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Zeolitic Alteration of Eocene Volcaniclastic Sediments at Metaxades, Thrace, Greece

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Zeolitic Alteration of Eocene Volcaniclastic Sediments at Metaxades, Thrace, Greece Applied Clay Science, 7 (1993) 509-526 509 Elsevier Science Publishers B.V., Amsterdam Zeolitic alteration of Eocene volcaniclastic sediments at Metaxades, Thrace, Greece A. Tsirambides, A. Filippidis and A. Kassoli-Fournaraki Department of Mineralogy-Petrology-Economic Geology, Aristotle University of Thessaloniki, 540 06 Thessaloniki, Greece (Received May 12, 1992; revised and accepted November 27, 1992) ABSTRACT Tsirambides, A., Filippidis, A. and Kassoli-Fournaraki, A., 1993. Zeolitic alteration of Eocene vol- caniclastic sediments at Metaxades, Thrace, Greece. Appl. Clay Sci., 7: 509-526. The conditions of alteration of the upper Eocene zeolite-bearing volcaniclastic sediments at Metax- ades, Thrace, Greece, were examined using a variety of petrographic and mineralogical techniques. A fine silt- to clay-size matrix, containing abundant altered glass shards, predominates. The primary minerals include quartz, K-feldspar, plagioclase, micas (especially biotite) and some opaque min- erals. The diagenetic phases, clinoptilolite, smectite and cristobalite, occur as microcrystalline aggre- gates within the matrix or as replacements of glass shards. The abundances of cristobalite and clinop- tilolite are related chiefly to the original composition of the rocks. The abundance of cristobalite increases and that of clinoptilolite+ smectite decreases as the abundance of the matrix increases. The formation of clinoptiloliteand cristobalite took place either at near-surface temperatures or at slightly elevated temperatures (lower than 70°C). The smectite content of the altered volcaniclastics de- creases with increasing depth in the 15 m thick exposed section. No other systematic variation in mineral assemblages with depth was observed. However, the ratio clinoptilolite/smectite increases systematically with depth suggesting to us that smectite may have formed subsequent to the formation of clinoptilolite and as an alteration product of clinoptilolite. The initial composition of the volcanic material and to a less extent the interstitial fluids, greatly affected the diagenetic mineral assemblages of the final alteration products. INTRODUCTION The variety of diagenetic minerals which can form in volcaniclastic sedi- ments is large and reflects both the nature of the parent rock and the condi- tions under which the alteration occurs (Boles and Coombs, 1975; Mumpton, 1977; Boles and Surdam, 1979). Zeolites are among the most abundant and widespread diagenetic silicates in these rocks. Correspondence to: A. Tsirambides, Department of Mineralogy-Petrology-EconomicGeology, Aristotle University of Thessaioniki, 540 06 Thessaloniki, Greece. 0169-1317/93/$06.00 © 1993 Elsevier Science Publishers B.V. All rights reserved. 510 A. TSIRAMBIDES ET AI, Zeolite-rich volcaniclastic rocks of Paleogene age, deposited in a marine environment, cover an area of several hundred square kilometers of Greece and Bulgaria in the eastern Balkan peninsula. These volcaniclastics consist of fine- to coarse-grained ash-falls and ash-flows, the latter of which contain a small but variable component of non-volcanogenic detritus of a wide range of grain sizes. The zeolitic alteration of these rocks has been studied by Aleksiev and Djourova ( 1975 ), Djourova and Aleksiev ( 1989 ), Tsirambides et al. ( 1989 ) and Tsolis-Katagas and Katagas ( 1990 ). There is little agreement among these authors about the temperature, fluid chemistry and other parameters which affected the alteration of the volcaniclastic rocks. Aleksiev and Djourova (1975) concluded that the zeolitic alteration of ash-flows in the Bulgarian territory occurred after deposition, as the result of infiltration of marine and meteoric water into hot ignimbrites. In contrast, Tsolis-Katagas and Katagas (1990) reported that the pyroclastic rocks in the Greek portion of the region were affected by burial diagenesis at temperatures intermediate between Iiji- ma's (1978) zones II and Ill. This study is an examination of the alteration products and processes of the zeolite-bearing volcaniclastic rocks of Metaxades, Thrace, Greece. Using a variety of petrographic and mineralogical techniques we have attempted to set limits on the conditions under which both zeolites and non-zeolitic dia- genetic silicates were formed. GEOLOGICAL SETTING During early Tertiary time the huge meta-Alpine basin of Thrace (Greece), was formed and filled with molassic sediments that lie unconformably on the Alpine rocks of the greater region. The area of our study lies along the south- ern edge of an elongated sub-basin which extends into Bulgaria (Fig. 1 ). The broader area is part of the Rhodope geotectonic zone that