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b,*
University of Blida, Science Engineering Faculty, BP. 270, Soummaa-Blida, Algeria UMR CNRS-UPS IDES, Bat. 504, Universite Paris-Sud, 91405 Orsay, France
Received 1 July 2005; received in revised form 29 December 2005; accepted 3 January 2006
KEYWORDS
Chlorine-36; Sahara; Conned aquifer; Groundwater; Residence time; Permeability
Summary The Continental Intercalaire from Sahara is one of the largest conned aquifers in the world. In the northern part of the basin, the depth of the aquifer ranges between 400 and 1800 m and the main ow direction is from west to east. Chlorine-36 analyses were performed on groundwater samples mainly collected along this owpath. They show a wide range of 36Cl contents, from 8 to 99 1015 at at1 expressed as 36Cl/Cl atomic ratio. In order to evaluate the epigene production, measurements were also performed on chloride extracted by leaching from a soil prole, near the recharge zone. This showed that the contribution of epigene production remains limited. A range of 36Cl/Cl ratios from 116 to 133 1015 was adopted for groundwater recharging the aquifer, including both meteoric production and epigene production. For most of the samples collected along the main owpath, a signicant decay effect was observed. An attempt of dating was made by using an equation that takes into account radioactive decay of the meteoricepigene input, deep production and chloride dissolution within the aquifer. The calculated 36Cl residence time varies from 16 to 500 ka for the minimum ages, and from 25 to 1200 ka for the maximum ages. An increase of residence time is observed up to about 500 km from the recharge zone. This corresponds to mean ow velocities of 0.20.5 m a1 and to an average permeability of 1.1 0.6 105 m s1, at the scale of several hundreds of kilometres. 2006 Elsevier B.V. All rights reserved.
Introduction
In the northern part of Sahara desert is located one of the world largest groundwater systems, the deep Continental Intercalaire (C.I.), extending across three countries, Alge* Corresponding author. Tel.: +33 1 6915 6791; fax: +33 1 6915 4917. E-mail address: michelot@geol.u-psud.fr (J.-L. Michelot).
ria, Tunisia and Libya, over an area of approximately 600,000 km2. The C.I. reservoir is vital in that arid region, where groundwater is virtually the only perennial resource. This resource is generally considered as being fossil, i.e., inherited from previous climatic conditions, more humid than at present, with a very limited modern recharge. However, it is very important, for the resource management, to estimate, even approximately, the age of such fossil groundwater. These estimates may provide an inde-
0022-1694/$ - see front matter 2006 Elsevier B.V. All rights reserved. doi:10.1016/j.jhydrol.2006.01.002
Chlorine-36 dating of deep groundwater from northern Sahara pendent check on ow velocities that are calculated using Darcys law, or on the validity at regional scale of punctual measurements of hydraulic conductivity (pumping tests). The radiocarbon method cannot be used for dating of C.I. groundwater: 14C contents are very low, close to, or often below, the detection limit (UNESCO, 1972; Gonantini et al., 1974; Guendouz, 1985; Edmunds et al., 1997). Chlorine-36, with its long half-life (301,000 a), is a good candidate to obtain information about residence time of C.I. groundwater. Some 36Cl measurements were performed for groundwater dating in the Great Oriental Erg as early as 1985 (Fontes et al., 1985; Guendouz, 1985; Michelot et al., 1989a). Complementary sampling was realized in 1994 in order to improve the covering of the basin, and to check the preliminary hypotheses that were built on the rst measurements. The main objective of the present paper is to gather all these unpublished 36Cl data, and to examine how they may be interpreted in terms of groundwater residence time.
