Environ Earth Sci (2016) 75:105 DOI 10.1007/s12665-015-4913-6

ORIGINAL ARTICLE

Composition and origin of the sabkha brines, and their environmental impact on infrastructure in Jizan area, Coast,

1 1,2 Mohammed H. Basyoni • Mahmoud A. Aref

Received: 2 March 2015 / Accepted: 8 August 2015 Ó Springer-Verlag Berlin Heidelberg 2015

Abstract The sulfate ( and is of modified marine water having an elevated CaCl2 con- ) and brines of Jizan sabkha cause corrosion of the tent, which may be derived from dissolution of mixed salt steel reinforcement and deterioration of the concrete, and from the Miocene salt dome in Jizan area. The chemical consequently hinder the development activity for building composition and origin of the brines, and mineralogy and new urban communities and industrial zones in Jizan area, textures of the evaporite minerals in Jizan sabkha help in Red Sea coastal plain of Saudi Arabia. The sabkha evaporite understanding the nature of the corrosive factors to the minerals below the sediment surface are represented by foundations in Jizan area. displacive and inclusive growth of lenticular and rosette gypsum, and nodular anhydrite. In small saline pans, Keywords Brine chemistry Á Genesis Á Gypsum Á precipitates form rafts, chevrons and cornets. The salinity Corrosion Á Infrastructure Á Sabkha Á Saudi Arabia (TDS) of the in the sabkha area is highly vari- able, and ranges from 12,900 to 495,000 mg/l, compared to the average value of the Red Sea water of 40,366 mg/l. The Introduction low salinity values of the sabkha brines are most probably caused by localized influx of groundwater of meteoric origin Sabkhas are ubiquitous geomorphic features in arid and from direct rain fall and/or temporary floods, in addition to semiarid regions where evapotranspiration potentials are seepage of sewage water from septic tanks. The electric very high and the hydrological inputs are conducive to the conductivity (EC) values range from 20,000 to 199,100 lS/ development of endoreic (internal) drainage systems cm which are conformable to the salinity values of the brine. (Goudie and Wells 1995; Shaw and Thomas 1997). They The dominant cation concentration order in seawater represent flat and barren surfaces that are in dynamic and brines of the sabkha is Na? [ Mg2? [ Ca2? [ K?,or equilibrium with eolian deflation and sedimentation con- Na? [ Mg2? [ K? [ Ca2?. The dominant anion concen- trolled by local water table level. Major geotechnical and - 2- - tration order is Cl [ SO4 [ HCO3 . The dominant brine constructional problems, namely, strength loss, differential type for most samples is sodium chloride, with variable settlement, concrete deterioration, and steel corrosion may proportions of the major cations Ca2? and Mg2? and the emerge due to the presence of sabkha (Abou Al-Heija and 2- major anion SO4 . Most brine samples indicate their source Shehata 1989; Shehata et al. 1990; Youssef et al. 2012; Youssef and Maerz 2013). In addition, salt crystallization usually occurs in the concrete pores above the water & Mahmoud A. Aref table leading to their slow disintegration due to the high [email protected] crystallization pressure that is enhanced by evaporation (Al-Amoudi and Abduljauwad 1994; Al-Amoudi et al. 1 Department of Petroleum Geology and Sedimentology, Faculty of Earth Sciences, King Abdulaziz University, 1995). There are three different models that explain the Jeddah, Saudi Arabia sources of the groundwater and solutes in sabkhas. These 2 Geology Department, Faculty of Science, Cairo University, are the ‘‘seawater flooding’’ model that was proposed by Giza, Egypt Kinsman (1969), Butler (1969), and Patterson and Kinsman 123 105 Page 2 of 17 Environ Earth Sci (2016) 75:105

