Contribution Of Hydrogeochemical And Statistic Tools To The Acquisition Of Water Quality In The North-Eastern Of Algeria: Annaba-El Tarf

doi:10.21203/rs.3.rs-2602678/v1

This work was conducted on 34 samples spread over 4 areas (Bouteldja, El Tarf, Les Salines et Barrahal) tapping the shallow and deep aquifer of groundwater in the North-eastern Algeria (Annaba-El Tarf), one sampling campaign was conducted in 2017 to describe the chemistry of the water and its interaction with the rock. The interpretation of the geological-geophysical and hydrogeological data allowed us to highlight two principal aquifers. The first consists of the sandy clay formations up to 18 m thick. It is generally free except at a few points where it is captive under clay levels. The second is more important localized in the gravel layer below first aquifer; it covers the entire study area. It is formed by Plio-Quaternary gravels, sands and pebbles and is contained in the collapse basin. The methodology used for the processing of the analysis results is based on multivariate statistical methods and characteristic ratios coupled with hydrochemical methods, as well as the calculation of saturation indices. The results show that the water quality is controlled both by the dissolution of the minerals of the evaporite formations and those of the carbonate formations, alteration of silicates and marine invasion.

groundwater

hydro geochemical characteristics

dissolution of the minerals

statistical characteristics

Annaba-El Tarf region

Groundwater is one of the most valuable natural resources, playing a fundamental role in human health and wellness, socio- economic development, and ecosystem functioning. Moreover, it is widelyused for various domestic, industrial, and irrigation activities (Derradji 2004; Djabri 2004).

Groundwater quality is based on the behavior of physical and chemical parameters that are influenced by geological formations, atmospheric precipitation, inland surface water, and geochemical processes as they are in contact with the rock and the various anthropogenic activities (Saravanan et al. 2015).

Groundwater is an important source of fresh water for domestic, agricultural and industrial uses in Algeria, especially in North Algeria and North-eastern Algeria, where surface water are little used, a fairly limited quantity is mobilized by dams (Chaffia, Mexa), lakes and some hill reservoirs and the rest flows towards the sea (Derradji and Saadali 2021) .

Water chemistry provides valuable information to determine the origin, transit time, flow patterns and water regimes, geological structure, and mineralogy of aquifers, as well as hydrogeochemical processes. Specific water quality is required to meet both domestic and irrigation needs. Their monitoring and evaluation are essential to design preventive measures on human health, animal life, and vegetation (Salcedo et al. 2017).

Statistical analyses, a Piper diagram, the saturation index and the correlations of chemical parameters were used to reveal the hydrogeochemistry and hydrogeochemical evolution of shallow groundwater in the north-eastern Algeria (Annaba-El Tarf). This effect has been widely studied (Bounab et al. 2017;Bounab et al. 2022).

The objective of this research was to carry out a geochemical study of the groundwater used as drinking water in Annaba El Taref region, by analyzing physicochemical parameters, major ions, together with chemical speciation, hydrogeochemical relationships. The study will be extremely important and useful in regional groundwater protection and management.

Location Of The Study Area:

The study region is located in the North-East of Algeria; it is included in 02 Wilayas Annaba and El Taref, distributed respectively over areas of 2998 km ², 1412 km ². It is limited to the North, by the Mediterranean Sea, to the South by the wilayas of Guelma-Souk Ahras, to the East by the Algerian-Tunisian borders and to the West by the wilaya of Skikda (Fig. 1). a relatively dense population of the order of 555,485 inhabitants concerning the wilaya of Annaba and of the order of 401,716 inhabitants that of the wilaya of El Tarf, concentrated especially in the agglomerations of Annaba city, El Hadjar, Sidi Amar, and El Bouni ... etc., And El-Tarf, Besbes, Dréan ... etc.

for the wilaya of El Tarf. The distribution of the population is mainly concentrated near industrial and agricultural activities : Sider complex, Asmidal, Naftal, Bounamoussa and Seybouse plains (Saou 2013).

