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Corrosion of Limestone Tablets in Sulfidic Ground-Water: Measurements and Speleogenetic Implications Sandro Galdenzi1

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Corrosion of Limestone Tablets in Sulfidic Ground-Water: Measurements and Speleogenetic Implications Sandro Galdenzi1 International Journal of Speleology 41(2) 149-159 Tampa, FL (USA) July 2012 Available online at scholarcommons.usf.edu/ijs/ & www.ijs.speleo.it International Journal of Speleology Official Journal of Union Internationale de Spéléologie Corrosion of limestone tablets in sulfidic ground-water: measurements and speleogenetic implications Sandro Galdenzi1 Abstract: Galdenzi S. 2012. Corrosion of limestone tablets in sulfidic ground-water: measurements and speleogenetic implications. International Journal of Speleology, 41(2), 149-159. Tampa, FL (USA). ISSN 0392-6672. http://dx.doi.org/10.5038/1827-806X.41.2.3 The measurement of the weight loss in limestone tablets placed in the Grotta del Fiume (Frasassi, Italy) provided data on the rate of limestone dissolution due to the sulfidic water and on the influence of local environmental conditions. A linear average corrosion rate of 24 mm ka-1 was measured in stagnant water, while the values were higher (68-119 mm ka-1) where the hydrologic conditions facilitate water movement and gas exchanges. In these zones the increase in water aggressivity is due to mixing with descending, O2-rich, seepage water and is also favored by easier gas exchange between ground-water and the cave atmosphere. Very intense corrosion was due to weakly turbulent flow, which caused evident changes in the tablets shape in few months. A comparison between the measured corrosion rates and the cave features showed that the values measured in the pools with stagnant water are too low to account for the largest solutional cave development, while the average values measured in the zones with moving water are compatible with the dimension of the cave rooms in the main cave levels, that must have developed when the base level was stable and hydrologic conditions favored the increase of water aggressivity. Keywords: karst corrosion; sulfidic water; limestone tablets; Frasassi caves Received 10 November 2011; Revised 29 January 2012; Accepted 7 February 2012 studied to get information about the mechanism of INTRODUCTION the cave development or the role of microbes: Cueva Many caves in the world were formed by sulfu- de Villa Luz (Hose et al., 2000), Movile (Sarbu & Kane, ric acid solution, one of the most efficient and rapid 1995), Frasassi (Sarbu et al., 2000; Macalady et al., mechanisms of cave development. In these caves, the 2006, 2007), Lower Kane Cave, Engel et al., 2004). oxidation of H S dissolved in the water is the most 2 Limestone corrosion rates due to sulfidic water important source of water aggressiveness. The H SO 2 4 were measured in the Grotta del Fiume at Frasassi, produced in the process interacts with the limestone, where limestone tablets were exposed for five years in contributing to its dissolution. In a limestone cave, the cave (Galdenzi et al., 1997). The corrosion rates the most evident byproduct is the deposition of re- were high, both in the water and in the atmosphere. placement gypsum on the cave walls exposed to H S 2 The tablets exposed to acidic exhalations in the exhalations. cave atmosphere were covered by a layer of replace- The corrosion due to H S released by the ground- 2 ment gypsum, and the limestone surface below the water was thought capable of creating entire caves gypsum layer was severely corroded, with deep pock- (Principi, 1931; Egemeier, 1981). The dissolution of ets. The weight loss in these tablets reached high limestone however also occurs underwater, and the values (linear corrosion rate up to 85 mm ka-1, with development of caves in deep zones of a sulfidic aqui- gypsum being removed before each measurement), fer have been hypothesized in Guadalupe Mountains and the average rate increased from 42 to 69 mm ka-1 caves (Davis, 1980; Hill, 1987), while the co-existence after 2.5 and 5 years of exposure. The site conditions of important solutional processes above and below strongly influenced the results and significant differ- the water-table was documented in the Frasassi caves ences occurred in tablets located only a few cm apart, (Galdenzi, 1990). depending on the acidic flow path. Caves produced by sulfuric acid reaction are gen- The corrosion rate of tablets placed underwater erally hypogenic and are known in different hydro- was about 58 mm ka-1, and the rate did not vary de- geology and morphologic conditions (Palmer 1991; pending on the length of exposure and site conditions. Klimchouk & Ford, 2009). Some active caves are The limestone had a slightly rough surface with cal- known in the world, although few of them have been cite veins protruding in relief (����������������������Fig. 1). �������������Similar meas- urements made in another noncirculating body of wa- ter in Frassasi (Mariani et al., 2007) resulted in low 1 Viale Verdi, 10 Jesi, Italy ([email protected]) corrosion values. 