Prof. Dr. Christian Limberg

Prof. Limberg erforscht die Struktur und Reaktivität von Metallkomplexen und Metalloxid-Systemen, insbesondere wie Metallzentren zusammenwirken, um kleine Moleküle (Stickstoff, Kohlendioxid, Sauerstoff, Wasserstoff) zu aktivieren und umzuwandeln. Seine aktuelle Arbeit konzentriert sich auf molekulare Modelle von Katalysator-Aktivzentren und auf die Kontrolle von Reaktionen durch räumliche Anordnung von Metallzentren — Erkenntnisse, die für die Entwicklung effizienterer Katalysatoren in der chemischen Industrie, der Energieumwandlung und der Wasserstoffwirtschaft unmittelbar nutzbar sind. Die Methoden umfassen Synthese, Spektroskopie und computergestützte Modellierung, um die genauen Mechanismen dieser Reaktionen aufzuklären.

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• Die Bismutmolybdat-vermittelte Propenoxidation - Modellierung reaktiver Intermediate und Synthese von Komplexen mit neuartigen Oxometall-Strukturelementen

  Quelle ↗

  Förderer: DFG Sachbeihilfe Zeitraum: 03/2003 - 12/2007 Projektleitung: Prof. Dr. Christian Limberg

• SFB 546 II-III: Synthese und Reaktivität von Molekülmodellen für die aktiven Stellen Vanadiumoxid-basierender Katalysatoren (Teilprojekt B 5)

  Quelle ↗

  Förderer: DFG Sonderforschungsbereich Zeitraum: 08/2003 - 06/2011 Projektleitung: Prof. Dr. Christian Limberg

• Homogene und heterogene Oxidationsreaktionen mit Molybdänoxo-Verbindungen - Modellierung von Intermediaten und Synthese von Komplexen mit neuartigen Oxometall-Strukturelementen

  Quelle ↗

  Förderer: DFG Sachbeihilfe Zeitraum: 02/2004 - 02/2005 Projektleitung: Prof. Dr. Christian Limberg

• The Mechanism of Water Oxidation: From Electrolysis via Homogeneous to Biological Catalysis

  2010

  ChemCatChem · DOI

  Abstract Striving for new solar fuels, the water oxidation reaction currently is considered to be a bottleneck, hampering progress in the development of applicable technologies for the conversion of light into storable fuels. This review compares and unifies viewpoints on water oxidation from various fields of catalysis research. The first part deals with the thermodynamic efficiency and mechanisms of electrochemical water splitting by metal oxides on electrode surfaces, explaining the recent concept of the potential‐determining step. Subsequently, novel cobalt oxide‐based catalysts for heterogeneous (electro)catalysis are discussed. These may share structural and functional properties with surface oxides, multinuclear molecular catalysts and the catalytic manganese–calcium complex of photosynthetic water oxidation. Recent developments in homogeneous water‐oxidation catalysis are outlined with a focus on the discovery of mononuclear ruthenium (and non‐ruthenium) complexes that efficiently mediate O 2 evolution from water. Water oxidation in photosynthesis is the subject of a concise presentation of structure and function of the natural paragon—the manganese–calcium complex in photosystem II—for which ideas concerning redox‐potential leveling, proton removal, and OO bond formation mechanisms are discussed. The last part highlights common themes and unifying concepts.

• Multifunctional “Clickates” as Versatile Extended Heteroaromatic Building Blocks: Efficient Synthesis via Click Chemistry, Conformational Preferences, and Metal Coordination

  2007

  Chemistry - A European Journal · DOI

  Click chemistry has been utilized to access 2,6-bis(1-aryl-1,2,3-triazol-4-yl)pyridines (BTPs) as versatile extended heteroaromatic building blocks for their exploitation in supramolecular chemistry, in particular foldamer and ligand design. In addition to their high-yielding synthesis using Cu(I)-catalyzed Huisgen-type 1,3-dipolar cycloaddition reactions the formed triazole moieties constitute an integral part of the BTP framework and encode both its pronounced conformational preferences as well as its chelating ability. A diverse set of symmetrical and non-symmetrical BTPs carrying electron-donating and -withdrawing substituents at both terminal aryl and the central pyridine moieties has efficiently been synthesized and could furthermore readily be postfunctionalized with amphiphilic side chains and porphyrin chromophores. In both solution and solid state, the BTP scaffold adopts a highly conserved horseshoe-like anti-anti conformation. Upon protonation or metal coordination, the BTP scaffold switches to the chelating syn-syn conformation. Iron and europium complexes have been prepared, successfully characterized by single-crystal X-ray diffraction analysis, and investigated with regard to their spin state and luminescent properties. The extended heteroaromatic BTP scaffold should prove useful for the design of responsive foldamer backbones and the preparation of new magnetic and emissive materials.