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Mechanistic Insights into Ruthenium-Catalyzed Production of H2 and CO2 from Methanol and Water: A DFT Study

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journal contribution
posted on 04.04.2014, 00:00 by Xinzheng Yang
A density functional theory study of the reaction mechanism of the production of H2 and CO2 from methanol and water catalyzed by an aliphatic PNP pincer ruthenium complex, (PNP)­Ru­(H)­CO, reveals three interrelated catalytic cycles for the release of three H2 molecules: the dehydrogenation of methanol to formaldehyde, the coupling of formaldehyde and hydroxide for the formation of formic acid, and the dehydrogenation of formic acid. The formation of all three H2 molecules undergoes the same self-promoted mechanism that features a methanol or a water molecule acting as a bridge for the transfer of a ligand proton to the metal hydride in a key intermediate, trans-(HPNP)­Ru­(H)2CO.