A Single Organoiridium Complex Generating Highly Active Catalysts for both Water Oxidation and NAD+/NADH Transformations
| Autor: | Gianfranco Bellachioma, Cristiano Zuccaccia, Savannah Dunn, Gabriel Menendez Rodriguez, Alberto Bucci, Alceo Macchioni, Carlo Nervi |
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| Jazyk: | angličtina |
| Rok vydání: | 2017 |
| Předmět: |
iridium complexes
NAD+hydrogenation NADH dehydrogenation NMR water oxidation Catalysis 010405 organic chemistry Nad nadh chemistry.chemical_element General Chemistry 010402 general chemistry Photochemistry Photosynthesis 01 natural sciences Medicinal chemistry 0104 chemical sciences chemistry.chemical_compound chemistry High activity NAD+ kinase Molecular oxygen Iridium Benzoic acid |
| Popis: | The complex [Cp*Ir(pica)Cl] (1; pica = picolinamidate = κ2-pyridine-2-carboxamide) was found to be an effective catalyst for both water oxidation to molecular oxygen and NAD+/NADH transformations, which are the key reactions of light-dependent natural photosynthesis. In particular, 1 exhibits high activity in water oxidation driven by CAN and NaIO4. With the former, the initial TOF exceeds that of [Cp*Ir(pic)Cl] (2; pic = picolinate = κ2-pyridine-2-carboxylate), which is the fastest iridium catalyst reported to date, whereas with NaIO4 it compares well with the best catalysts. 1 exhibits top performances also in the hydrogenation of NAD+ with HCOOK, leading to the regiospecific formation of 1,4-NADH (pH 7) with TOF = 143 h–1, which is about 3 times higher than the previous highest value (54 h–1) reported for [Cp*Ir(4-(1H-pyrazol-1-yl-κN2)benzoic acid)(H2O)]SO4 (3). The activity seems to be critically affected by the presence of the NH functionality, as indicated by its drop of about 1 order of magnitude w... |
| Databáze: | OpenAIRE |
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