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Chemical interactions in multimetal/zeolite catalysts

Technical Report ·
DOI:https://doi.org/10.2172/5837780· OSTI ID:5837780

For Pt/NaY catalysts our analysis of the mechanism of metal particle formation has enabled us to produce at will samples which contain either the majority of the Pt particles in supercages, without filling these cages completely, or the Pt particles bulge into neighboring cages. The catalytic selectivity is distinctly different for these preparations, in the former case molecules can enter a supercage which is partially filled by the Pt cluster, in the second case adsorption takes place through the cage window. Applying the same principles of catalyst preparation of bimetallic catalysts enables us to produce PtCu particles in supercages of NaY, which contain, initially a Pt core, surrounded by a Cu mantle. Earlier we have found that Ni ions migrate into hexagonal prisms during calcination of Ni/NaY; this process can be partially suppressed by first filling these prisms with Mn or Cr ions. In more recent work we found that addition of Pt strongly lowers the temperature of Ni reduction. Part of the Ni ions is reduced by hydrogen while still inside the smaller cages. This reduction process is, however, reversible; at elevated temperature and in an inert atmosphere protons re-oxidize the Ni atoms and dihydrogen gas is developed. In this way it seems possible to count the Ni atoms in small cages. The calcination stage in the preparation of zeolite supported metals has been studied in considerable detail for Pd/NaY. The Pd is introduced as a tetrammin complex; during calcination the ammine ligands are successively oxidized. Once three ammine ligands are destroyed, the Pd ions which carry only one ligand, surprisingly jump from the supercages to the sodalite cage.

Research Organization:
Northwestern Univ., Evanston, IL (United States)
Sponsoring Organization:
DOE; USDOE, Washington, DC (United States)
DOE Contract Number:
FG02-87ER13654
OSTI ID:
5837780
Report Number(s):
DOE/ER/13654-1; ON: DE92008103
Country of Publication:
United States
Language:
English