Article

Catalysis Letters

, Volume 135, Issue 3, pp 282-290

Vanadium Oxide Based Nanostructured Materials for Catalytic Oxidative Dehydrogenation of Propane: Effect of Heterometallic Centers on the Catalyst Performance

  • M. Ishaque KhanAffiliated withDepartment of Biological, Chemical and Physical Sciences, Illinois Institute of Technology Email author 
  • , Sangita DebAffiliated withDepartment of Biological, Chemical and Physical Sciences, Illinois Institute of Technology
  • , Kadir AydemirAffiliated withDepartment of Biological, Chemical and Physical Sciences, Illinois Institute of Technology
  • , Abdulrahman A. AlwarthanAffiliated withChemistry Department, Science College, King Saud University
  • , Soma ChattopadhyayAffiliated withDepartment of Biological, Chemical and Physical Sciences, Illinois Institute of Technology
  • , Jeffrey T. MillerAffiliated withChemical Sciences and Engineering Division, Argonne National Laboratory
  • , Christopher L. MarshallAffiliated withChemical Sciences and Engineering Division, Argonne National Laboratory

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Abstract

Catalytic properties of a series of new class of catalysts materials—[Co3(H2O)12V18O42 (XO4)].24H2O (VNM-Co), [Fe3(H2O)12V18O42(XO4)].24H2O (VNM-Fe) (X = V, S) and [H6Mn3(H2O)12V18O42(VO4)].30H2O for the oxidative dehydrogenation of propane is studied. The open-framework nanostructures in these novel materials consist of three-dimensional arrays of {V18O42(XO4)} (X = V, S) clusters interconnected by {–O–M–O–} (M = Mn, Fe, Co) linkers. The effect of change in the heterometallic center M (M = Mn, Co, Fe) of the linkers on the catalyst performance was studied. The catalyst material with Co in the linker showed the best performance in terms of propane conversion and selectivity at 350 °C. The material containing Fe was most active but least selective and Mn containing catalyst was least active. The catalysts were characterized by Temperature Programmed Reduction (TPR), BET surface area measurement, Diffuse Reflectance Infrared Fourier Transform Spectroscopy, and X-ray Absorption Spectroscopy. TPR results show that all three catalysts are easily reducible and therefore are active at relatively low temperature. In situ X-ray absorption near edge spectroscopy (XANES) and extended X-ray absorption fine structure spectroscopy (EXAFS) studies revealed that the oxidation state of Co(II) remained unchanged up to 425 °C (even after pretreatment). The reduction of Co(II) into metallic form starts at 425 °C and this process is completed at 600 °C.

Graphical Abstract

Catalytic property studies of a series of nanostructured materials—[Co3(H2O)12V18O42 (XO4)].24H2O (VNM-Co), [Fe3(H2O)12V18O42(XO4)].24H2O (VNM-Fe) (X = V, S) and [H6Mn3(H2O)12V18O42(VO4)].30H2O for the oxidative dehydrogenation of propane shows the considerable effect of heterometallic centers on the catalyst performance; the catalyst containing cobalt showed the best performance in terms of propane conversion and selectivity at 350°C.
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Keywords

Vanadium oxides Oxidative dehydrogenation Heterogeneous catalysis Propylene X-ray absorption spectroscopy EXAFS