573 taceous (Neocomian, Barremian, Aptian, Albian). The aquifer is continuous north to south, from the Saharan Atlas to the Tassili of Ahaggar, and west to east, from the Guir-Saoura valley to the Libyan desert (Fig. 1). A major NS structure, the Mzab dorsal (Cornet, 1964; UNESCO, 1972; Bishop, 1975) divides the basin into two sub-basins (occidental and oriental). The studied area is situated in the oriental basin (Great Oriental Erg), which crosses Algeria, Tunisia and Libya. In this eastern part, the C.I. aquifer is overlain by a homogeneous layer of Cenomanian clays and evaporites. It is located within a complex succession of clastic sediments of Mesozoic age, the thickness and lithology of which show signicant lateral variations. The depth of the aquifer roof increases from south to north. It is approximately 1000 m below the surface in the lower Sahara and reaches 2000 m in the region of the saline lakes of Chott Melrhir (Algeria) and Chott Djerid (Tunisia), thus giving rise to a high artesian pressure (Fig. 2). The principal features of the geological succession in Algeria and Tunisia are shown in Fig. 2. In the centre of the basin, the strata forming the reservoir are purely continental in facies, whilst towards the borders, especially in the east, appear rst lacustrine facies and then marine facies. At its maximum, the aquifer thickness exceeds
Figure 1
574
Figure 2 Schematic cross-section of the Continental Intercalaire aquifer in Algeria and Tunisia, showing the main aquifer horizons (after Edmunds et al., 1997).
Figure 3 Spatial variability of selected hydrochemical parameters (conductivity, SO2 , Cl, Na+, K+, Br) along the main ow path 4 in Algeria (data from Edmunds et al., 1997).
1500 m. The geological succession is differentiated into several units of detrital sediments separated by clay-rich strata, leading to a high degree of heterogeneity in the heart of the
C.I. aquifer. Some thin but relatively permeable horizons may be very important in controlling groundwater ow and hydraulic continuity. This phenomenon is particularly
Chlorine-36 dating of deep groundwater from northern Sahara marked where the Saharan platform passes to the lower-Sahara region in the south: thickening of the units and lithological changes give rise to changes in piezometry and chemical composition of water. In this southern region, which has been tectonically very active, faulting has introduced some lateral compartmentalisation in the C.I. aquifer (UNESCO, 1972; Edmunds et al., 1997). Groundwater ows in the C.I. of the Great Oriental Erg converge towards a single discharge zone in Tunisia (Chott Djerid/Chott Fedjedj region and Gulf of Gabes). The main ` owpath, WE, comes from the Saharan Atlas and the MZab dorsal in Algeria. Two secondary ow directions may be distinguished: SWNE from southern Algeria and SN from the Dahar region of Tunisia.
575 path (WE) (Fig. 5). The other six were sampled in the central area of Great Oriental Erg basin and in the Atlas border. After removing SO2 ions from the water samples with 4 2+ Ba , Cl was precipitated by adding AgNO3. The AgCl precipitates were repeatedly dissolved in ultrapure NH4OH, ltered and re-precipitated with HNO3. The puried AgCl samples were dried and placed in sealed boxes. The 36Cl/Cl ratios were measured by accelerator mass spectrometry (AMS) at the Rochester University (USA) (Elmore et al., 1979) for the groundwater samples collected in 1985, and at the Australian National University (Field et al., 1990) for the samples collected in 1994. Chlorine-36 contents (Table 1), expressed as atomic ratio (36Cl/Cl) and in atomic concentration (at l1), vary, respectively, from 8 to 99 1015 at at1 and from 0.90 to 3.53 108 at l1.
Meteoric production of
36
Cl
The contribution of 36Cl of meteoric origin may be estimated from the natural fallout rate prevailing prior to the
10000
Sodium (mg.l-1)
1000
C.I. Groundwater Halite Dissolution Line 100 100 1000 Chloride (mg.l-1) 10000
a
10
Bromide (mg.l-1)
Chlorine-36
Sample preparation and
36
10000
Cl measurement
Fifteen samples, collected in 1985 and 1994 from the C.I. aquifer were analysed for chlorine-36. Among these samples, nine were collected along the main groundwater ow-
Figure 4 Chloride versus sodium concentrations (a) and chloride versus bromide concentrations (b) in groundwaters from the Continental Intercalaire aquifer (data from Edmunds et al., 1997).
576
Figure 5
36
nuclear tests (Lal and Peters, 1967). At the latitude of the C.I. aquifer recharge area (Saharan Atlas, $34N), this contribution would be approximately of 25 at m2 s1. Taking into account a mean annual precipitation of 100 mm (Dubief, 1963; ONM, 19802000), a present-day evapotranspiration rate of 97.5% (ONM, 19802000) and a chloride concentration in precipitation of 4 mg l1 (Moulla and Guendouz, 1996), this would correspond to a 36Cl concentration of about 3 108 at l1, and to a 36Cl/Cl ratio of about 116 1015 at at1.
