A Site-Isolated Rhodium-Diethylene Complex Supported on Highly Dealuminated Y Zeolite: Synthesis and Characterization
The reaction of Rh(C{sub 2}H{sub 4}){sub 2}(acac) with the partially dehydroxylated surface of dealuminated zeolite Y (calcined at 773 K) and treatments of the resultant surface species in various atmospheres (He, CO, H{sub 2}, and D{sub 2}) were investigated with infrared (IR), extended X-ray absorption fine structure (EXAFS), and {sup 13}C NMR spectroscopies. The IR spectra show that Rh(C{sub 2}H{sub 4}){sub 2}(acac) reacted readily with surface OH groups of the zeolite, leading to loss of acac ligands from the Rh(C{sub 2}H{sub 4}){sub 2}(acac) and formation of supported mononuclear rhodium complexes, confirmed by the lack of Rh-Rh contributions in the EXAFS spectra; each Rh atom was bonded on average to two oxygen atoms of the zeolite surface with a Rh-O distance of 2.19 Angstroms. IR, EXAFS, and {sup 13}C NMR spectra show that the ethylene ligands remained bonded to the Rh center in the supported complex. Treatment of the sample in CO led to the formation of site-isolated Rh(CO){sub 2} complexes bonded to the zeolite. The sharpness of the CO bands in the IR spectrum gives evidence of a nearly uniform supported Rh(CO){sub 2} complex and, by inference, the near uniformity of the mononuclear rhodium complex with ethylene ligands from which it was formed. The supported complex with ethylene ligands reacted with H{sub 2} to give ethane, and it also catalyzed ethylene hydrogenation at 294 K.
- Research Organization:
- Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source
- Sponsoring Organization:
- Doe - Office Of Science
- DOE Contract Number:
- DE-AC02-98CH10886
- OSTI ID:
- 913815
- Report Number(s):
- BNL-78383-2007-JA; JPCBFK; TRN: US200804%%84
- Journal Information:
- J. Phys. Chem. B, Vol. 109; ISSN 1089-5647
- Country of Publication:
- United States
- Language:
- English
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