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• W3042178434 endingPage "8949" @default.
• W3042178434 startingPage "8933" @default.
• W3042178434 abstract "Environmentally friendly and low-cost catalysts are required forlarge-scale nonoxidative dehydrogenation of propane to propene (PDH)to replace currently used CrOx- or Pt-basedcatalysts. This work introduces ZnO-containing ZrO2- orMZrOx-supported (M = Ce, La, Ti or Y)catalysts. The most active materials outperformed the state-of-the-artcatalysts with supported CrOx, GaOx, ZnOx, or VOx species as well as bulk ZrO2-basedcatalysts without ZnO. The space–time yield of propene of 1.25kgC3H6·kg–1cat·h–1 at a propane conversion of about 30% with a propeneselectivity of 95% was obtained over Zn­(4 wt %)/TiZrOx at 550 °C. For deriving key insights into thestructure of active sites, reactivity, selectivity, and on-streamstability, the catalysts were characterized by XRD, HRTEM, EDX mapping,XPS, X-ray absorption, CO-TPR, CO2-TPD, NH3-TPD,pyridine-FTIR, operando UV–vis spectroscopy, Raman spectroscopy,TPO, and temporal analysis of products. In contrast with previousreports that used bulk ZrO2-based catalysts without ZnO,coordinatively unsaturated Zr cations are not the main active sitesin the ZnO-containing catalysts. Supported ZnOx species were concluded to participate in the PDH reaction.The current X-ray absorption analysis proved that their structureis affected by the type of metal oxide used as a dopant for ZrO2 and by the crystallinity of ZrO2. Isolated tricoordinatedZn2+ species were concluded to show high activity and on-streamstability. Their intrinsic activity is enhanced when TiO2 and ZrO2 coexist in the support or when ZrO2 is promoted by TiO2. This is probably due to acceleratinghydrogen formation in the course of the PDH reaction as concludedfrom temporal analysis of products with sub-millisecond resolution.The results of temperature-programmed oxidation of spent catalystsas well as ex situ Raman and operando UV–vis studies enabledus to conclude that the high on-stream stability of isolated tricoordinatedZn2+ species in the PDH reaction is related to their lowability to form coke. In general, the tendency for coke formationseems to increase with an increase in the degree of ZnOx agglomeration." @default.
• W3042178434 created "2020-07-16" @default.
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• W3042178434 date "2020-07-10" @default.
• W3042178434 modified "2023-10-16" @default.
• W3042178434 title "Elucidating the Nature of Active Sites and Fundamentals for their Creation in Zn-Containing ZrO₂–Based Catalysts for Nonoxidative Propane Dehydrogenation" @default.
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• W3042178434 doi "https://doi.org/10.1021/acscatal.0c01580" @default.
• W3042178434 hasPublicationYear "2020" @default.
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