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Celadonite in the Tuff of Oya, Tochigi Prefecture, Japan

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Celadonite in the Tuff of Oya, Tochigi Prefecture, Japan MINERALOGICAL JOURNAL, VOL. 6, No. 5, pp. 299-312, SEPT ., 1971 CELADONITE IN THE TUFF OF OYA, TOCHIGI PREFECTURE, JAPAN NORIHIKO KOHYAMA, SUSUMU SHIMODA and TOSHIO SUDO Geological and Mineralogical Institute, Faculty of Science, Tokyo University of Education, Otsuka, Tokyo, Japan ABSTRACT Celadonite occurs as an alteration product of glass fragments in rhyolitic tuff at Oya, Tochigi Prefecture. The chemical composition: SiO2, 55.99%; TiO2, 0.49%; A12O3,11.13%; Fe2O3, 4.65%; FeO, 7.34%; MnO, 0.20%; MgO, 2.27%; CaO, 0.22%; Na2O, 1.30%; K20, 8.00%; H2O+, 4.22%; H2O-, 3.68%; total, 99.50%. The structural formula: (K0.73Na0.18Ca0.02)(Mg0.30Mn0.01Fe2+0.44Fe3+0.25Al0.93) (Si3.99A10.01) (OH)2. O10 Although the amounts of A12O3and FeO are slightly larger than in earlier data, the Oya specimen is identified to be celadonite from its mode of oc currence, X-ray powder pattern, i. r. absorption spectrum and DTA curve. Introduction Many kinds of clay minerals have been found in rhyolitic tuff distributed at Oya, Tochigi Prefecture. An iron-rich mineral of the montmorillonite group was reported by Sudo and Ota (1952). Clino ptilolite was widely found as an alteration product (devitrification) of glass fragments. Further a sodium sulphate mineral (mirabilite) was recently found on the surface of the Oya-tuff in deep caves or on the ground. Pyrite and gypsum are rarely found in this locality. The purpose of this paper is to describe the mineralogical pro perties of celadonite found in the Oya-tuff. Mode of occurrence Bluish green patches are usually found in the Oya-tuff. Some of them immediately turn black when exposed in the air, while 3 0 0 Celadonite in the tuff of Oya, T Table 1. X-ray powder data of 1M illites, glauconite and celadonites. ochigi Prefe ctur e N . KOHYAMA, SHIMODA and T . SUDO 1. 1M illite (Levinson, 1955) ; 2. 1M illite (KA 60) (Kodama, 1962) ; 3. Glauconite (Warshaw, ASTM 9-439) ; 4. Celadonite (Wise and Eugster, 1964); 5. Oya-celadonite. 30 1 302 Celadonite in the tuff of Oya, Tochigi Prefecture Fig. 1. Microphotograph of Oya-celadonite. (C), celadonite ; (PI), plagioclase; (Q), quartz; (G), glass and clinoptilolite. others do not change colour in the air. The former contains an iron-rich montmorillonite and can easily be identified by the change of colour, and the latter is composed of celadonite. Under the mi croscope (Fig. 1), the patches are glass fragments altered into a bluish green mineral. The specimens in the present study were carefully collected by hand picking from the aggregates of the bluish green material, and the fractions smaller than 2 ƒÊ were ob tained by the usual sedimentation method. Mineralogical properties X-ray data: As shown in Table 1, X-ray powder reflections of the present specimen agree well with those of celadonite and glau conite. It is of the dioctahedral type as indicated by the 060 reflec tion at 1.51 A. The very weak 002 reflection at 5.0 A is due to the N. KOHYAMA, S. SHIMODA and T. SUDO 303 large amount o£ iron in the crystal structure. The powder pattern scarcely changed after heating at 500•Ž for one hour, however after heating at 700•Ž for one hour, slight shifts, were noticed of some principal lines, such as 10.1•¨10.2 A (001), 4.56•¨4.50 A (020, 110), Table 2. Observed X-ray data and calculated structure factors for the basal reflections of the Oya-celadonite. Fig. 2. One-dimensional Fourier projection of Oya-celadonite. The full and dotted curves indicate the observed and calculated electron densities respectively. 304 Celadonite in the tuff of Oya, Tochigi Prefecture 3.33•¨3.37 A (003), and 1.511•¨1.503 A (060, 330). These shifts suggest that dehydroxylation has caused an increase of the periodicity along the c*-direction and a decrease along a* and/or b*. No signs of interstratified minerals were detected in the X-ray diffraction pat terns. The X-ray powder reflections of the present sample are sharp, and the pattern is closer to that of the 1M mica than that of the 1 Md mica as far as those characteristic X-ray powder reflections appearing in the region of 23-29•‹in 20 (CuKa). A fairly good agreement was obtained between observed and calculated F-values based on a structural model of the 1M type (Table 2), and its one-dimensional Fourier projection is shown in Table 3. Chemical composition of celadonite and glauconite. * Ignition loss (at 120•Ž) ** Containing 0 .15% of Li2O (1). Oya-celadonite (2). Celadonite from Shiroishi, Miyagi Pref. (Sudo, 1951) (3). Glauconitic illite (Porrenga, 1968) (4). Celadonite (Wise & Eugster, 1964) (5). Glanconite (Warshaw, ASTM 