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  Ru(N2P2Cl2) Noyori-type hydrogenation catalyst

Ru-complexes with an N2P2Cl2 ligand set are used as hydrogenation catalysts, even to perform enantioselective hydrogenation (Noyori). The Ru(II) central atom is redox active and can be oxidized to Ru(III).
We characterize the thermodynamics and the mechanism of this redox reaction with cyclic voltammetry. In particular, combinatorial redox screening techniques CombiSECM are employed to quickly determine the voltammetric properties of extended collections of such complexes. It appears that the qualitative shape of the voltammograms correlates with their catalytic activity (C=O vs. C=C hydrogenation in α,β-unsaturated carbonyl compounds).
The catalytically active complexes are bound by means of a siloxan-spacer to Pt metal surfaces or to Stöber silica nanoparticles. In the former case, chemically modified electrodes are generated.

Coworkers in this project

Filip Novak, Nicolas Plumeré, Diana Straub and Carsten Tittel

We closely cooperate with the group of Hermann A. Mayer.

We acknowledge funding of this project by the Deutsche Forschungsgemeinschaft, Bonn - Bad Godesberg (within the Graduiertenkolleg "Chemie in Interphasen") and the Max-Buchner-Forschungsstiftung.

Publications from this project

A. Budny, F. Novak, N. Plumeré, B. Schetter, B. Speiser, D. Straub, H.A. Mayer and M. Reginek, Langmuir 51, 10605 - 10611 (2006); Redox-Active Silica Nanoparticles. Part 1. Electrochemistry and Catalytic Activity of Spherical, Nonporous Silica Particles with Nanometric Diameters and Covalently Bound Redox-active Modifications.

F. Novak, B. Speiser, E. Lindner, Z.-L. Lu und H.A. Mayer, Angew. Chem., 116, 2059 - 2062 (2004); Elektrochemie von Übergangsmetallkatalysatoren. Teil 11. Eine chemisch modifizierte Platinelektrode als zweizähniger Diaminligand zur Bildung wohldefinierter immobilisierter Bis(η1-P-ether-phosphan)(diamin)ruthenium(II)-Komplexe; Angew. Chem. Int. Ed. 43, 2025 - 2028 (2004); Electrochemistry of Transition Metal Complex Catalysts. Part 11. A Chemically Modified Platinum Electrode as a Bidentate Diamine Ligand for Forming Well-Defined, Immobilized Bis(η1-P-ether-phosphane)(diamine)ruthenium(II) Complexes; Berichtigung: Angew. Chem., 116, 2934 (2004).

 
© AG Speiser 2011