These numbers are calculated for the present-day arid conditions. These conditions have obviously changed with time and it is highly probable that annual precipitation, evaporation rate and perhaps chloride concentration of precipitation have varied since recharge has occurred. The atmospheric production rate of chlorine-36 itself was not constant with time, due to variations of geomagnetic eld intensity, as documented by 36Cl data from ice cores (see, e.g. Wagner et al., 2000; Beer et al., 2002). It is very difcult to assess such variations, over several hundreds of
Table 1 Oxygen-18, deuterium, chloride and chlorine-36 concentrations in groundwater from the C.I. aquifer (stable isotope data from Guendouz, 1985 and Edmunds et al., 1997) Sampling site Berriane Laghouat Rhourde-El-Baguel Hassi-Messaoud Djamaa Tolga Hassi-Delaa Touggourt Hadjira Ette bat Oued-Souf (S. Berry) Oued-Souf (Town) Zelfana Metlili Gassi-Touil Ref. no. 01 06 07 09 11 14 17 18 30 37 38 39 42 45 64 d18O (&V-SMOW) 8.1 7.7 8.5 8.6 8.2 8.3 8.1 8.3 8.3 7.9 8.0 8.1 8.2 8.0 8.3 d2H (&V-SMOW) 60 53 60 61 61 61 58 59 60 61 61 63 61 56 64 Cl (mg l1) 188 234 1000 400 426 550 318 533 550 560 426 480 511 210 1300
36
36
Cl (108 at l1)
95 8 61 7 19 5 26 6 15 5 37 12 64 5 10 5 18 8 23 3 13.5 3 25 3 29 8 99 34 83
3.05 0.25 2.43 0.28 3.23 0.85 1.77 0.40 1.09 0.36 3.45 1.12 3.46 0.27 0.90 0.42 1.68 0.75 2.19 0.28 1.10 0.24 2.04 0.24 2.52 0.69 3.53 1.21 1.76 0.66
Chlorine-36 dating of deep groundwater from northern Sahara thousands of years, but the large uncertainties they induce have to be kept in mind.
577 duction and epigene production, under the present-day climatic conditions. This range is almost identical to the estimate of initial 36Cl/Cl ratio (131 11 1015) recently obtained by Sturchio et al. (2004) for the Nubian Aquifer (equivalent to C.I.) in Egypt, from the correlation between 36 Cl/Cl ratio and 81Kr ages. It is also in very good agreement with the value (125 10 1015) estimated by Love et al. (2000) for the Great Artesian Basin, in Australia.
Table 2 Chlorine-36 contents of chloride extracted by leaching from a soil prole located near the recharge area of the C.I. aquifer Depth (cm) 1020 3050 6580 80100 135140 255270 340360
36
160 Main W-E Flowpath (Albian) Main W-E Flowpath (Barremian) Saharan Atlas Border (Albian) Grand Erg Oriental Calculated Meteoric Production
140
120
100
80
Mixing Zone
36
60
0.006
0.007
0.008
1/Cl (1/mg.l )
Figure 6
36
Cl/Cl versus 1/Cl relationship in groundwaters from the Continental Intercalaire aquifer.