9-439) N. KOHYAMA, S. SHIMODA and T. SUDO 305 Fig. 2. The value of ƒ°'|(|F0|-|Fc|)|/ƒ°|F0| for these basal reflec tions was 0.09. Chemical composition: As shown in Table 3, FeO and Al2O3 are contained more in the Oya-celadonite than those reported earlier, though there is no significant difference in the amounts of the other components between them. The structural formula (for a half-cell) was obtained on the basis of O10(OH)2 as follows: (K0.73Na0.18Ca0.02) (Mg0.30Mn0.01Fe2+0.44Fe3+0.25Al0.93) (Si3.99Al0.01)O10(OH)2. It is to be noticed that the total number of interlayer cations is 0.93 which is very close to 1.0, and the amount of Al substituting Fig. 3. Diagramatic expression of the chemical compositions of glauconite and celadonite. (1), (2), (3), (4) and (5) correspond to those used in Table 3. Data of glauconites: Hendricks & Ross, 1941; Burst, 1958; Deer, Howie & Zussman, 1962; Aida, 1968; Porrenga, 1968; Warshaw in ASTM. Data of celadonites: Hendricks & Ross, 1941; Sudo, 1955; Wise & Eugster, 1964. 306 Celadonite in the tuff of Oya, Tochigi Prefecture for Si in the tetrahedral sites is, extremely small. The chemical composition of the Oya-celadonite will be represented by a point near the region of celadonite in the diagrams prepared by Yoder and Eugster (1955) and Foster (1969). In Fig. 3, the relationship will be visualized between the amount of R3+ (IV) in the tetrahedral sites and the ratio R3+/(R2+R3+) of divalent and trivalent octahedral cations. These values R3+ (IV) and R3+/(R2++R3+) fall in the ranges, 0.2-0.4 and 0.65-0.80 in glauconite, and 0.0-0.3 and 0.45-0.70 in cela donite respectively. DTA curve: The DTA curve was recorded under the following conditions: weight of sample, 300mg; sample holder, nickel; mean heating rate, 10•Ž per minute. The result is shown in Fig. 4. The Fig. 4. DTA curve of Oya-celadonite. feature of the curve is similar to that of illite (Grim, 1953; Mackenzie, 1957) except that the temperature for the second endothermic peak is somewhat higher and the exothermic peak is rather enhanced in place of the s-shaped peak characteristic of illite. Electron micrograph: Electron micrographs of the present spe cimen show aggregates of lath-shaped and well-difined particles (Fig. 5). Infrared absorption spectrum: About 2mg of the specimen pow der was mixed with 200mg of KBr and pressed in vacuum under the pressure of 8 ton/cm2 with an oil presser. The infrared absorption spectrum is shown in Fig. 6 and Table N. KOHYAMA, S. SHIMODA and T. SUDO 307 Fig. 5. Electron micrographs of Oya-celadonite. 308 Ce1adonite in the tuff of Oya, Tochigi Prefecture Fig. 6. Infrared absorption spectrum of Oya-celadonite. 4. The OH stretching vibration bands (3600-3500cm-1), and the absorption bands in the region 1200-400cm-1 of the present specimen agree with those of ferric celadonite reported by Farmer and Russel (1963). A pair of double absorption bands will be seen at 1075 and 976 cm-1. According to Wise and Eugster (1964), these double bands will suggest the extremely small amount of Al in the tetrahedral sites. A considerable number of reports (Tuddenham & Lyon, 1959, Lyon & Tuddenham, 1960; Lyon, 1963; Liese, 1963) have been pu blished about the effect of the amount of Al in the tetrahedral sites upon the Si-O vibration revealed by infrared absorption spectra, and Wise and Eugster (1964) found that glauconite and celadonite can be discriminated by the infrared absorption spectra; glauconite (A1 (IV): 0.25-0.40) gives a single and/or a pair of double peaks in the region 1150-970cm-1 and celadonite (Al (IV): 0.0-0.3) a pair of double peaks. The present specimen shows a pair of double bands at 1075 and 976cm-1 and this fact is in accordance with its che mical composition. N. KOHYAMA, S. SHIMODA and T. SUDO 309 Table 4. Frequency (cm-1) of infrared absorption bands . s: strong, m: medium, w: weak, sh: shoulder, ?: unreported. 1. 1M illite (Oinuma & Hayashi, 1968); 2 and 3. Glauconite (Lyon, 1963); 4. Ferric-celadonite (Lyon, 1963); 5. Ferric-celadonite (Farmer & Russel, 1963); 6. Oya-celadonite. Discussion and conclusion Glauconite and celadonite are minerals akin to each other and were often considered to be different from each other in the modes of occurrence and paragenesis (Hendricks & Ross, 1941), or in the mode of origin (Savich-Zablotzky, 1954). However, recent studies 310 Celadonite in the tuff of Oya, Tochigi Prefecture have revealed the difference of chemical composition between glau conite and celadonite, and at the same time, it has been noticed that the chemical compositions of these minerals show some correla tions to their other properties. (Hendricks & Ross 1941; Sudo, 1949; Yoder & Eugster 1955; Wise & Eugster, 1964; Foster, 1969).
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