The V(IV) Species, Location and Adsorbate Interactions in VH-SAPO-11 studied by ESR and ESEM
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Abstract
Vanadium-incorporated aluminophophate molecular sieve VH-SAPO-11 has been studied by electron spin resonance (ESR) and electron spin echo modulation (ESEM) spectroscopies to determine the vanadium location and interaction with various adsorbate molecules. As-synthsized VH-SAPO-11 contains only vanadyl species with distorted octahedral coordination. After calcinations in O2 and exposure to moisture, only species A is observed with reduced intensities. Species A is suggested as a VO(H2O)22+ complex coordinate to three framework oxygen bonded to aluminum. When calcined, hydrate VH-SAPO-11 is dehydrated at elevated temperature, species A loses its water ligands and transforms to VO2+ ions coordinated to three framework oxygens (species B). Species B reduces its intensities significantly after treatment with O2 at high temperature, thus suggesting oxidation of v4+ to v5+. When dehydrated VH-SAPO-11 contacts with D2O at room temperature, the ESR signal of species A is observed. This species assumed as a VO(Of)3(D2O)2, by considering 3 framework oxygens. Adsorption of deuterated methanol on dehydrated VH-SAPO-11 results in another new vanadium species D, which is identified as a VO(CD3OH) complex. When deuterated ethanol is adsorbed on dehydrated VH-SAPO-11, another new vanadium species E identified as a VO(C2H5OD)2+, is observed. When deuterated propanol is adsorbed on dehydrated VH-SAPO-11, a new vanadium species F identified as a VO(C3H7OD), is observed. Possible coordination geometries of these various complexes are discussed.
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