(1977, 1981). The ‘‘evaporative pumping’’ model was Jizan sabkha. The water and brine samples were taken in proposed by Hsu¨ and Siegenthaler (1969); Hsu¨ and Sch- this area from seawater, groundwater, surface shallow pan neider (1973), and McKenzie et al. (1980). The recent or surface excavations in Jizan sabkha (Fig. 1; Tables 1, 2). model of ‘‘ascending brine’’ or ‘‘conceptual’’ model was During the field work, the salinity, temperature and pH proposed by Wood and Sanford (2002), Yechieli and Wood value of the brine in trenches dug in the sabkha were (2002), Wood et al. (2005), and Tyler et al. (2006) for the measured. The salinity was determined by glass hydrom- recent sabkha and most coastal-sabkha environments. In eters taking into account the measuring of standard sea this model, capillary forces bring solutes and water to the water. The hydrometer measures the mass % NaCl in the surface, where the water evaporates and halite and other brine up to 250 %. Temperatures were measured at the soluble minerals are precipitated. Retrograde minerals, surface by mercury thermometer ranging from 0 to 100 °C sensu Wood et al. (2005), such as gypsum, anhydrite, in 0.1 °C divisions. The density of the brine samples was calcite, and dolomite precipitate and accumulate in the measured by using two portable glass hydrometers, the first capillary zone beneath the surface of the coastal sabkha. measures density from 1.00 to 1.10 g/cm3, and the second Sabkha sediments in Jizan area have a negative impact measures density from 1.10 to 1.2 g/cm3. The pH value of on infrastructure causing problems to buildings. The degree the brine was measured in the field by these portable pH- of damage depends on the characteristics of the sabkha, the meters. Thirteen (13) samples (10 samples from sabkha amount of subsidence and the bearing capacity of the brines and 3 samples from the Red Sea water) were sabkha (Shabel 2007). In addition, salt domes offer some chemically analyzed at the Geochemistry Lab, Saudi problems related to underground dissolution in the Jizan Geological Survey, following the procedures given by area, especially in the old city of Jizan. These include Clesceri et al. (1998). The chemical analyses were carried surface collapse, building failure, fractures, tilting, cracked out for the major cations Na?,K?,Ca2?, and Mg2? and the - 2- 2- - roads, undulating ground surface, tilting of posts and major anions HCO3 ,CO3 ,SO4 and Cl . Total dis- electricity poles or even damage of the old buildings and solved solids (TDS) were measured by sample evaporation infrastructure (Erol 1989; Al-Mhaidib 2002; Youssef et al. techniques. Calcium (Ca2?) and magnesium (Mg2?) are 2012; Youssef and Maerz 2013). Most studies carried out determined by compleximetric titration using standard on Jizan sabkha are related to the geotechnical properties of EDTA solution. Chloride (Cl-) is determined by titration - the sabkha soil and the problems related to construction on with standard (0.05 N) AgNO3. Bicarbonate ions (HCO3 ) the sabkha (Dhowian et al. 1987; Dhowian 1990; Erol are determined by titration with standard (0.1 N) HCl. 1989; Al-Shamrani and Dhowian 1997; Al-Mhaidib 2002; Sodium (Na?) and potassium (K?) are measured by flame 2- Shabel 2007; Youssef et al. 2012; Youssef and Maerz photometry. Sulfate ions (SO4 ) are determined colori- 2013). Erol and Dhowian (1988) found severe and wide- metrically using spectrophotometer technique. The ana- spread damage in the settlements of Jizan city, which is lytical precision of the ions is determined by calculating related to sinkholes and to linear depressions associated the absolute error in ionic balance in terms of equivalents with solution channels in the salt dome. The regional per milligram (meq/l), which is found in all samples within composition of the sediments in the Jizan sabkha is the a standard limit of ±5 %. All concentration values were interest of Al-Shamrani and Dhowian (1995, 1997), expressed in milligram per liter (mg/l) unless otherwise Youssef et al. (2012), and Youssef and Maerz (2013). indicated. The chemical data on the major cations and The objectives of the present paper are: (1) identification anions were displayed in graphical forms of the Trilinear of the evaporite composition and textures of the Piper and Sulin diagrams to delineate the composition and sabkha sediments, (2) understanding the hydrochemistry, origin of the brines in the sabkha. brine evolution and genesis of Jizan sabkha, and (3) understanding the effect of brine and evaporite minerals to building failure in Jizan sabkha. The results can be used to Previous studies interpret the chemistry and source of the brines, formation and textures of gypsum, anhydrite and halite in ancient In the Red Sea coastal plain of Saudi Arabia, most of the sabkha deposits. hydrochemical works are concerned with coastal pollution that resulted from sewage plants and other human inference (Turki 2007; Badr et al. 2009; Basaham et al. 2009). Some Materials and methods works are concerned also with the hydrochemistry of coastal and supratidal sabkhas in the Red Sea and The present paper is based on the results of 10 days of field Arabian Gulf coasts (e.g., Bahafzullah et al. 1993; Basyoni work and excavation of several shallow trenches down to 1997; Basyoni and Mousa 2009; Al-Shaibani 2013; Taj and the groundwater table (36–150 cm in depth) in the area of Aref 2015). Bahafzullah et al. (1993) classified the sabkha 123 Environ Earth Sci (2016) 75:105 Page 3 of 17 105

b a 13 Jizan

1 Duba NORTH

EGYPT SUDI ARABIA SAUDI ARABIA

Jeddah RED SEA 12 RED SUDAN SEA Jizan 11 10 0 250 km YEMEN

9 Quaternary surficial deposits

8 Pleistocene basalt

Mesozoic & Paleozoic sedimentary rocks 2 7 RED SEA Hijaz-Asir complex

6 Granite pluton Proterozoic rocks

5 4 3 Seawater sample Wet mudflat/sandflat Brine sample 0 3km Dry mudflat/sandflat 5 Sample number Miocene salt dome

Fig. 1 Surface sediments in Jizan sabkha and geologic setting of Jizan area. (a) Surface sediments and location of seawater and brine samples in Jizan sabkha, (b) Geology of Jizan area (After Blank et al. 1986) development around Sulaymaniya area into four to chloride type with neutral pH value …’’. Al-Harbi et al. stages; these are: (1) incipient; (2) slightly developed; (3) (2008) studied the hydrogeochemical processes and the moderately developed; and (4) well developed. They found isotopic characteristics of Al-Awshaziyah inland sabkha in that the salinities of the water samples in incipient and Al-Qaseem region, central Saudi Arabia, as well as the slightly developed sabkhas are very saline and slightly waters from shallow and deep wells. They compared the hypersaline waters, whereas the moderately to well-de- salinity, cations and anions concentrations, and found that veloped sabkhas are moderately to highly hypersaline. the water types of the sabkha are sodium-magnesium Basyoni (1997) found that the groundwater in Al-Lith chloride, magnesium-sodium-chloride and sodium-chlo- sabkha is moderately hypersaline and highly hypersaline, ride, and of meteoric origin. Alsaaran (2008) studied the whereas slightly hypersaline and very saline water exist brine chemistry of Jayb Uwayyid sabkha, eastern Saudi south of Al-Lith sabkha. He found positive correlations Arabia, and found that the average total dissolved solids in between TDS, and Na? and CI-. The TDS values, cations the sabkha brines is 243 %, and the order of cation dom- 2- ? 2? 2? ? and anions, except SO4 of the pore water decrease with inance is Na [ Mg [ Ca [ K , and the anion - 2- - depth. The pH values of the groundwater of Al Lith sabkha dominance is Cl [ SO4 [ HCO3 . He concluded that range from 6.8 to 7.9, in contrast to the 8.0–8.2 pH values sabkha brines have evolved from deep groundwater rather of the Red Sea water. Serhan and Sabtan (1999) measured a than from other near surface sources (i.e., direct rainfall, salinity range of 55–95 % in the groundwater in Al- runoff from the surroundings, or inflow of shallow Nekhaila sabkha, south Jeddah. This water has a high groundwater). Al-Dakheel et al. (2009) interpreted the content of sulfate and chloride that cause corrosive action major hydrodynamic process in Al Asfar Lake, Al Hassa on reinforced concrete. Banat et al. (2005) studied area, Saudi Arabia, as possibly due to the upward migration numerous water samples from coastal sabkhas between of subsurface brines from groundwater by capillary action Jeddah and Yanbu Al-Bahar, Red Sea coast. They assumed due to evaporation, that precipitate salt on the surface. that the climatic conditions over the Red Sea sabkhas lead Basyoni and Mousa (2009) interpreted the brines of Murayr to the formation of ‘‘ …marine brines of magnesium-sodic sabkha, Arabian Gulf as belonging to chloride type (MgCl2

123 105 Page 4 of 17 Environ Earth Sci (2016) 75:105

and CaCl2) that recharged mainly from seepage of recent marine water from the Gulf side and from marine and