The study region is one of the wettest regions of Algeria. It is subject to a Mediterranean climate, mild and humid in winter and hot and dry in summer. The annual average rainfall varies between 608.49mm and 832.18mm under an annual average temperature of around 17.15 ° C. The mean evaporation of the area is 1774.25 mm or 65% of rainfall. Runoff and infiltration are respectively an average of 130.10 mm / year and 127.3 mm / year. This coastal region is fully integrated into the large Mediterranean area, which characterizes its climate, its type of relief and its vegetation (Joleaud 1936).

Geological And Hydrogeological Settings

The geology of the study area was investigated by several authors (Gaud 1975; Bousnoubra et al. 2002; Villa 1980; Lahondére 1987). The plains of the Annaba-Bouteldja region is part of the geological complex of the Tell Algerian Nord Oriental ( l'Edough massif), presents metamorphic rocks in borders (gneiss, schists, micaschists, marbles, and metamorphic limestone), which constitute areas of feeds for groundwater of alluvial sediments potentially aquiferous of Mio-Plio-quaternary that form the major part of the plain. The existence of two pits separated by a shoal which carries the Daroussa hillock, namely the Ben-Ahmed pit, oriented S-N and that of Ben-M’hidi, oriented SW-NE. The filling of the pits comprises several aquifer horizons, from lenticular to continuous over the entire extent of the plains of Annaba and El Taref (Kherici and Messadi 1992).

The hydrogeologic and hydrodynamic studys allows distinguishing two different aquifers, with unequal quantitative and qualitative importance regarding the extent. The one superficial (free); consisting of fine sand and gravel with a thickness of 10 to 15 meters. It includes, in the constitution of its substratum, sand lenses, compact gray clays. These lenses are more common near the Seybouse wadi and on the outskirts of the Numidian sandstone outcrops. The other deep; semi-captive becomes captive in the West, has a depth which varies from 12 to 80 meters (Fig. 2).It is formed by Plio-Quaternary gravels, sands and pebbles and is contained in the collapse basin. The roof of the gravel layer has variable characteristics from permeable to impermeable; it is formed of clayey sands, sandy clays or clays [15]. These aquifers are widely exploited by numerous catchments to meet the needs of drinking water supply, industry and agriculture (Rodier 1989).

Sampling And Analytical Methods

Groundwater samples were collected for geochemical analysis at different depths from 40 production wells tapping the shallow aquifers during May 2016 (Fig. 1). Electrical conductivity and pH were measured in situ using a multiparameter WTW set (Multiline P3 PH/LF SET). At the same time, samples of nonacidified water were taken in 1.5 dm³ polyethylene bottles and stored in darkness at 4°C. Chemical analyses were undertaken at the laboratory of the Algerian Water Company Annaba (SEATA). The bicarbonates and carbonates were measured immediately after sampling by titration with the methyl orange endpoint; the concentration of chloride was determined by titration and precipitation of AgCl until silver chromate appears (Mohr’s method); sulphate was determined by the nephelometric method; and nitrate, were analysed by the colorimetric method. Calcium and magnesium were determined by complex metric titration, and emission spectrometry was used to determine the concentration of sodium and potassium (Parkhurst and Appelo 1999).

After physiochemical analysis, the accuracy of the analysis results was checked via charge balance. Generally speaking, the relative error should be within ±5%,

The results suggest that the maximum relative error is 4.56%, which is within the acceptable error limit. The analysis results are accurate and can be used for the study.

The identification of water facies was carried out by the software «Diagrams» by projecting the points directly on the diagram of piper. A statistical analysis of the data was performed starting with a descriptive statistic of the measured parameters, ending with a multiple correlation by a principal component analysis (PCA).

The saturation index (SI) is a widely used indicator in hydrogeochemical studies. The geochemical program PHREEQC was used to compute the saturation index (SI) of certain major minerals (Gibbs 1970; Li et al.2010; Parkhurst and Appelo 1999), including calcite, dolomite, fluorite and gypsum.

When SI = 0, the minerals in the aqueous solution are in equilibrium. When:

SI < 0, the minerals in the aqueous solution are unsaturated and follow a dissolution trend, and when SI > 0, the supersaturated status of minerals in the aqueous solution causes deposition to occur (Barna 2008).

