Publication

Back to overview

A homogeneous transition metal complex for clean hydrogen production from methanol-water mixtures.

Type of publication Peer-reviewed
Publikationsform Original article (peer-reviewed)
Publication date 2013
Author Rodríguez-Lugo Rafael E, Trincado Mónica, Vogt Matthias, Tewes Friederike, Santiso-Quinones Gustavo, Grützmacher Hansjörg,
Project Unconventional Approaches to the Activation of Dihydrogen (FOR 1175) (D-A-CH/LAE)
Show all

Original article (peer-reviewed)

Journal Nature chemistry
Volume (Issue) 5(4)
Page(s) 342 - 7
Title of proceedings Nature chemistry
DOI 10.1038/nchem.1595

Abstract

The development of an efficient catalytic process that mimics the enzymatic function of alcohol dehydrogenase is critical for using biomass alcohols for both the production of H2 as a chemical energy carrier and fine chemicals under waste-free conditions. Dehydrogenation of alcohol-water mixtures into their corresponding acids with molecular hydrogen as the sole by-product from the reaction can be catalysed by a ruthenium complex with a chelating bis(olefin) diazadiene ligand. This complex, [K(dme)2][Ru(H)(trop2dad)], stores up to two equivalents of hydrogen intramolecularly, and catalyses the production of H2 from alcohols in the presence of water and a base under homogeneous conditions. The conversion of a MeOH-H2O mixture proceeds selectively to CO2/H2 gas formation under neutral conditions, thereby allowing the use of the entire hydrogen content (12% by weight). Isolation and characterization of the ruthenium complexes from these reactions suggested a mechanistic scenario in which the trop2dad ligand behaves as a chemically 'non-innocent' co-operative ligand.
-