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The formation and stabilization of reduced silver species in the regularly interstratified clay minerals, trioctahedral smectite/chlorite (tri-Sm/Ch) and dioctahedral smectite/mica (di-Sm/M), have been studied by electron paramagnetic resonance (EPR) spectroscopy. Both minerals loaded with Ag+ cations after degassing and dehydration were g-irradiated at 77 K and monitored by EPR as the temperature increased. Some samples were exposed to water or methanol vapor after dehydration. In both hydrated and dehydrated samples only the doublets assigned to Ag0 atoms were observed with no evidence of the formation of Ag clusters. However, the EPR parameters of silver atoms in both matrices are different. In tri-Sm/Ch the narrow anisotropic EPR lines overlap with the broader isotropic lines, whereas in di-Sm/M only broad lines are recorded. The hyperfine splitting - Aiso(Ag0) is larger in tri-Sm/Ch than in di-Sm/M. Also the stability of Ag0 in both clay minerals is distinctly different. Ag0 doublet in di-Sm/M disappears completely above 230 K, whereas in tri-Sm/Ch it is still recorded at 310 K. It is proposed, basing on the EPR results that Ag0 atoms appear at different sites in both matrices: - in tri-Sm/Ch in the middle of smectite interlayer and in hexagonal cavities in the silicate sheets of tetrahedron layer and in di-Sm/M in hexagonal cavities only. When samples had been exposed to methanol before irradiation, the silver clusters become stabilized in the interlayer sites. In tri- Sm/Ch matrix the silver dimer Ag2+ formed by g-irradiation at 77 K is transformed to tetrameric cluster, Ag43+ at 150 K. In di-Sm/M the radiation-induced silver agglomeration proceeds in a similar way, but with a slower rate and Ag tetramer is formed only above 190 K. In both clay minerals, Ag43+ clusters decay above 250 K.
Czasopismo
Rocznik
Tom
Strony
131--136
Opis fizyczny
Bibliogr. 23 poz., rys.
Twórcy
autor
- Ecomaterials Center, National Institute for Materials Science, Namiki 1-1 Tsukuba, Ibaraki 305-0044, Japan, Tel.: +81-29-860-4667, Fax: +81-29-860-4667
autor
- Institute of Nuclear Chemistry and Technology, 16 Dorodna Str., 03-195 Warsaw, Poland
autor
- Ecomaterials Center, National Institute for Materials Science, Namiki 1-1 Tsukuba, Ibaraki 305-0044, Japan, Tel.: +81-29-860-4667, Fax: +81-29-860-4667
autor
- Ecomaterials Center, National Institute for Materials Science, Namiki 1-1 Tsukuba, Ibaraki 305-0044, Japan, Tel.: +81-29-860-4667, Fax: +81-29-860-4667
autor
- Institute of Nuclear Chemistry and Technology, 16 Dorodna Str., 03-195 Warsaw, Poland
autor
- Institute of Nuclear Chemistry and Technology, 16 Dorodna Str., 03-195 Warsaw, Poland
Bibliografia
- 1. Brindley GW (1980) Order-disorder in clay mineral structure. In: Brindley GW, Brown G (eds) Crystal structures of clay minerals and their X-ray identification. Mineralogical Society, London, pp 126−195
- 2. Brown DR, Findlay TJV, Symons MCR (1976) Radiation mechanisms. Part 12. ESR studies of electron capture by silver(I) ions, nitrate ions and their ion pairs and clusters in methyl cyanide. J Chem Soc, Faraday Trans 72:1792−1798
- 3. Brown DR, Luca V, Kevan L (1991) Electron paramagnetic resonance and electron spin echo modulation analysis of silver atom environment in γ-irradiated silver-exchanged sodium montmorillonite and its Al13 pillared derivative. J Chem Soc, Faraday Trans 87:2749−2754
