A Site-Isolated Iridium Diethylene Complex Supported on Highly Dealuminated Y Zeolite: Synthesis And Characterization
Highly dealuminated Y zeolite-supported mononuclear iridium complexes with reactive ethylene ligands were synthesized by chemisorption of Ir(C{sub 2}H{sub 4}){sub 2}(C{sub 5}H{sub 7}O{sub 2}). The resultant structure and its treatment in He, CO, ethylene, and H2 were investigated with infrared (IR) and extended X-ray absorption fine structure (EXAFS) spectroscopies. The IR spectra show that Ir(C{sub 2}H{sub 4}){sub 2}(C{sub 5}H{sub 7}O{sub 2}) reacted readily with surface OH groups of the zeolite, leading to the removal of C{sub 5}H{sub 7}O{sub 2} ligands and the formation of supported mononuclear iridium complexes, confirmed by the lack of Ir-Ir contributions in the EXAFS spectra. The EXAFS data show that each Ir atom was bonded to four carbon atoms at an average distance of 2.10 {angstrom}, consistent with the presence of two ethylene ligands per Ir atom and in agreement with the IR spectra indicating {pi}-bonded ethylene ligands. The EXAFS data also indicate that each Ir atom was bonded to two oxygen atoms of the zeolite at a distance of 2.15 {angstrom}. The supported iridium-ethylene complex reacted with H{sub 2} to give ethane, and it also catalyzed ethylene hydrogenation at atmospheric pressure and 294 K. Treatment of the sample in CO led to the formation of Ir(CO){sub 2} complexes bonded to the zeolite. The sharpness of the V{sub CO} bands indicates a high degree of uniformity of these complexes on the support. The iridium-ethylene complex on the crystalline zeolite support is inferred to be one of the most nearly uniform supported metal complex catalysts. The results indicate that it is isostructural with a previously reported rhodium complex on the same zeolite; thus, the results are a start to a family of analogous, structurally well-defined supported metal complex catalysts.
- Research Organization:
- SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Sponsoring Organization:
- USDOE
- DOE Contract Number:
- AC02-76SF00515
- OSTI ID:
- 953900
- Report Number(s):
- SLAC-REPRINT-2009-492; TRN: US201004%%637
- Journal Information:
- J. Phys. Chem. C111:15064,2007, Vol. 111, Issue 41; ISSN 1932-7447
- Country of Publication:
- United States
- Language:
- English
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