, chloride meteoric waters reacted with the surrounding carbonates. 4 They assumed that the capillary rise of these waters from , chloride 4 the shallow water table to the surface is a consequence of surface evaporation that led to deposition of evaporite minerals in the sabkha. Hussein and Loni (2011) studied the Jizan thermal springs that flowed through fractures within the Precambrian- Cambrian Arabian Shield rocks. The thermal springs are characterized by having a lower - 2- - (Cl ? SO4 )/HCO3 ratio (0.38–0.56), higher ? ? 2? 2? - 2- (Na ? K )/(Ca ? Mg ) ratio ([4) and Cl [ SO4 . Al-Shaibani (2013) estimated the concentrations and total masses of magnesium, potassium, calcium, and sodium from 20 shallow wells in Jayb Uwayyid sabkha, eastern Saudi Arabia. His results showed that Jayb Uwayyid sab- kha contains about 1.4, 0.4, 0.9, and 9.9 million metric tons TDS PH Mg/Ca Brine type of magnesium, potassium, calcium and sodium, respec-

4 tively. In the south Jeddah area, Taj and Aref (2015) found PO that the supratidal saline pans increase in salinity from 80

2 to 140, and 220–375 % during deposition of gypsum and halite, respectively. The dominant cations and anions concentration order in the saline pans is Na? [ Mg2? [ - ? 2? - 2- - K [ Ca , and Cl [ SO4 [ HCO3 , respectively. FNO They indicated that the brines were derived mainly from

4 recent and old marine waters of MgCl2 and CaCl2 char-

NH acters, with minor contribution of meteoric water. - 2 4 Study area SO - 3 Geologic setting and location of Jizan sabkha HCO Three topographic zones exist in the Jizan area, which run for 1800 km parallel to each other in a northwest-southeast

- direction (Blank et al. 1986; Hussein and Loni 2011), these Cl are (Fig. 1b): (1) the dissected highland of Hijaz-Asir escarpment that forms a narrow belt of strongly eroded ?

K terrain of Precambrian basement complex; (2) the central plateau is a west-east gently sloping peneplain that pene- trated by west-east trending which drain the western ? highlands. It consists of the Cambro- Wajid Na Sandstone that rests unconformably on peneplain Precam-

a brian basement rocks and below rocks (Powers ? 1 2 et al. 1966); and (3) the Tihama, low-elevation and gently Mg sloping coastal plain that forms a strip of land that consists

? of the Quaternary eolian sands to alluvial terrace deposits. 2 A Miocene salt dome forms a prominent high land (\50 m) that intersects the monotonous flat coastal plain area. Recent moist, sabkha sediments are widespread near the epm 36.9epm 171.35 41.1 581.2 329.04 11.8 640.7 609.9 12.3 2.11 575.7 91.61 2.25 3.81 86.40 0.34 epm 33.9 164.52 531.0 9.5 557.6 2.05 83.28 2.46 Concentration values of the major cations and anions in the seawater of Jizan area shore of the Red Sea, whereas loess and sand exist in the dry land to the east of the coastal plain. The Jizan 3Maximum mg/lMinimum 824.0Average 824 4000.00 680 14727.5 4000 480.0 748 2000 20406.0 14727.5 2694.3 137.00 480 12,206 13431.1 4150.00 370 21619 437.5 6.15 19,466 137 20,497 1.95 125 130.3 0.06 4400 0.27 4183.3 4000 41,900 68.7 39.7 7.52 6.15 1.96 1.763 4.85 1.38 0.23 0.15 0.34 0.29 Ca, 0.06 Mg, sodium, chloride 41,900 40366.6 0.26 7.86 38,500 8.09 3.53 4.85 7.52 2.82 1 mg/l 680.0 2000.00 12206.0 370.0 19466.0 125.00 4000.00 44.40 1.96 0.23 0.34 38500 7.97 2.94 Mg, Ca, sodium, SO 2 mg/l 740.0 2083.00 13360.0 462.5 21619.0 129.00 4400.00 68.70 1.38 0.17 0.26 40,700 8.09 2.82 Mg, sodium, SO Location of samples is in Fig. Table 1 S. no. Unit Ca sabkha is present in- and around Jizan city at the 123 nio at c (06 515 ae5o 7105 17 of 5 Page (2016)75:105 Sci Earth Environ

Table 2 Concentration values of the major cations and anions in the brines of Jizan sabkha 2? 2? ? ? - - 2- S. Brine nature unit Ca Mg Na K Cl HCO3 SO4 NH4 FNO2 PO4 TDS PH Mg/ Brine type no. Ca

4 Water table; depth mg/l 3140.0 1633.00 3590.0 168.0 9527.0 87.00 2150.00 0.41 1.20 0.06 0.30 17,700 7.45 0.52 Ca, Mg, sodium, 36 cm epm 156.7 134.33 171.8 4.3 268.8 1.43 44.76 0.02 chloride 5 Halite pond mg/l 15500.0 10390.00 55800.0 2400.0 136981.0 113.00 1950.00 177.00 1.52 0.66 8.65 223,000 6.63 0.67 Mg, sodium, chloride epm 773.5 854.68 2427.3 61.4 3864.2 1.85 40.60 9.81 6 Water table; depth mg/l 4800.0 2340.00 4998.0 132.0 26548.0 69.00 2550.00 135.00 1.64 0.19 1.35 43,200 6.91 0.49 Mg, Na, calcium, 150 cm epm 239.5 192.49 217.4 3.4 748.9 1.13 53.09 7.48 chloride 7 Water table; depth mg/l 1332.0 830.00 2292.0 520.0 5367.0 137.00 3200.00 2.50 1.57 0.07 0.28 12,900 7.39 0.62 Ca, Mg, sodium 150 cm epm 66.5 68.28 99.7 13.3 151.4 2.25 66.62 0.14 chloride

8 Artificial mg/l 1024.0 8350.00 251700.0 11450.0 213023.0 117.00 8950.00 174.00 1.35 0.98 0.19 495,000 7.15 8.15 Mg, sodium, SO4, excavation epm 51.1 686.87 10949.0 292.9 6009.4 1.92 186.34 9.64 chloride

