期刊
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 3, 期 7, 页码 1383-1390出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/b009942m
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The copper-ion-exchanged ZSM-5 type zeolite, prepared by ion-exchange in an aqueous solution of Cu(CH3COO)(2) and evacuation at 873 K, gives a distinctive IR band at 2151 cm(-1) due to the adsorbed CO species. More efficient adsorption of N-2 was exhibited by this sample, compared with samples prepared by other methods, implying site-selective ion-exchange in the preparation process. On the basis of X-ray absorption near-edge structure (XANES) spectra the exchanged copper ion was proved to be in a monovalent state; one of the splitting strong bands, due to the 1s-4p(z) transition of the monovalent copper ion, loses its intensity on N-2 adsorption. The extended X-ray absorption fine structure (EXAFS) spectral pattern around the copper ion also changed on N-2 adsorption and a shoulder appeared at around 1.5 Angstrom (no phase-shift correction), in addition to the strong band at around 1.65 Angstrom (no phase-shift correction). It was concluded that the monovalent copper-ion-exchanged site giving the 2151 cm(-1) band due to the adsorbed CO species is the active site for specific N-2 adsorption. A first principles calculation was carried out with the object of finding the most appropriate model for the CO species adsorbed on the exchanged copper ions in ZSM-5. The data obtained suggest that a three-coordinate copper ion bonded to three lattice oxygen atoms adsorbs CO to give the 2151 cm(-1) band. A pseudo-planar structure including the monovalent copper ion bound to three oxygen atoms is assumed to change to a pseudo-tetrahedral arrangement on N-2 adsorption. Such a site-selectively ion-exchanged substance has potential for the development of materials for N-2 separation or fixation and activation catalysts, as well as for the analysis of NO-decomposition sites.
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