期刊
CHEMCATCHEM
卷 9, 期 24, 页码 4508-4519出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cctc.201701067
关键词
heterogeneous catalysis; platinum; structure-activity relationships; supported catalysts; tungsten
资金
- University of the Basque Country (UPV/EHU)
- European Union through the European Regional Development Fund (ERDF) (Spanish MICIN Project) [CTQ2015-64226-C3-2R]
- Basque Government (Researcher Training Program of the Department of Education, Universities and Research)
Three aluminium oxide materials and a HZSM-5 zeolite were used as supports of bimetallic Pt-WOx catalysts to establish structure-activity relationships in the glycerol hydrogenolysis reaction. The surface W density and the intimate contact between Pt and WOx were key parameters. Surface W density controls the formation of polytungstates, the only species able to produce the weak Bronsted acidity that is required to produce 1,3-propanediol selectively. The comparison between the HZSM-5 and the Al2O3 supports demonstrated that an increment of the medium Bronsted acidity is detrimental for the selective 1,3-propanediol formation as it promotes reactions that yield 1-propanol and propane. An increase of the dispersion of Pt on the Pt/WOx/Al2O3 catalysts led to higher glycerol conversions but also promoted the hydrogenolysis routes that lead to 1,2-and 1,3-propanediol similarly. On the contrary, an increase of the Pt metal content favoured the hydrogenolysis route that leads to 1,3-propanediol significantly. A more intimate contact between Pt and WOx promoted the hydrogenation of the intermediate carbocation, formed and stabilised on a polytungstate active site, into 1,3-propanediol.
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