9 Water table; depth mg/l 16500.0 15500.00 87900.0 16050.0 226789.0 45.00 465.00 72.00 0.65 0.58 1.75 363,000 6.01 0.94 Ca, Mg, sodium, SO4, 120 cm epm 823.4 1275.03 3823.7 410.6 6397.7 0.74 9.68 3.99 chloride 10 Water table; depth mg/l 6550.0 5000.00 176650.0 617.5 47440.0 95.00 4100.00 117.00 0.77 0.26 1.08 67,400 6.99 0.76 Sodium, chloride 150 cm epm 326.8 411.30 7684.3 15.8 1338.3 1.56 85.36 6.48 11 Water table; depth mg/l 1112.0 8800.00 54300.0 1650.0 122748.0 189.00 8950.00 43.00 2.16 0.39 1.80 200,000 6.77 7.90 Ca, Na, magnesium 70 cm epm 55.5 723.89 2362.1 42.2 3462.7 3.10 186.34 2.38 chloride 12 Artificial mg/l 17100.0 15000.00 35280.0 1520.0 132160.0 95.00 2150.00 132.00 2.05 0.19 0.90 129,200 6.60 0.88 Mg, sodium chloride excavation epm 853.3 1233.90 1534.7 38.9 3728.2 1.56 44.76 7.31 13 Water table; depth mg/l 18100.0 15000.00 27720.0 1560.0 123660.0 86.00 4150.00 117.00 1.55 0.41 1.30 118,400 6.05 0.83 Sodium chloride 80 cm epm 903.2 1233.90 1208.8 39.9 3488.5 1.41 86.40 6.48 Maximum 18,100 15,500 251,700 16,050 226,789 189 8950 177 2.16 0.98 8.65 495,000 7.45 8.15 Minimum 1024 830 2292 132 5367 45 465 0.41 0.65 0.06 0.19 12,900 6.01 0.49 Average 8515.8 8284.3 70,023 3606.7 104,424 103.3 3861.5 96.99 1.45 0.38 1.76 166,980 6.795 2.176 Location of samples is in Fig. 1a 123 105 Page 6 of 17 Environ Earth Sci (2016) 75:105 southwestern sector of Saudi Arabia, between latitudes (2012) measured the highest point of the barchan dunes as 16°480 and 16°580N and longitudes 42°320and 42°380E about 4 m with a slope angle reaching 40°. The high slope (Fig. 1a). angle of the dunes may be related to the occurrence of efflorescent gypsum and/or halite cements between the Climate sand grains at/or near their sediment surface. Three areas are distinguished in the sabkha that vary in The Jizan area has a subtropical desert climate, where the composition and mechanism of formation of the several ephemeral systems drain to the Red Sea, such evaporite minerals, and the nature and depth of the brine as Jizan, al Khums, Mais, Bish and others (Abdelrahman that precipitates the evaporite minerals; these are the halite and Ahmad 1995). Jizan city is characterized by sparse rain pan, wet sabkha, and dry sabkha. Few, small halite pans storms which vary in intensity and duration. The southern (\25 m2 in diameter, and 20–50 cm deep) exist in the part of the city is sometimes exposed to the risk of flash lowest topographic depressions in the sabkha (Fig. 3a). floods due to the heavy rain intensity, and the wadis flow They are filled with high salinity brine ([250 %, and from the east towards west (Elsebaie et al. 2013). Abdel- density 1.26 g/cm3). Halite crystallizes in these pans at the rahman (1997) reported that the average temperature in brine surface as thin rafts and pyramidal hoppers, and on Jizan area is 23 °C, the annual precipitation is 1.3 cm, and the floor of the pan as aggregates of chevrons and cornets the average relative humidity varies between 45 and 65 % (Fig. 3b). The wet sabkha is represented by wet mudflat in winter, and 25 and 40 % in summer. The mean rate of and sandflat areas, where the water table ranges from 36 to evaporation at Jizan was estimated as 156 cm/year by 150 cm below the surface (Fig. 3c). The sabkha sediments Abdelrahman and Ahmad (1995), and 128.72 cm/year by are composed mainly of moist, loose sand and silt that form Al-Subhi (2012). The prevailing winds at Jizan blow from adhesion ripples, in addition to a variable abundance of the west during summer and southwest during winter, with gypsum, anhydrite and halite minerals (Basyoni and Aref, wind speeds ranging between 2 and 50 km/h. Elsebaie 2015). The surface of the wet sabkha is composed of et al. (2013), in their study on the of Jizan city, buckling petee crusts (Fig. 3d). The petee structure is stated that the average surface temperature of the Red Sea composed of black and green microbial mats and gypsum water in Jizan area ranges between 26 °C in winter and layers that form elongated, hollow, twisted ridges (Fig. 3d). 32 °C in summer. The seawater at the southern part of the The dry sabkha is composed of \1 cm thick halite crusts Jizan area has a lower salinity (36–37 %) than the northern that form inverted, V-shaped, polygonal tepee structures part (37–38.5 %). (Fig. 3e). The subsurface sediments in all sabkha areas are composed of interbedded brown, sand and grey, mud lay- ers. Scattered lenticular and rosette gypsum crystals Sediment characteristics of the sabkha area (Fig. 3f) are aggregated and form thin layers at the depths of 10, 40 and 90 (Fig. 3c). Nodular mosaic and enterolithic The coastal plain of Jizan area extends approximately folds of milky white, soft anhydrite are recorded at the 10 km inland to the foothills of the Red Sea escarpment, depth of 15 cm (Fig. 3g). and is covered by Quaternary eolian sand, alluvial sand and gravel, loess and flood plain silt deposits. The prominent elevated relief on the coastal plain is a salt dome at Jizan city (Fig. 1a). The recent sediments are represented by sabkha deposits on the wet, coastal plain of Jizan area, in addition to sand dunes and loess deposits in the dry land. The old city of Jizan is situated at an elevated terrain, 5–50 m (above sea level) underlain by the Miocene salt dome covering an area of 4 km2. The salt dome is covered by cap rocks of brecciated gypsum, anhydrite, dolomite, shale and sandstone layers. Several dissolution sinkholes of a diameter\4 m and depth exceeding 6 m are observed on the floor of the abandoned salt quarries (Fig. 2). Loess sediment is distributed over the eastern side of Jizan city. Loess form small hills, \5 m in height, and is composed of well-sorted, silt to fine sand-sized quartz, feldspar, and mica grains. Sand dunes (barchan) and sand sheets form Fig. 2 A funnel-shaped sinkhole forms due to recent dissolution of most of the eastern part of the coastal plain. Youssef et al. halite and its partial filling with clastic sediments 123 Environ Earth Sci (2016) 75:105 Page 7 of 17 105

ab

c d

e

f g

Fig. 3 Evaporite deposition in the sabkha area. (a) Shallow, desic- V-shaped, polygonal ridges (\5 cm in height) of tepee halite crusts, cated pan encrusted with white halite rafts and skeletal crystals. partially covered with eolian sand. (f) Aggregates of lenticular and (b) Bedding plane view showing the variable size of halite cubes that rosette gypsum grow inclusively in brownish silt. (g) Milky white form the rafts. (c) A general sand mud layering, with gypsum anhydrite nodules grow displacively at a certain level in the wet sand crystallization at several levels (arrows). (d) Elongated, wavy, ridges of the sabkha with smooth upper surface form the petee structure. (e) Inverted,