150 Corrosion of limestone tablets in sulfidic ground-water Fig. 1. Limestone tablets after five years of exposure in the cave (after Galdenzi et al., 1997). A tablet placed in the ground-water (right) and one corroded in the cave atmosphere, after the removal Fig. 2. Plan view of the caves. of the replacement gypsum (left). The limestone tablets were placed in different cave pools to verify the local corrosion rate and compare In this paper, the results of a new cycle of mea- it with the data already acquired in Ramo Sulfureo surements will be discussed. Some limestone tab- (Galdenzi et al., 1997). The experiment started in lets were newly placed in the cave with the purpose November 2006, with a planned duration of two years, to quantify the corrosion due to the direct action of and two different sites were chosen: Lago Verde, in ground-water in different setting and through differ- the Grotta del Fiume, the most important cave in the ent seasons. In this case corrosion due to H2S in the Frasassi Gorge and the Grotta Sulfurea, close to the cave air was not measured. sulfidic spring (Fig. 2). In June 2007 a new set of tablets was placed in THE USE OF LIMESTONE TABLETS the Grotta del Fiume to verify a possible influence of The use of limestone tablets to quantify the rate of seasonal cycles on the corrosion rate. These tablets erosion in the surface karst processes was introduced were placed in Ramo Sulfureo, exactly in the same by Trudgill (1975) and Gams (1985). This method was place as the 1997 experiments. One tablet remained also used to measure active corrosion processes due continuously in the water for two years, while some to sulfidic water in the cave environment (Galdenzi et tablets were placed and removed from the same lo- al., 1997). cation according to season. Some tablets were used The same procedure used by Galdenzi et al. (1997) in the wet period, and the others in the dry period. to prepare the limestone tablets was also used here to Each “seasonal” tablet therefore was placed, removed, better compare the old and new data. The tablets were weighted and newly placed following the hydrologic prepared with limestone blocks taken from local quar- cycle. An additional “seasonal” station was also cre- ries. A pure micritic limestone (Calcare Maiolica Fm., ated in the Lago Verde, near the previously placed Early Cretaceous) was used due to its homogeneity tablets. facilitating the preparation and weighing of tablets, During the measurement period, technical diffi- and also because the cave develops at least in part in culties resulted in changes to the planned procedure. this formation. In particular the station in the Grotta Sulfurea was The limestone was cut into tablets about 8 x 4 x soon discarded. Seasonal changes in flow moved the 0.8 cm, which were polished, measured in detail to soft sediment in the bottom of the pool disrupting the get their total surface area, and weighed after being conditions of tablet exposure. For this reason, Ramo dried at 110°C. Their initial mass varied between 60 Sulfureo and Lago Verde remained the only monitored and 70 g. The tablets were placed in the cave using a places. nylon string and, at the end of the exposure period, Throughout the whole period, data loggers placed they were washed, dried and weighed again. The ra- in the cave got almost continuous data on water level tio between weight loss and area of each tablet was and conductivity. These instruments stayed in the cave then referred to a standard period of exposure to get for an independent study of the ground-water flow pat- comparable data. For this reason, the weight loss is terns, which data are useful also in the discussion of reported as mg cm-2 a-1 represented as an estimated experimental results on the corrosion rate. linear corrosion rate (mm ka-1). International Journal of Speleology, 41(2), 149-159. Tampa, FL (USA). July 2012 Sandro Galdenzi 151 THE CAVE HYDROLOGY The hydrologic year can be divided into two pe- The ground-water chemistry is well known, and a riods, roughly corresponding to a “wet season”, in recent study provides detailed information (Galdenzi winter and spring, and a “dry season”, in summer et al., 2008). The sulfidic water in the main aquifer and autumn. These periods are poorly related to rain is cold (~13°C), and has a higher salinity (up to 2 g distribution, that evidence two maxima, the main L−1) than the normal bicarbonate water infiltrating one in autumn, and a secondary one in the spring. from the karst surface. It is enriched in sodium and Only winter and spring precipitations directly influ- chloride, and contains sulfate and hydrogen sulfide. ence the ground-water, because evapotranspiration Mixing phenomena between descending bicarbonate in the summer and soil storage in the autumn reduce and rising mineralized water determine the composi- the amount of recharge.
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