- 4. Brown R, Kevan L (1986) Comparative electron spin resonance and optical absorption studies of silver-exchanged sodium Y zeolites: Silver centers formed on dehydration, oxidation, and subsequent γ-irradiation. J Phys Chem 90:1129−1133
- 5. Greene-Kelly R (1953) The identification of montmorillonoids in clays. J Soil Sci 4:233−237
- 6. Kevan L (1992) Applications of electron spin echo modulation to transition metal ions in smectite clays. Pure Appl Chem 64:781−788
- 7. Kevan L, Schlick S (1976) Spin trapping of radicals formed in gamma-irradiated methanol: effect of the irradiation temperature from 77 K to 300 K. Chem Phys Lett 38:505−509
- 8. Lim CH, Jackson ML (1986) Expandable phyllosilicate reactions with lithium on heating. Clays Clay Miner 34:346−352
- 9. Luca V, Brown DR, Kevan L (1991) Electron spin resonance and electron spin-echo modulation studies of silver ion solvation in silver-exchanged synthetic fluorohectolite and synthetic beidellite. J Phys Chem 95:10065−10070
- 10. Michalik J (1996) Silver atoms and clusters in molecular sieves and clays. Appl Magn Reson 10:507−537
- 11. Michalik J, Azuma N, Sadlo J, Kevan L (1995) Silver agglomeration in SAPO-5 and SAPO-11 molecular sieves. J Phys Chem 99:4679−4686
- 12. Michalik J, Kevan L (1986) Paramagnetic silver clusters in Ag-NaA zeolite: electron spin resonance and diffuse reflectance spectroscopic studies. J Am Chem Soc 108:4247−4253
- 13. Michalik J, Sadlo J, Kodaira T, Shimomura S, Yamada H (1998) ESR and optical studies of cationic silver clusters in zeolite rho. J Radioanal Nucl Chem 232:135−137
- 14. Michalik J, Sadlo J, Yu JS, Kevan L (1996) Tetrameric silver clusters in rho zeolite stable above room temperature – ESR studies. Colloids Surf A 115:239−247
- 15. Michalik J, Yamada H, Brown DR, Kevan L (1996) Small silver clusters in smectite clay interlayers. J Phys Chem 100:4213−4218
- 16. Michalik J, Yamada H, Wasowicz T, Kevan L (1995) Pulsed electron spin resonance studies of silver atoms and clusters in smectite clays. In: IS&T’s Annual. Conf, Final Program Adv Print Pap, 48th:309−311
- 17. Newman ACD, Brown G (1987) Interstratified clay minerals. In: Newman ACD (ed) Chemistry of clays and clay minerals. Wiley, New York, pp 92−107
- 18. Reynolds RC (1980) Interstratified clay minerals. In: Brindley GW, Brown G (eds) Crystal structures of clay minerals and their X-ray identification. Mineralogical Society, London, pp 249−303
- 19. Reynolds RC, Hower J (1970) The nature of interlayering in mixed-layer illite-montmorillonite. Clays Clay Miner 18:25−36
- 20. Sadlo J, Wasowicz T, Michalik J (1995) Radiation-induced silver agglomeration in molecular sieves: a comparison between A and X zeolites. Radiat Phys Chem 45:909−915
- 21. Wasowicz T, Mikosz J, Sadlo J, Michalik J (1992) Organosilver radicals in gamma-irradiated Ag-NaA zeolites with methanol adsorbate. J Chem Soc, Perkin Trans 2:1487−1491
- 22. Yamada H, Fujita T, Nakazawa H (1988) Design and calibration of a rapid quench hydrothermal apparatus. J Ceram Soc pn 96:1041−1044
- 23. Yamada H, Nakazawa H, Yoshioka K, Fujita T (1991) Smectites in the montmorillonite-beidellite series. Clay Minerals 26:359−369
Typ dokumentu
Bibliografia
Identyfikator YADDA
bwmeta1.element.baztech-article-BUJ6-0005-0070