Reduction of ion-exchanged PdFe/NaY with H-2 at 773 K results in the f
ormation of Fe2+ ions and PdFe alloy clusters; no FeO is formed by red
ucing Fe/NaY. The extent of Pd-enhanced reduction of Fe2+ to FeO decre
ases with increasing proton concentration in the zeolite. Data obtaine
d by Mossbauer spectroscopy, ferromagnetic resonance, and FTIR of adso
rbed CO indicate prevalent formation of PdFe alloy clusters. Temperatu
re-programmed reduction (TPR) and desorption (TPD) show the extent of
Fe reduction and the reoxidation by zeolite protons of FeO in bimetal
particles. An average composition of Pd16Fe and Pd10Fe3 was found for
the reduced clusters in PdFe/NaHY and neutralized PdFe/NaY, respective
ly. No alpha-Pd hydride is formed with PdFe(x) under conditions where
this hydride is prevalent for unalloyed Pd clusters. The propensity to
form Pd hydride is restored by oxidative leaching of the Fe atoms fro
m the bimetallic clusters. A strong ferromagnetic resonance signal fro
m PdFe(x) particles isolated in different zeolite cages and containing
only one or two Fe atoms suggests that Pd atoms surrounding an Fe ato
m become polarized.