Development of Molecular and Solid Catalysts for the Direct Low-Temperature Oxidation of Methane to Methanol

The direct low‐temperature oxidation of methane to methanol is demonstrated on a highly active homogeneous molecular catalyst system and on heterogeneous molecular catalysts based on polymeric materials possessing ligand motifs within the material structure. The N‐(2‐methylpropyl)‐4,5‐diazacarbazoly...

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Bibliographic Details
Published in:ChemSusChem 2010-02, Vol.3 (2), p.277-282
Main Authors: Palkovits, Regina, von Malotki, Christian, Baumgarten, Martin, Müllen, Klaus, Baltes, Christian, Antonietti, Markus, Kuhn, Pierre, Weber, Jens, Thomas, Arne, Schüth, Ferdi
Format: Article
Language:English
Subjects:
Catalysis
heterogeneous catalysis
homogeneous catalysis
Methane - chemistry
Methanol - chemistry
oxidation
Oxidation-Reduction
platinum
polymers
Polymers - chemistry
Structure-Activity Relationship
Temperature
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Summary:The direct low‐temperature oxidation of methane to methanol is demonstrated on a highly active homogeneous molecular catalyst system and on heterogeneous molecular catalysts based on polymeric materials possessing ligand motifs within the material structure. The N‐(2‐methylpropyl)‐4,5‐diazacarbazolyl‐dichloro‐platinum(II) complex reaches significantly higher activity compared to the well‐known Periana system and allows first conclusions on electronic and structural requirements for high catalytic activity in this reaction. Interestingly, comparable activities could be achieved utilizing a platinum modified poly(benzimidazole) material, which demonstrates for the first time a solid catalyst with superior activity compared to the Periana system. Although the material shows platinum leaching, improved activity and altered electronic properties, compared to the conventional Periana system, support the proposed conclusions on structure–activity relationships. In comparison, platinum modified triazine‐based catalysts show lower catalytic activity, but rather stable platinum coordination even after several catalytic cycles. Based on these systems, further development of improved solid catalysts for the direct low‐temperature oxidation of methane to methanol is feasible. The direct low‐temperature oxidation of methane to methanol is demonstrated on both a highly active homogeneous molecular catalyst and on heterogeneous molecular catalysts based on polymeric materials. Superior activities are achieved and some heterogeneous systems maintain stability and activity for several catalytic cycles.
ISSN:1864-5631
1864-564X
DOI:10.1002/cssc.200900123