123 105 Page 8 of 17 Environ Earth Sci (2016) 75:105

Results and discussion from 12,206 to 14,727 mg/l, with the average of 13,431.1 mg/l (Table 1). The dominant anion in the brines Chemical composition of seawater and the brines of Jizan sabkha is Cl- where its concentration ranges from 5367 to 226,789 mg/l, and the average is 104,424 mg/l, The distribution of the concentrations of the cations Na?, which accounts for more than 50 % of the charge balance ? 2? 2? - 2- - ? K ,Ca and Mg , the anions Cl ,SO4 , and HCO3 , in the brines. The dominant cation is Na , where its con- NH4, TDS and pH are presented in Figs. 4 and 5. The centration ranges from 2292 to 251,700 mg/l, with the statistical parameters, such as maximum, minimum and average concentration value of 70,023 mg/l. Such con- mean of the chemical composition of the brines in Jizan centrations of Cl- and Na? in the brines of Jizan sabkha sabkha are also presented in Tables 1 and 2. Generally, the are several times higher than their concentration in sea- concentrations of cations and anions in the seawater are water of Jizan area. They are also slightly higher than the lower than the concentration values of the sabkha brines in average concentration values of chloride (96,851 mg/l) and most samples, except samples Nos. 4 and 7 (Fig. 4), which sodium (45,239 mg/l), measured in the groundwater of have also lower salinity values due to recharge from rain Dahaban sabkha by Banat et al. (2005). water, temporary floods and seepage of sewage water from The Ca2? concentration in seawater of Jizan area ranges septic tanks. Na? has the highest concentration with from 680 to 824 mg/l, with the average of 748 mg/l, and respect to the cations K?,Mg2? and Ca2? in the brines of the Mg2? concentration ranges from 2000 to 4000 mg/l, the sabkha (Fig. 4a). Mg2? concentration is next in abun- with the average of 2694 mg/l (Table 1). In the brines of dance, followed by Ca2? in most samples, whereas K? Jizan sabkha, the Ca2? concentration ranges from 1024 to concentration value is the lowest, except in samples Nos. 18,100 mg/l, with the average of 8516 mg/l, and the Mg2? 12 and 13 (Fig. 4a). For the anions, the Cl- concentration concentration ranges from 830 to 15,500 mg/l, with the 2- is the highest among all samples, SO4 concentration is average of 8248 mg/l (Table 2). The average concentra- - 2? 2? very low, whereas the HCO3 is the lowest (Fig. 4b). tions of Ca and Mg in the brines of Jizan sabkha The Cl- concentration in the seawater of Jizan area greatly exceed the values measured from the seawater of ranges from 19,466 to 21,619 mg/l, with an average value Jizan area. They are also higher than the average concen- of 20,497 mg/l, whereas the Na? concentration ranges trations of Ca2? (2832 mg/l) and Mg2? (4314 mg/l),

a b

Seawater Brine sample Seawater Brine sample

c d pH

Seawater Seawater Brine sample Brine sample

2? 2? ? ? - 2- 2- Fig. 4 Histograms representing the concentration of the cations (Ca ,Mg ,Na and K ), anions (Cl , HCO3 and SO4 ) and TDS, and pH values in seawater and brine samples of Jizan sabkha 123 Environ Earth Sci (2016) 75:105 Page 9 of 17 105 measured by Banat et al. (2005) for Dahaban sabkha, north health problems that may arise from either deficiency or Jeddah. excess amount (Gopal and Gosh 1985). Fluoride can be K? ions have a narrow range of 370–480 mg/l in sea- considered as one of the main trace element in ground- water of Jizan area, with the average of 437 mg/l (Table 1). water, where it occurs generally as natural constituent (Al- The concentration of K? in the brines of Jizan sabkha Ahmadi 2013). The high concentrations of fluoride are ranges from 132 to 16,050 mg/l, with the average of generally due to rocks containing fluoride minerals (Wen- 3607 mg/l (Table 2). The K? values in the brines exceed zel and Blum 1992; Bardsen et al. 1996). 3- the values in Jizan seawater, and the average value of The concentration of phosphate (PO4 ) in the brines of 1911 mg/l in the groundwater of Dahaban sabkha mea- Jizan sabkha ranges from 0.19 to 8.65 mg/l, with a mean sured by Banat et al. (2005). value of 1.76 mg/l. The phosphate is usually found in 2- The SO4 concentration in seawater of the Jizan area groundwater with a minimal level due to the low solubility ranges from 4000 to 4400 mg/l, with the average of of native phosphate minerals and the ability of soil to retain 2- 4183 mg/l (Table 1). The SO4 concentration in the bri- phosphate (Rajmohan and Elango 2005). nes of Jizan sabkha ranges from 465 to 8950 mg/l, with the Total dissolved solids (TDS) in the seawater of Jizan 2- average of 3861 mg/l (Table 2). The average SO4 con- area range from 38,500 to 41,900 mg/l, with the average of centration in seawater and brines of Jizan area are similar. 40,366 mg/l (Table 1). The TDS in the brines of Jizan They are also similar to the average concentration value of sabkha range from 12,900 to 495,000 mg/l, with the 3819 mg/l in the Dahaban sabkha, measured by Banat et al. average of 166,980 mg/l (Table 2; Fig. 4c). The TDS 2- (2005). However, seven brine samples have SO4 con- values of seawater in Jizan area are nearly similar to TDS centration less than the average in Jizan seawater, indi- value that generally recorded for the Red Sea water. Two 2- cating the removal of SO4 due to gypsum precipitation brine samples from trenches in Jizan sabkha have a lower 2- and/or the reduction of SO4 ions by sulfate-reducing TDS value of 17,700 and 12,900 mg/l in samples 4 and 7, bacteria, similar to observations by Deng et al. (2010), than the average TDS in seawater of Jizan area. The brines Spadafora et al. (2010), and Glunk et al. (2011). of these samples may be derived from a mix with rain- - HCO3 ions have low concentration in seawater of the water, groundwater of meteoric origin or seepage of sew- Jizan area, as well as in the brines of Jizan sabkha age water from septic tanks. For the brines of Jizan sabkha - (Tables 1, 2). The HCO3 concentration in seawater of that have higher TDS values than the average TDS of Jizan area ranges from 125 to 137 mg/l, with the average of seawater (40,366 mg/l), are likely related to extensive - 130 mg/l, whereas the HCO3 concentration in the brines evaporation rate with respect to the small groundwater of Jizan sabkha ranges from 45 to 189 mg/l, with the inflow, rainfall or seawater seepage. The very high salinity - average of 103 mg/l. The average HCO3 concentration in values of 495,000 and 363,000 mg/l (Table 2) of the sab- Dahban sabkha is 204 mg/l (Banat et al. 2005), which is kha brines may be related to dissolution of halite in the salt slightly higher than the average values measured for the dome. Red Sea water and sabkha water in Jizan area. The low The values of electrical conductivity (EC) range from - concentration values of HCO3 in seawater and brines in 20,000 to 199,100 lS/cm with a mean value of 99,800 lS/ Jizan sabkha are due to their removal during precipitation cm. The high values in EC are attributed mainly to evap- of the carbonate minerals. oration process and increase in the salinity of the brine.

