Project Details
Projekt
SFB 706: Selective Catalytic Oxidation of C-H Bonds with Molecular Oxygen
Subject Area
Chemistry
Thermal Engineering/Process Engineering
Thermal Engineering/Process Engineering
Term
from 2006 to 2010
Project identifier
Deutsche Forschungsgemeinschaft (DFG) - Project number 15581711
Oxidation of C-H bonds in hydrocarbons is of great importance in laboratory syntheses, in large-scale industrial processes, and is also a relevant process in the metabolism of living cells.
Molecular oxygen is involved in many of these processes, but the great potential of this abundant, non-toxic, and sustainable oxidising agent could not be realised up to now. Reasons for this shortcoming are the relative inertness of molecular oxygen towards C-H bonds and the poor selectivity in reactions involving organic substrates.
The aim of the Collaborative Research Centre is to turn molecular oxygen into a selective oxidising agent for organic substrates. The activation of molecular oxygen and the oxidation of C-H bonds will take place at metal centres with well-defined environment which means metals in confined geometries (zeolites, molecular sieves), metal complexes in solution, and metal ions as part of active centres of enzymes, enzyme/protein complexes and of whole cells.
The investigations are focussed on three subtopics where the preparative methodology and mechanistic understanding are at present not very well developed and, therefore, new insights would be of great interest: Oxidation of various alkanes to alcohols and to ketones (A), oxidation of 1,3-dicarbonyl compounds to 2-hydroxy-1,3-dicarbonyl compounds, of diverse alkenes to allyl alcohols or oxidative coupling of phenol derivatives (B) and oxidation of aromatic compounds to phenols (C). Moreover, the selected different types of reactions play an important role in the synthesis of pharmaceutic products, natural materials with interesting biological properties, fine chemicals, and industrial products.
Suitable spectroscopic and theoretical methods will be used in order to obtain a detailed picture of catalysis on a molecular level and by this means make it possible to develop improved catalysts.
In the long run the aim of the project is to make ubiquitous oxygen into a universally usable and selective oxidising agent.
Molecular oxygen is involved in many of these processes, but the great potential of this abundant, non-toxic, and sustainable oxidising agent could not be realised up to now. Reasons for this shortcoming are the relative inertness of molecular oxygen towards C-H bonds and the poor selectivity in reactions involving organic substrates.
The aim of the Collaborative Research Centre is to turn molecular oxygen into a selective oxidising agent for organic substrates. The activation of molecular oxygen and the oxidation of C-H bonds will take place at metal centres with well-defined environment which means metals in confined geometries (zeolites, molecular sieves), metal complexes in solution, and metal ions as part of active centres of enzymes, enzyme/protein complexes and of whole cells.
The investigations are focussed on three subtopics where the preparative methodology and mechanistic understanding are at present not very well developed and, therefore, new insights would be of great interest: Oxidation of various alkanes to alcohols and to ketones (A), oxidation of 1,3-dicarbonyl compounds to 2-hydroxy-1,3-dicarbonyl compounds, of diverse alkenes to allyl alcohols or oxidative coupling of phenol derivatives (B) and oxidation of aromatic compounds to phenols (C). Moreover, the selected different types of reactions play an important role in the synthesis of pharmaceutic products, natural materials with interesting biological properties, fine chemicals, and industrial products.
Suitable spectroscopic and theoretical methods will be used in order to obtain a detailed picture of catalysis on a molecular level and by this means make it possible to develop improved catalysts.
In the long run the aim of the project is to make ubiquitous oxygen into a universally usable and selective oxidising agent.
DFG Programme
Collaborative Research Centres
Completed projects
- A01 - Selektivoxidation von n-Alkanen an edelmetallhaltigen Gästen in Zeolithen als Wirten (Project Heads Bertagnolli, Helmut ; Weitkamp, Jens )
- A02 - Neuartige oktaedrische Redoxmolekularsiebe für die heterogen katalysierte Selektivoxidation von Cyclohexan (Project Heads Gläser, Roger ; Hasse, Hans ; Schleid, Thomas )
- A03 - Untersuchung des aktiven Eisenzentrums bei katalytischen Oxidationen mittels in situ-Mößbauer-Spektroskopie und nuklear-inelastischer Streuung (Project Head Asthalter, Tanja )
- A04 - Biokatalytische Oxidation von cyclischen und acyclischen Alkanen durch bakterielle Cytochrom P450-Monooxygenasen (Project Heads Gläser, Roger ; Pleiss, Jürgen ; Urlacher, Vlada )
- A06 - Entwicklung aerober, artifizieller oder biomimetrischer, selektiver Reoxidationscyclen für die biologische und chemische Alkanoxidation (Project Head Plietker, Bernd )
- A07 - Darstellung hochoxidierter Ruthenium-Katalysatoren für die aerobe stereo- und chemoselektive Oxidation nicht-aktivierter Alkane (Project Head Plietker, Bernd )
- B01 - Luftsauerstoff als Oxidationsmittel für die Ce-katalysierte Hydroxylierung von 1,3-Dicarbonylverbindungen: mechanistische Untersuchungen und synthetische Anwendungen (Project Heads Bertagnolli, Helmut ; Christoffers, Jens ; Niemeyer, Mark )
- B02 - Enantioselektive aerobe katalytische Allyloxidation unter Verwendung von bakteriellen Monooxygenasen und Übergangsmetallkomplexen (Project Heads Laschat, Sabine ; Pleiss, Jürgen ; Traa, Yvonne ; Urlacher, Vlada )
- B03 - Metabolic Engineering rekombinanter Escherichia coli-Zellen zur Gewinnung von Antioxidantien: Astaxanthin und Vitamin E (Project Heads Reuss, Matthias ; Sprenger, Georg )
- B04 - Enzymkatalysierte oxidative Phenolkupplungen durch Laccasen und Kombinationen aus Laccase und dirigierenden Proteinen (Project Heads Beifuss, Uwe ; Pleiss, Jürgen ; Schaller, Andreas ; Schmid, Rolf )
- C01 - Wechselwirkung und Elementarprozesse der Benzoloxidation in Zeolithen - ein molekulares Bild (Project Head Roduner, Emil )
- C02 - Ab initio Methoden zur theoretischen Beschreibung von katalytischen Oxidationsreaktionen mit molekularem Sauerstoff (Project Head Werner, Hans-Joachim )
- C03 - Zwischenstufen der kupferinduzierten C-H-Aktivierung mittels O2 (Project Head Kaim, Wolfgang )
- C04 - Berechnung von Reaktionspfaden und Charakterisierung reaktiver Zwischenstufen in katalytischen Oxidationen (Project Heads Rauhut, Guntram ; Stoll, Hermann )
- C05 - Übergangsmetall-katalysierte oxidative Funktionalisierung von Aromaten und Alkanen (Project Head Hashmi, A. Stephen K. )
- Z - Zentrales Verwaltungsprojekt (Project Head Laschat, Sabine )
Applicant Institution
Universität Stuttgart
Participating University
Universität Hohenheim
Spokesperson
Professorin Dr. Sabine Laschat