578
A. Guendouz, J.-L. Michelot the generally admitted secular equilibrium values for sedimentary rocks: it brackets the value of 4.68 1015 calculated for typical sandstone by Bentley et al. (1986). In Fig. 6, three different types of samples are within the mixing zone: the samples taken near recharge area on the main owpath, most of the samples collected near the Atlas border, and two samples from the centre of the Great Oriental Erg. For all these samples, chloride dissolution is the main factor controlling the 36Cl/Cl ratios, and 36Cl concentrations cannot be used to compute a residence time of water. On the other hand, for most of the samples collected along the main owpath, a signicant decay effect is observed. This is conrmed by Fig. 7 where a decreasing trend in 36Cl concentrations, expressed in atoms per litre, with the distance to the recharge zone clearly appears. This trend can only result from radioactive decay and/or from a general increase of 36Cl concentration in recharge water with time (from past to present), which could result from an increase of evaporation rate in the recharge area due to a progressive aridication of climate. However, we believe that the former phenomenon, radioactive decay, prevails because: (i) a simple continuous trend to aridication over the (very long) considered period of time is very unlikely, an alternance of humid and dry periods being much more probable, (ii) the 36Cl/Cl ratios also decreases,
5 Main W-E Flowpath (Albian) 4.5 4 3.5 Main W-E Flowpath (Barremian) Meteoric-Epigene Production
3 2.5 2 1.5 1 0.5 0 0 100 200 300 400 500 600 700 800
579
Sampling site Berriane Metlili Zelfana Hadjira Djamaa Touggourt Ette bat Oued-Souf (Town) Oued-Souf (S. Berry)
36
36
95 8 99 34 29 8 18 8 15 5 10 5 23 3 25 3 13.5 3
0 < 17 > 55 0 < 0 > 134 0 < 98 > 238 113 < 273 > 529 339 < 464 > 640 366 < 542 > 844 106 < 159 > 220 140 < 190 > 245 422 < 509 > 619
49 < 87 > 129 0 < 20 > 223 130 < 271 > 479 306 < 561 > 1261 593 < 827 > 1372 730 < 1275 > Sec.Eq. 298 < 377 > 474 319 < 390 > 474 743 < 932 > 1275
Age Min. is calculated by using minimum value for initial ratio and maximum value for secular equilibrium ratio. Age Max. is calculated by using maximum value for initial ratio and minimum value for secular equilibrium ratio. Analytical uncertainties are also taken into account.
(iii) even when the chloride concentration is almost constant (samples 42, 30, 11, 18), the 36Cl concentration still decreases; thus, radioactive decay is clearly involved and this is a favourable case for the application of 36Cl dating method, as stated by Andrews and Fontes (1993). An attempt of dating can be made by using a general equation with three terms that take into account (i) radioactive decay of the meteoricepigene input, (ii) deep production and (iii) chloride dissolution within the aquifer (Michelot, 1988; Michelot et al., 1989b): RC Ri Ci ekt Re Ci 1 ekt Re C Ci where R and C are the measured 36Cl/Cl ratio and Cl concentration of groundwater, Ri and Ci are the initial 36Cl/Cl ratio and Cl concentration at the aquifer recharge, Re is the 36Cl/Cl ratio at secular equilibrium, and k is the decay constant for 36Cl. Time estimates have been calculated with a Ri value of 116 and Re value of 0, in order to obtain a minimum age, and with a Ri value of 133 and Re value of 8 in order to obtain a maximum age. Results are presented in Table 3. The calculated 36Cl residence time, for the points situated on the main owpath, ranges from 16 to 500 ka for the minimum age, and from 25 to 1200 ka for the maximum age. A continuous increase of residence time is observed up to about 500 km from the recharge zone. Beyond this limit, for three samples (37, 38 and 39), the distribution of the calculated residence times does not follow any longer this logical trend. It is difcult to precisely determine the reasons of change in the behaviour with only three samples. However, this limit corresponds also to: a change in the lithology (from sands, sandstone and clay in the west towards sandstone, limestone, dolomite, anhydrite and clayey facies in the east), a change in the tapped horizon (Albian to Barremian), a relative rise of the C.I. basement in the east of the ow direction, a general change of the geochemical tracer behaviours (see Edmunds et al., 2003).
580
Acknowledgements
This work is dedicated to the memory of the late Professors J.Ch. Fontes and J.N. Andrews. Under the direction of the rst named, we performed in 1984 the rst sampling campaign related to the investigation of 36Cl contents in groundwater from the C.I. in Algeria, with a rst trial of interpretation. In 1985, J.N. Andrews joined the team for a second sampling program. We thank Dr. D. Elmore (formerly at Rochester University, USA) and the Dr. L.K. Field (National Australian University, in Canberra) for AMS analyses of 36Cl. We also thank Dr. A.S. Moulla, (Algiers Nuclear Research Centre, Applied Hydrology and Sedimentology Department) for his help during complementary eldwork and during the preparation of the manuscript.
References
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