The concentrations of ammonia (NH4) in the brines of Both TDS and EC are affected by the high concentration ? 2? 2? - 2- Jizan sabkha and seawater range from 0.41 to 177, and values of Na ,Ca ,Mg ,Cl , and SO4 . 6.15–68.7 mg/l, respectively, and their mean values are The pH values in the seawater of Jizan area range from 96.99 mg/l and 39.7, respectively. The concentration of 7.52 to 8.09, with the average of 7.86 (Table 1). The pH nitrite (NO2) ranges from 0.06 to 0.98 mg/l, and the mean values in the brine samples of Jizan sabkha range from 6.01 value is 0.38 mg/l in the brines of Jizan sabkha. The high to 7.45, with the average of 6.79 (Table 2), which are lower values of NH4 and NO2 may be due to leakage from septic than the values recorded from the Red Sea water in Jizan tanks of the houses in Jizan city, or from fertilizers in area (Fig. 4d). Six brine samples have values slightly \7, nearby agriculture fields. It is worth to mention that during which indicate neutral or slightly acidic brines. Whereas, excavation of the lands for the foundations of new houses, four samples have values more than 7, indicating that all - high quantities of groundwater having a bad odor have carbonate alkalinity is in the form of HCO3 (Stumm and seeped from nearby old houses. This water may provide the Morgan 1996; Drever 1998). elevated NH4 and NO2 in the brine of Jizan sabkha. An isochronal map of the cations in the brines of Jizan The concentration of fluoride (F-) in the brine of Jizan sabkha indicates that Na? increases to [250,000 mg/l in sabkha ranges from 0.65 to 2.16 mg/l, with a mean value of the halite pans at central western margin of the sabkha area, 1.45 mg/l. Fluoride is considered as an essential element in while low values of Na? (\10,000 mg/l) dominate the 123 105 Page 10 of 17 Environ Earth Sci (2016) 75:105

Na K

Ca Mg

123 Environ Earth Sci (2016) 75:105 Page 11 of 17 105 b 2? 2? 2- Fig. 5 Contour lines representing the distribution of the major cations Ca and Mg and the major anion SO4 cations and anions in seawater and brine samples of the studied (Tables 1, 2). Three samples have Ca2?,Mg2?, sodium sabkha, Jizan area chloride brine type, two samples have the following brine 2? 2- 2? types Mg , sodium, SO4 , chloride, or Mg , sodium chloride, and only one sample has the following brine types ? 2? 2? 2- 2? ? eastern margin of the sabkha (Fig. 5). K values follow Mg ,Ca , sodium, SO4 , chloride, or Mg ,Na, ? 2? 2? 2- Na , where the highest value is 16,000 mg/l in the central calcium chloride, or Ca ,Mg , sodium, SO4 , chloride, western part of the studied sabkha, and the K? concen- or Ca2?,Na?, magnesium chloride (Tables 1, 2). tration decreases to values less than 2000 mg/l in the north, Despite the dominance of Na? and Cl- ions in most of east and southeastern sides (Fig. 5). The low values of Na? the studied brine samples that exhibited a marine-like and K? concentrations at the eastern margin of the sabkha chemical character (Herczeg et al. 2001), a broad range of is attributed to dilution from the landward side of the secondary processes can significantly affect the evapora- sabkha, less evaporation and lower salinity (up to tive pathways and are responsible for the variables brine 12,900 mg/l) compared to the western margin of the sab- types in the Jizan sabkha, similar to the interpretation kha area. The Ca2? concentration value is the reverse of the proposed by Radke et al. (2002). The secondary processes concentration of Na? and K?.Ca2? concentration is lower may include mineral dissolution, cation exchange reac- at the southwestern part of the sabkha (\1000 mg/l), and tions, sulfate reduction, brine mixing, brine reflux, mineral increases to 2200 mg/l to the northeastern side of the precipitation and recycling of soluble salts within the sabkha (Fig. 5). The Mg2? concentration increases from sabkha. 1500 mg/l in the southeastern part of the sabkha to [10,000 mg/l in the central western part of the sabkha, Ion inter-relationship and then increases gradually to 15,000 mg/l in the northern part of the sabkha (Fig. 5). The isochronal map of the The correlations of the concentration of cations, anions, anions showed that the concentration of Cl- is similar to TDS and pH are shown in Fig. 6. The correlation between Na?, where the highest value of [200,000 mg/l is recorded Na? and Cl- for most samples (except samples 9 and 11 in the central western margin of the sabkha, and decreases which have very high Na? values) indicates a positive 2- - 2 to the east and north sides (Fig. 5). The SO4 and HCO3 correlation (R = 0.9017) (Fig. 6a). This positive correla- concentrations are similar, and they increase to the western tion indicates the enrichment of the brines with NaCl margin of the sabkha, to values of 9000 and 180 mg/l, (halite) that may be precipitated at high salinity. The cor- 2- 2? 2? respectively (Fig. 5). The concentrations of SO4 and relation between Ca and Mg (Fig. 6b) also indicates a - 2 HCO3 decrease to the northeastern side of the sabkha to positive correlation (R = 0.7237). This is contrary to the 2? 180 and 45 mg/l, respectively. The concentration of NH4 fact that the brine should have lower Ca concentration shows a narrow range, but it generally increases to the west due to the earlier precipitation of CaCO3 (calcite and/or and north margins of the sabkha (Fig. 5). High concen- aragonite) and CaSO4.2H2O (gypsum). Most probably, the 2? tration of NH4 and NO2 in Jizan sabkha may indicate relatively high Ca concentration is due to dissolution of intrusion into the sabkha water from adjacent sewage carbonate grains in the sediments. No pronounced corre- 2? 2- 2 waters and agricultural areas which receive excess nitrogen lation exists between Ca and SO4 (R = 0.2827) fertilizers (such as urea and ammonium nitrate) that are (Fig. 6c). This is due to the possible precipitation of

