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Reduction and cluster growth of palladium in zeolite Y containing transition metal ions. X-ray absorption studies

Journal Article · · Journal of Physical Chemistry; (USA)
DOI:https://doi.org/10.1021/j100365a062· OSTI ID:6656590
;  [1]
  1. Univ. of New Mexico, Albuquerque (USA)

The effect of a second transition metal on the reducibility and agglomeration behavior of palladium in zeolite Y is studied by EXAFS spectroscopy. Special attention is given to the potential bonding interactions between both metal constituents that could result in chemical anchoring of the noble metal to the support via the unreduced cocation. Zeolite Y was coexchanged with Fe{sup 2+} or Co{sup 3+} and Pd{sup 2+} and with each ion alone. Dehydration in oxygen atmosphere and reduction with hydrogen was performed at different temperatures up to 623 K. The structure of the samples during various stages of pretreatment and reduction was studied with EXAFS on both absorption edges. Palladium is partially reduced to Pd{sup 0} at room temperature and forms small metal clusters at higher temperatures. Iron is oxydized under oxygen atmosphere and is partially present in the form of iron oxide particles, which are redispersed under reducing conditions. A small enhancement of the reducibility of palladium is observed if iron is present in the zeolite, but neither a chemical anchoring nor an effect on the final agglomeration process of palladium is detected by the presence of iron cations. In contrast, coexchange with cobalt results in a substantially higher dispersion of the Pd(0) phase after high-temperature reduction. Apparently, the change in cation distribution induced by the Co ions influences the reduction process of palladium. When palladium ions are diffused into the zeolite containing aqueous Fe(II) ions, a Pd(0) phase consisting of larger crystallites is formed at room temperature by a redox reaction with Fe(II).

DOE Contract Number:
AS05-80ER10742
OSTI ID:
6656590
Journal Information:
Journal of Physical Chemistry; (USA), Journal Name: Journal of Physical Chemistry; (USA) Vol. 94:2; ISSN 0022-3654; ISSN JPCHA
Country of Publication:
United States
Language:
English