Paramagnetic Silver Species in Irradiated Ag-NaA Zeolites. An EPR and ESEEM Study

被引:14
作者
Michalik, J. [2 ]
van der Pol, A. [1 ]
Reijerse, E. L. [1 ]
Wasowicz, T. [2 ]
de Boer, E. [1 ]
机构
[1] Univ Nijmegen, Fac Sci, Dept Mol Spect, NL-6525 ED Nijmegen, Netherlands
[2] Inst Nucl Chem & Technol, Dept Radiat Chem & Technol, PL-03195 Warsaw, Poland
关键词
D O I
10.1007/BF03166778
中图分类号
O64 [物理化学(理论化学)、化学物理学]; O56 [分子物理学、原子物理学];
学科分类号
070203 ; 070304 ; 081704 ; 1406 ;
摘要
Several polymeric silver clusters have been observed in Ag(x)-NaA zeolite ( x = 1,6) of varying water content, which was exposed to x-rays at 77 K and annealed at higher temperatures, (109)Ag(1)-NaA zeolite dehydrated at 130 degrees C yields the dimer (109)Ag(2)(+) and the trimer (109)Ag(3)(2+) after irradiation at 77 K and annealing at 240 K. Owing to the use of one Ag isotope the EPR spectra of these species are highly resolved exhibiting g and hyperfine anisotropy. By irradiation of (109)Ag(x)-NaA zeolite (x = 1,6) in hydrated form two new trimeric silver clusters I and II are produced. The ratio between I and II depends on the initial Ag content. ESEEM spectra of these species show interaction with aluminum nuclei of the framework and with distant water molecules. If Ag(6)-NaA zeolite dehydrated at 130 degrees C is irradiated the hexameric cluster Ag(6)(n+) is formed. The ESEEM spectrum shows interaction only to aluminum nuclei. From ESEEM experiments on Ag(6)(n+) with added adsorbates (D(2)O, CD(3)OD) it could be inferred that Ag(6)(n+) is only stable if the neighbouring cages do not contain adsorbate molecules.
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页码:19 / 35
页数:17
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