules

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Inspired by multimetallic assemblies and their role in enzyme catalysis, chemists have developed a plethora of heterobimetallic complexes for application in homogeneous catalysis. Starting with small heterobimetallic complexes with σ-donating and π-accepting ligands, such as N-heterocyclic carbene and carbonyl ligands, more and more complex systems have been developed over the past two decades. These systems can show a significant increase in catalytic activity compared with their monometallic counterparts. This increase can be attributed to new reaction pathways enabled by the presence of a second metal center in the active catalyst. This review focuses on mechanistic aspects of heterobimetallic complexes in homogeneous catalysis. Depending on the type of interaction of the second metal with the substrates, heterobimetallic complexes can be subdivided into four classes. Each of these classes is illustrated with multiple examples, showcasing the versatility of both, the types of interactions possible, and the reactions accessible.

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Section: Heterobimetallic Complexes In Homogeneous Catalysismentioning

confidence: 99%

Added Complexity!—Mechanistic Aspects of Heterobimetallic Complexes for Application in Homogeneous Catalysis

Fickenscher

Hey‐Hawkins

2023

Molecules

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Unraveling the Light‐Activated Reaction Mechanism in a Catalytically Competent Key Intermediate of a Multifunctional Molecular Catalyst for Artificial Photosynthesis

et al. 2019

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Understanding photodriven multielectron reaction pathwaysrequires the identification and spectroscopic characterization of intermediates and their excited-state dynamics, which is very challenging due to their short lifetimes.Tothe best of our knowledge,this manuscript reports for the first time on in situ spectroelectrochemistry as an alternative approach to study the excited-state properties of reactive intermediates of photocatalytic cycles.U V/Vis,r esonance-Raman, and transient-absorption spectroscopyhave been employed to characterizet he catalytically competent intermediate [(tbbpy) 2 Ru II -(tpphz)Rh I Cp*] of [(tbbpy) 2 Ru(tpphz)Rh(Cp*)Cl]Cl(PF 6 ) 2 (Ru(tpphz)RhCp*), ap hotocatalyst for the hydrogenation of nicotinamide (NAD-analogue) and proton reduction, generated by electrochemical and chemical reduction. Electronic transitions shifting electron density from the activated catalytic center to the bridging tpphz ligand significantly reduce the catalytic activity upon visible-light irradiation.

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Umwandlung vonEscherichia coliProteomembranen in artifizielle Chloroplasten durch molekulare Photokatalyse

et al. 2022

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In der lichtabhängigen Reaktion der Photosynthese koppeln grüne Pflanzen photoinduzierte Kaskaden von Redoxreaktionen mit transmembranen Protonentransfers um Reduktionsäquivalente und chemische Energie in Form von NADPH (Nikotinamidadenindinukleotidphosphat) und ATP (Adenosintriphosphat) zu erzeugen. Wir imitieren diese grundlegenden Prozesse durch Kombination von molekularen Rutheniumpolypyridinkomplexen und invertierten Vesikeln, die aus Escherichia coli gewonnen werden. Bei Bestrahlung mit sichtbarem Licht führt das Zusammenspiel von photokatalytischer Nikotinamidreduktion und enzymatischer, membranlokalisierter Atmung zur gleichzeitigen Bildung der beiden biologisch aktiven Cofaktoren NADH (Nikotinamidadenindinukleotid) und ATP. Dieses anorganisch‐biologische Hybridsystem ahmt daher die Cofaktor‐bereitstellende Funktion eines aktiven Chloroplasten nach.

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Gezielte Optimierung von molekularen Photokatalysatoren zur Wasserstoffproduktion mit sichtbarem Licht

Abstract: In einem intramolekularen Photokatalysator,b estehend aus einem Ru II

Cited by 26 publications

References 47 publications

Added Complexity!—Mechanistic Aspects of Heterobimetallic Complexes for Application in Homogeneous Catalysis

Added Complexity!—Mechanistic Aspects of Heterobimetallic Complexes for Application in Homogeneous Catalysis

Unraveling the Light‐Activated Reaction Mechanism in a Catalytically Competent Key Intermediate of a Multifunctional Molecular Catalyst for Artificial Photosynthesis

Umwandlung vonEscherichia coliProteomembranen in artifizielle Chloroplasten durch molekulare Photokatalyse

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