assumed to increase the agricultural production. CaSO4.2H2O (gypsum) from the brine and dissolution of 2? - carbonate grains. No correlation between Ca and HCO3 Brine types (R2 = 0.3519) (Fig. 6d) in two groups of the brines, may be interpreted as a result of oxidation of organic matter in The ionic concentrations of the seawater and brines in the sediments and reduction of sulfate ions, which lead to - samples numbers 3, 4, 6, 7, 8, 9, 11 and 13 (Tables 1, 2) the increase in HCO3 . There are strong positive relations have the following general pattern: Na? [ Mg2? [ between TDS and Na? (R2 = 0.8653) (Fig. 6e), and Ca2? [ K?. Some samples, however, (2, 12 and 13) have between TDS and Cl- (R2 = 0.8903) (Fig. 6f), and no ? 2? ? 2? 2- the abundance Na [ Mg [ K [ Ca , and three pronounced relation between TDS and SO4 samples have variable abundances such as Na? [ (R2 = 0.1163) (Fig. 6g). The positive relations indicate Ca2? [ Mg2? [ K?,orCa2? [ Na? [ Mg2? [ K?,or that the TDS is mainly represented by Na? and Cl- ions, 2? ? 2? ? 2- Mg [ Na [ Ca [ K (Tables 1, 2). On the other whereas changes in SO4 does not affect the TDS of the hand, the abundance of the major anions in all samples is brine. Plotting of the values of TDS and pH indicates no - 2- - 2 Cl [ SO4 [ HCO3 . The brine type for most samples relation between them (R = 0.1869) (Fig. 6h). The pH is sodium chloride, with variable proportions of the major values of seawater are around 8 that decrease to about 6 123 105 Page 12 of 17 Environ Earth Sci (2016) 75:105

Cl SO4

HCO3 NH4

Fig. 5 continued 123 Environ Earth Sci (2016) 75:105 Page 13 of 17 105

2 a R2 = 0.9017 b R = 0.7237

c R2 = 0.2827 d R2 = 0.3519

e R2 = 0.8653 f R2 = 0.8903

2 g R = 0.1163 h R2 = 0.1869

Fig. 6 Scatter diagrams showing the correlations between various anions, cations, TDS and pH values with the increases in the salinity of the brine. This result is high values of 8.15 and 7.90, respectively (Fig. 7). The low in agreement with the data of Ba˛bel and Schreiber (2014). Mg2?/Ca2? ratio in most brine samples is most probably The Mg2?/Ca2? ratio of seawater at Jizan area ranges due to the dissolution of carbonate grains in the sediments from 2.82 to 4.85, with the average of 3.53 (Table 1; that increases the concentration of Ca2? ions. Whereas the Fig. 7a). Whereas for the Jizan sabkha, the Mg2?/Ca2? high Mg2?/Ca2? ratio in samples 8 and 11 is due to the ratio of the brines range from 0.49 to 8.15, with the average removal of Ca2? ions through precipitation of calcite and of 2.176 (Table 2; Fig. 7a). All brine samples have lower gypsum. However, the dominant low Mg2?/Ca2? ratio Mg2?/Ca2? ratio than that measured in Jizan seawater, indicates that the brine has a low potential to dolomitize the except samples numbers 8 and 11, which have exceedingly high Mg-calcite and aragonite minerals. Only the brines in

123 105 Page 14 of 17 Environ Earth Sci (2016) 75:105

the precipitation of calcite, aragonite and gypsum. The chemical characters (ionic concentration patterns and brine types) of the studied brine samples in Jizan sabkha and seawater are similar, which indicate that the brine chem- istry of Jizan sabkha has been modified from initial sea- water composition to the stages of deposition of calcium carbonate, followed by calcium sulfate and finally to sodium chloride dominant composition (Fig. 8).

Genesis of the brines

Results of the chemical analyses were recalculated for both the major cations and major anions and plotted on a Sulin graph (Fig. 9) to interpret the origin of brine of Jizan sabkha. It is clear that the seawater samples and four brine samples of Jizan sabkha are located in the field of recent

marine water origin and of MgCl2 composition (Fig. 9). However, most of the brine samples in Jizan sabkha are

