ZrO2‐Based Alternatives to Conventional Propane Dehydrogenation Catalysts: Active Sites, Design, and Performance. Issue 52 (13th November 2015)

• Record Type: Journal Article
• Authors: Otroshchenko, Tatyana; Sokolov, Sergey; Stoyanova, Mariana; Kondratenko, Vita A.; Rodemerck, Uwe; Linke, David; Kondratenko, Evgenii V.
• Is Part Of: Angewandte Chemie international edition. Volume 54:Issue 52(2015)
• Page Start: 15880
• Page End: 15883
• Publication Date: 2015-11-13
• Subjects: active sites -- heterogeneous catalysis -- propane dehydrogenation -- propene -- zirconia; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.201508731
• Languages: English
• ISSNs: 1433-7851

Abstract

Abstract: Non‐oxidative dehydrogenation of propane to propene is an established large‐scale process that, however, faces challenges, particularly in catalyst development; these are the toxicity of chromium compounds, high cost of platinum, and catalyst durability. Herein, we describe the design of unconventional catalysts based on bulk materials with a certain defect structure, for example, ZrO2 promoted with other metal oxides. Comprehensive characterization supports the hypothesis that coordinatively unsaturated Zr cations are the active sites for propane dehydrogenation. Their concentration can be adjusted by varying the kind of ZrO2 promoter and/or supporting tiny amounts of hydrogenation‐active metal. Accordingly designed Cu(0.05 wt %)/ZrO2 ‐La2 O3 showed industrially relevant activity and durability over ca. 240 h on stream in a series of 60 dehydrogenation and oxidative regeneration cycles between 550 and 625 °C. Abstract : The support is the catalyst : In a new approach to propane dehydrogenation catalysts, surface, coordinatively unsaturated, Zr cations in bulk ZrO2 ‐based catalysts are the catalytically active sites. Their concentration can be tuned through doping ZrO2 with metal oxides inducing the formation of such structural defects or by depositing tiny amounts (up to 0.05 wt %) of hydrogenation‐active metals that promote ZrO2 reduction.