straddles the Greek- Bulgarian border. The volcaniclastic sediments of Metaxades have an upper Eocene age. Fytikas et al. ( 1984 ) reported, in a study of the evolution of Ter- tiary to Quaternary volcanism in the Aegean region, that rhyo-dacitic volca- nism occurred in the Rhodope area between 33 and 23.6 Ma. Aleksiev and Djourova (1975 ) interpreted the depositional environment as shallow marine. Solakius and Tsapralis ( 1987 ) come to the same conclu- sion on the basis of microfossils contained in the marl overlying the volcani- clastics and in marl pebbles included within the volcaniclastics. The structural features of the Metaxades deposits are similar to those listed by Fisher and Schmincke (1984) as characteristics of ash-falls and ash-flows. They exhibit massive-bedding in the upper and lower portions of the volca- niclastic sequence and thin to thick cross-bedding, as well as alignment-bed- ZEOLITICALTERATION OF EOCENE VOLCANICLASTICSEDIMENTS 511 ~'.. •. C:° o.. ~~'.~.....-...... :../ . N • ~'.'.!, • • • •- "~.'.-'.'-." J" ~':."."-" • ", " .. ~.,/,•°o° . ..\-; ..--.. -..~-~. -.'.-..-.-.-..~. U i~r• ~ e • - - ~ • -.-e ~.-:.-~-" " ".'" t •,,,~.,,,, ° ~,." o o..T-;-~,~.'.'-x:,:.,.~.mmc>zest.i.~ , • e..;/, , ~'v~l% ~., -~/..~. - e..~.--........-...~, - • ('.'.'~ ,.7~.1:1~~-" ".'.':~;--.--~ x -. "~ • ""~'.~~-~'_ :~'~-. - e-. ; ". -~ "" " " " "" " • -' --~-.'~._~o .'°;~" "" " ° ° o~'"" "" "' E .~ \~-'~o-~-/o o • • ° .'?..':.'.~' ).e~'~" • X~(. -.-..'.". ,,_._- ¢ :.".'-.\y ~~ ~.~.'...-..~ ..... " "" • "'.'" • 4 .'.: • " ~ " .'"'.', •4, • : .%.'" , • .- ~" ,~i, ~'~-i~-~ 2~.-/ alluvium • ._.t Bulg. ,~ •Holocene S~W'i,.... _~. [~Plio-Pleistocene sediments [~']Eocene molasse sediments ['~Oligocene molasse sediments L'~Diabase and serpentinite ~AC~lahibolites and gneisses GREECE Fig. 1. Geologic map and geographic position of the Metaxades area, Thrace, Greece (from Bornovas and Rondogianni-Tsiambaou, 1983). ding, in the middle portion. No structures attributable to post-depositional processes have been reported in the literature or noted in this study. A representative stratigraphic column of the Metaxades area is shown in Fig. 2. During early Lutetian (early Eocene) time, a basal clastic series of breccias and conglomerates was deposited unconformably upon the meta- morphosed basement. This series is unconformably overlain by Priabonian (upper Eocene) volcaniclastic tufts which are the focus of this study. Arikas (1979) reported that these tufts are interbedded with thin layers of sand- stones, siltstones and claystones, but we did not observe any interbedded clas- tic zones in the outcrops we studied. The tufts are a product of calc-alkaline volcanism which began in late Eocene time and reached maximum intensity during the Oligocene, during which time a series of marls and claystones con- taining intercalated rhyolites and tufts, was deposited overlying the Eocene sediments. Only a thin (about 1 m) layer of these exists in our area. Finally, a transgressive sequence, about 2 m thick, of Miocene coastal sediments (mainly porous limestones, rich in marine microfossils, marls and sand- ,5 1 ~, A TSIRAMB1DES ErI ' A i massive -i7" ~~¢'- - bedded al ignment and l cross-bedded F2 Fa massive bedded Fig. 2. Representative stratigraphic column of the Metaxades area, Thrace, Greece. ko= Miocene marly limestone; F~ = Oligoeene marl and clay with thin layers of sandstone and tuff; F2 = Upper Eocene volcanic tuff in layers alternating with thin sandstone, siltstone and claystone; F3 = Lower Eocene conglomerate and breccia; F4 = Metamorphic bedrock (amphibolites and gneisses ). Fig- ure also shows the detailed section of the stratigraphic interval sampled in this study. Con- structed using data from Arikas (1979), Solakius and Tsapralis (1987) and our own field observations. stones) was deposited on the Oligocene sediment (Solakius and Tsapralis, 1987). Tsolis-Katagas and Katagas (1990) estimated that the maximum depth to which the volcaniclastic sediments of the Metaxades area have been buried is 1500 m. The average geothermal gradient in Thrace at depths < 1400 m is 37 °C/km (Fytikas and Kolios, 1979). This would imply a maximum tem- perature of the volcaniclastic sediments of 70°C (assuming a surface temper- ature of 15 °C), in the absence of local heating by volcanic or hydrothermal activity. MATERIALS AND METHODS The geological observations in this study are based on the examination of three quarry faces and several outcrops. The samples analyzed were taken from vertical sections with thicknesses of 15 and 10 m in two of the quarry faces. None of the sections studied penetrated entirely through the volcani- clastic section, which was inferred by Tsolis-Katagas and Katagas (1990) from drilling data in nearby regions to have a maximum thickness of 35 m. ZEOLITIC ALTERATION OF EOCENE VOLCANICLASTIC SEDIMENTS 513 Thin sections were
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