located in the field of old marine water origin and of CaCl2 composition (Fig. 9). Therefore, the main supply to the brines of Jizan sabkha is through seawater seepage that may be modified with reaction with the old marine water from dissolution of the halite crystals of the Miocene salt dome. This modified seawater is the source of the brines in Jizan sabkha. The localized formation of sinkholes at the floor of the abandoned salt quarries (Fig. 2) and collapse of the buildings of the old Jizan city point to an additional salt Fig. 7 Relationship between Mg/Ca and sample number, and TDS dissolution by rain water and fresh and/or sewage waters from houses. The possible contribution of fresh water samples 8 and 11 could dolomitize the carbonate grains in through Wadi Jizan or occasional rainfall has a minor the sediments due to their high Mg2?/Ca2? ratio. Banat effect on those samples that are located close to the field of et al. (2005) found that the increases in the Mg?2/Cl- meteoric water origin in Sulin graph (Fig. 9). Bagheri et al. 2- concentration and decreases in SO4 concentration lead to (2014) mentioned three main potential processes that may the formation of protodolomite in the coastal sabkha sed- cause high salinity values in the Kangan gasfield, these are iments between Jeddah and Yanbu Al-Bahar. halite dissolution, membrane filtration, and evaporation of water. They indicated that the evaporated ancient seawater Brine evolution trapped in lagoonal and sabkha carbonates, gypsum, and clastic rocks is the cause of salinization based on the The hydrochemical evolution of the brines of Jizan sabkha concentrations of Cl, Na, and TDS in comparison with Br can be understood using the analytical data obtained from concentration. brine samples as a result of plotting the major cations and anions in the Piper Trilinear diagrams (Fig. 8). The dia- Environmental impact of the sabkha brines grams show that all brine samples in Jizan sabkha have and minerals similar affinity and composition, which are similar to the composition of seawater. The diagrams show two groups of Sabkha evaporite brines and minerals cause severe damage samples, the first group shows that the majority of the brine to buildings and infrastructure in Jizan area. In addition, samples of Jizan sabkha fall in the field NaCl type of water. partial dissolution of the nearby salt dome can modify the The second group shows approximately equal percentage composition of the brines which increases their corrosive of the alkali metals (Na? ? K?), and the alkaline earth effect on steel reinforcement and deterioration of the elements Mg2? and Ca2?, whereas the strong acid (Cl-) concrete in the sabkha area. The evaporite minerals gyp- - 2- greatly exceeds the weak acid (HCO3 and CO3 ), and sum and anhydrite are common in the wet sabkha area. 2- the strong acid (SO4 ) (Fig. 8). Also, from the Piper plot, They are recorded with a variable abundance in the cap- the deficiency of Ca2? in the brines of the sabkha is due to illary evaporation zone of both shallow (36 cm) and deep 123 Environ Earth Sci (2016) 75:105 Page 15 of 17 105

Fig. 8 Piper Trilinear diagrams showing the brine evolution in Jizan sabkha Brine salinity

< 40 g/l 40 – 80 g/l 80 – 220 g/l 220 - 350 g/l > 350 g/l

Fig. 9 Sulin graph showing the 100 origin and type of the brines, 90 CaCl 2 rCl- – r(K+ + Na+) Old Marine Water > 1 Jizan sabkha 80 2-

) rMg + 70 + Na

+ 60 = 1 50

+ + –r(K r(K + Na ) -

= 1 rCl 40 < 1 rCl- 30 MgCl2 Recent Marine Water 2- 20 r SO4 10 100 90 80 70 60 50 40 30 20 10

10 20 30 40 50 60 70 80 90 100 10 r Mg2+ NaSO4 20 Deep Meteoric Water 30 - r(K+ + Na+) – rCl- 40

2- < 1 rSO 50 ) – rCl

4 + 60 + Na

= 1 NaHCO + 3 70

Shallow Meteoric Water r(K Seawater from tidal flat & area > 1 80 90 Brine sample from the water table of the sabkha 100

(150 cm) groundwater. In this area halite is only recorded displacive nodules near the sediment surface. Both gypsum in saline pans within the sabkha area. These evaporite and anhydrite form from brines with salinity \200 %, but minerals reflect the salinity and chemical characteristics of halite is recorded as rafts, chevrons and cornets in those the brines. Gypsum is displacively grown as lenticular and pans with salinity exceeding 250 %. The crystallization rosette crystals in the subsurface sediments of the sabkha pressure exerted from displacive growth of gypsum and down to the underlying water table. Anhydrite forms anhydrite in pore spaces of the foundations causes their

123 105 Page 16 of 17 Environ Earth Sci (2016) 75:105 sever damage. The sulfate nature of the brines causes improved the manuscript. Thanks also to Mr. Murad Rajab and Mr. corrosion of the steel reinforcement of infrastructure. Ali Khofani for their field assistance. Fluctuation of the water table during summer and winter Compliance with ethical standards months increases the degree of damage and corrosion in the foundation in the sabkha area. Funding This project was funded by the Deanship of Scientific Research (DSR), King Abdulaziz University, Jeddah, Saudi Arabia, under Grant No. (307/145/1432).

Conclusions Conflict of interest The authors declare that they have no conflict of interest. The concentrations of cations and anions in most of the sabkha brines exceed their respective values within seawater due to intensive evaporation. However, two brine samples References have a lower salinity value and a lower concentration of cations and anions than seawater, and these may be related to Abdelrahman SM (1997) Seasonal fluctuations of mean sea level at Jizan, Red Sea. J Coast Res 13(4):1166–1172 the mixing of groundwater with meteoric water, leakage Abdelrahman SM, Ahmad F (1995) Red Sea surface heat fluxes and water from septic tanks in Jizan city, or from fertilizers in advective heat transport through Bab El-Mandab. J King Abdu- nearby agriculture fields. 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The composition and Red Sea based on the AVHRR sea surface temperature data. texture of the evaporite minerals in the sabkha area, and the J King Abdulaziz Univ Mar Sci 23(1):77–89 brine composition and origin can be used to interpret similar Ba˛bel M, Schreiber BC (2014) Geochemistry of and evolution of seawater, In: Holland H, Turekian K (eds) sabkha sediments in the rock record. Sediments, and sedimentary rocks, vol. 9, Treatise on geochemistry, 2nd edn. pp 483–560 Acknowledgments This project was funded by the Deanship of Badr NBE, El-Fiky AA, Mostafa AR, Al-Mur BA (2009) Metal Scientific Research (DSR), King Abdulaziz University, Jeddah, under pollution records in core sediments of some Red Sea coastal grant No. (307/145/1432). The authors, therefore, acknowledge with areas, Kingdom of Saudi Arabia. Environ Monit Assess thanks DSR technical and financial support. We thank the reviewers 155:509–526 B. Charlotte Schreiber, an anonymous reviewer, and the Editor-in- Bagheri R, Nadri A, Raeisi E, Kazemi GA, Eggenkamp HGM, Chief Olaf Kolditz for their helpful comments which greatly Montaseri A (2014) Origin of brine in the Kangan gasfield:

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