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Catalytic and electron spin resonance studies of propylene oxidation on copper(II)-exchanged X zeolite: Temperature dependence of copper(II) migration

Journal Article · · Journal of Physical Chemistry; (USA)
DOI:https://doi.org/10.1021/j100382a056· OSTI ID:6469117
The copper(II)-catalyzed oxidation of propylene on CuK-X zeolite was studied under conditions of excess oxygen over the temperature range of 100 to 400{degree}C in a flow system to investigate the temperature dependence of the catalytic activity and the migration of copper(II) species and Cu(II) coordination complexes in the zeolite framework. It is shown that the percent of propylene conversion depends upon the reaction temperature and upon the extent of Cu(II) exchanged into the zeolite. Temperature causes the cupric ions to migrate near the six-ring window between the {alpha} and {beta} cages of the zeolite structure where they complex with propylene and induce the oxidation reaction. Arrhenius activation energies decrease with increasing copper(II) content. The decreasing activation energy with decreasing Cu(II) content is associated with different site occupancies of Cu(II) within the zeolite structure. Electron spin resonance studies show that cupric ions are initially distributed in SI hexagonal prism sites and SI{prime} sites in the {beta} cage adjacent to the hexagonal prisms in dehydrated CuK-X zeolite.
OSTI ID:
6469117
Journal Information:
Journal of Physical Chemistry; (USA), Journal Name: Journal of Physical Chemistry; (USA) Vol. 94:19; ISSN 0022-3654; ISSN JPCHA
Country of Publication:
United States
Language:
English