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Geochemical Journal
Geochemical Journal An open access journal for geochemistry
Published for geochemistry community from Geochemical Society of Japan.

Studies on allophane and imogolite by high-resolution solid-state 29Si- and 27Al-NMR and ESR

Hiroshi Shimizu, Tokuko Watanabe, Teruo Henmi, Akimasa Masuda, Hajime Saito
Geochemical Journal, Vol. 22, No. 1, P. 23-31, 1988


The high-resolution 29Si- and 27Al-NMR spectra and ESR spectra for five allophanes (SiO2/Al2O3=1.19, 1.22, 1.75, 1.77 and 1.90) are reported, together with the spectra for two imogolites (SiO2/Al2O3 = 0.96 and 1.0) and a halloysite (SiO2/Al2O3 = 2.0). It is apparently seen that 29Si-NMR spectra for allophanes vary depending on SiO2/Al2O3 ratios, indicating structural variations of allophanes with the change of the SiO2/Al2O3 ratios. Allophanes with SiO2/Al2O3 molar ratios close to 1.0 show a broad absorption at -79 ppm with a second, minor resonance around 90 ppm in the 29Si-NMR spectra; this suggests that orthosilicate is a main component of allophanes with lower SiO2/Al2O3 ratios. On the other hand, allophanes with higher SiO2/Al2O3 ratios show complicated 29Si-NMR spectra with several peaks between -79 and -97 ppm; these spectra indicate that these allophanes contain Si atoms in the orthosilicate structure as well as several different states of polymerized silicates with various Si-O-Si angles and Si-O bond strengths. Further, it is indicated that the relative abundances of polymerized silicates to orthosilicate tend to increase with the increase of the SiO2/Al2O3 ratio of allophane samples up to 1.75 and decrease at higher ratios. 27Al-NMR spectra for four allophanes studied show the resonance mainly at the chemical shift of 2.9-4.1 ppm, indicative of six-coordinated Al.

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