Journal ArticleDOI
Visible-Light-Driven Alcohol Dehydrogenation with a Rhodium Catalyst
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TLDR
In this paper, the photocatalytic dehydrogenation of alcohols with a Rh catalyst and I− in an acidic medium was reported, which increased linearly for 4 days with no significant decrease in activity.Abstract:
We report the photocatalytic dehydrogenation of alcohols with a Rh catalyst and I− in an acidic medium. The catalyst screening of a structurally diverse family of Rh complexes found [RhIII(dtbbpy)2(OSO2CF3)2](CF3SO3) (Rh7; dtbbpy=4,4′-di-tert-butyl-2,2′-bipyridine) to be the best catalyst. All components (Rh7, HI, alcohol, and light) were found to be essential for the dehydrogenation to occur. Under optimal conditions, generation of both H2 and acetone (for isopropyl alcohol) was observed, which increased linearly for 4 days with no significant decrease in activity. The proposed mechanism involves the formation of [RhIII(dtbbpy)2(I)2]+ [Rh7(a)] followed by the generation of photoinduced I3− via a ligand (I−) to metal (RhIII) charge transfer. The resulting RhI species reduces H+ and I3− oxidizes the alcohol, which completes the catalytic cycle. Supporting evidence for the catalytic mechanism was obtained by using UV/Vis spectroscopy, electrospray ionization mass spectrometry, cyclic voltammetry and time-dependent DFT calculations.read more
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Journal ArticleDOI
Hierarchical Integration of Photosensitizing Metal-Organic Frameworks and Nickel-Containing Polyoxometalates for Efficient Visible-Light-Driven Hydrogen Evolution.
Xiang-Jian Kong,Xiang-Jian Kong,Zekai Lin,Zhi-Ming Zhang,Zhi-Ming Zhang,Teng Zhang,Wenbin Lin,Wenbin Lin +7 more
TL;DR: This work shows that POM@MOF assemblies not only provide a tunable platform for designing highly effective photocatalytic HER catalysts but also facilitate detailed mechanistic understanding of HER processes.
Journal ArticleDOI
Homogeneously catalyzed acceptorless dehydrogenation of alcohols: A progress report
TL;DR: In this paper, an overview of recent progress in homogeneously catalyzed acceptorless alcohol dehydrogenation is presented in which the introduction of multifunctional cooperative ligands in the coordination sphere of the metal center in order to improve catalytic activity under photochemical, electrochemical or thermal conditions is discussed.
Journal ArticleDOI
Light-Driven Hydrogen Generation from Microemulsions Using Metallosurfactant Catalysts and Oxalic Acid
TL;DR: Mechanistic insights were provided by gas-phase Raman, electrochemical, and luminescence quenching analysis, suggesting oxidative quenched to be the principle reaction pathway.
Journal ArticleDOI
Iridium(III) Bis-Pyridine-2-Sulfonamide Complexes as Efficient and Durable Catalysts for Homogeneous Water Oxidation.
TL;DR: A family of tetradentate bis(pyridine-2-sulfonamide) (bpsa) compounds was synthesized as a ligand platform for designing resilient and electronically tunable catalysts capable of performing water oxidation catalysis and other processes in highly oxidizing environments.
Journal ArticleDOI
Rational design of carbon support to prepare ultrafine iron oxide catalysts for air oxidation of alcohols
TL;DR: In this article, a mesoporous carbon support with abundant surface functional groups and a tunable pore size was proposed for fabricating ultrafine iron oxide catalysts, and the resultant catalysts exhibit an obviously higher activity in air oxidation of several benzyl alcohols compared with the catalysts with other synthetic carbon as supports.
References
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