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Single-Site Zeolite-Anchored Organoiridium Carbonyl Complexes: Characterization of Structure and Reactivity by Spectroscopy a...

by Claudia Martinez-macias, Mingyang Chen, David Dixon, Bruce Gates
Publication Type
Journal
Journal Name
Chemistry—A European Journal
Publication Date
Page Numbers
11825 to 11835
Volume
21
Issue
33

A family of HY zeolite-supported cationic organoiridium carbonyl complexes was formed by reaction of Ir(CO)(2)(acac) (acac=acetylacetonate) to form supported Ir(CO)(2) complexes, which were treated at 298K and 1atm with flowing gas-phase reactants, including C2H4, H-2, (CO)-C-12, (CO)-C-13, and D2O. Mass spectrometry was used to identify effluent gases, and infrared and X-ray absorption spectroscopies were used to characterize the supported species, with the results bolstered by DFT calculations. Because the support is crystalline and presents a nearly uniform array of bonding sites for the iridium species, these were characterized by a high degree of uniformity, which allowed a precise determination of the species involved in the replacement, for example, of one CO ligand of each Ir(CO)(2) complex with ethylene. The supported species include the following: Ir(CO)(2), Ir(CO)(C2H4)(2), Ir(CO)(C2H4), Ir(CO)(C2H5), and (tentatively) Ir(CO)(H). The data determine a reaction network involving all of these species.