A more efficient copper-ion-exchanged ZSM-5 zeolite for N2 adsorption at room temperature: Ion-exchange in an aqueous solution of Cu(CH3COO)2

Yasushige Kuroda, R. Kumashiro, A. Itadani, M. Nagao, H. Kobayashi

Research output: Contribution to journalArticle

44 Citations (Scopus)

Abstract

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 N2 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-4pz transition of the monovalent copper ion, loses its intensity on N2 adsorption. The extended X-ray absorption fine structure (EXAFS) spectral pattern around the copper ion also changed on N2 adsorption and a shoulder appeared at around 1.5 Å (no phase-shift correction), in addition to the strong band at around 1.65 Å (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 N2 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 N2 adsorption. Such a site-selectively ion-exchanged substance has potential for the development of materials for N2 separation or fixation and activation catalysts, as well as for the analysis of NO-decomposition sites.

Original languageEnglish
Pages (from-to)1383-1390
Number of pages8
JournalPhysical Chemistry Chemical Physics
Volume3
Issue number7
DOIs
Publication statusPublished - Apr 1 2001

Fingerprint

Copper
Ion exchange
Ions
aqueous solutions
Adsorption
copper
adsorption
room temperature
Carbon Monoxide
ions
Temperature
X ray absorption
Phase shift
oxygen atoms
Oxygen
ZSM-5 zeolite
phase shift
Atoms
planar structures
shoulders

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Atomic and Molecular Physics, and Optics

Cite this

A more efficient copper-ion-exchanged ZSM-5 zeolite for N2 adsorption at room temperature : Ion-exchange in an aqueous solution of Cu(CH3COO)2. / Kuroda, Yasushige; Kumashiro, R.; Itadani, A.; Nagao, M.; Kobayashi, H.

In: Physical Chemistry Chemical Physics, Vol. 3, No. 7, 01.04.2001, p. 1383-1390.

Research output: Contribution to journalArticle

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abstract = "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 N2 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-4pz transition of the monovalent copper ion, loses its intensity on N2 adsorption. The extended X-ray absorption fine structure (EXAFS) spectral pattern around the copper ion also changed on N2 adsorption and a shoulder appeared at around 1.5 {\AA} (no phase-shift correction), in addition to the strong band at around 1.65 {\AA} (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 N2 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 N2 adsorption. Such a site-selectively ion-exchanged substance has potential for the development of materials for N2 separation or fixation and activation catalysts, as well as for the analysis of NO-decomposition sites.",
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