The saturation index (SI) is defined as:

Where IAP is the relevant ion activity product in a mineral dissolution reaction, which can be obtained by multiplying the ion activity coefficient γi and composition concentration mi; and K is the equilibrium constant of mineral dissolution at a certain temperature (Kouzana et al.2010; Scott 2011).

General Hydrochemical Characteristics

The analytical results of the physiochemical indices are shown in Table 1. values of the electrical conductivity oscillating between 121 and 283 μS / cm for all the Bouteldja boreholes and values ranging from 1975 to 2740 μS / cm in the boreholes of saline, with three groups of chemical elements. The first has dominant contents of Na + 2 - Cl- (11-24 to 417-691 mg / l), followed by HCO3- - Ca + 2 (2- 1.6 to 448-208 mg / l) and SO4-2 - Mg + 2 (5.7- 1 to 413-100) respectively.

Table 1. Results of the physiochemical analyses and statistical analyses.

Parameter	Units	Minimum	Maximum	Average	SD
Température	°C	14,5	24,20	19,826	2,429
pH	/	5,080	7,780	6,469	0,634
EC	µS /cm	120,000	2740,000	641,909	882,167
NO2	mgL-1	0,010	0,110	0,028	0,022
NO3	mgL-1	1,100	21,260	7,644	5,257
Ca	mgL-1	1,600	208,420	45,543	68,295
Mg	mgL-1	0,910	99,650	18,907	28,498
Na	mgL-1	11,700	417,000	83,356	111,727
K	mgL-1	0,200	4,700	2,245	1,160
Fe	mgL-1	0,010	3,370	0,455	0,717
HCO3	mgL-1	2,220	448,350	107,872	165,230
Cl	mgL-1	24,820	691,330	134,091	189,675
SO4	mgL-1	5,760	412,800	57,057	96,748

Explanations: EC = electrical conductivity, SD = standard deviation, Source: own study.

EC (Fig.3), shows that the salinity of the waters of the Annaba-El Tarf region is in direct connection with the effect of evaporites for most of the samples taken.

Correlation matrix.

The correlation matrix (Table. 2) shows that the conductivity is highly correlated with the ions, Cl-, HCO3-, Na +, Ca2 +, Mg2 +, K + (r> 0.8). The strong correlation between Na + and Cl- (r = 0.985) is linked to the dissolution of halite by the presence of salt formations according to the reaction:

𝑁𝑎𝐶𝑙 → 𝑁𝑎⁺ + 𝐶𝑙⁻ (1)

And by a salinity of marine origin (Djabri 2004).

A very strong correlation between Ca2 + and HCO3- (r = 0.988), indicates that calcite is an important source of Ca2 +. The relationship of Ca2 + and SO42- (r = 0.804), indicates that the presence of sulfate and calcium ions in groundwater is linked to the dissolution of gypsum formations (Debieche 2002), according to the relationship:

CaSO4, 2H₂O → Ca² + SO₄−2 (2)

On the other hand, a strong correlation between Ca2 + and Na + (r=0.942) , Mg2 + and Na + (r = 0.871), can also be explained by the dissolution of silicates, which is a probable source of Na + in groundwater, as well as the base exchange between Ca2 + or Mg2 + and Na+. A very strong correlation between Ca2 + and Mg2 + (r = 0.931), indicates that the dissolution of calcite and dolomite is an important process for controlling Ca2 + and Mg2 + concentrations in groundwater. The origins of calcium are comparable to that of magnesium (Maya and Loucks 1995) they can also come from the combined dissolution of calcite, dolomite and gypsum depending on the reactions:

𝐶𝑎, 𝑀𝑔 (𝐶𝑂₃).₂= 𝐶𝑎⁺² + 𝑀𝑔⁺² + 2𝐶𝑂₃ (3)

𝐶𝑎𝐶𝑂 3 (𝑆) + 𝐻2(𝐿) + 𝐶𝑂2(𝑔) = 2𝐻𝐶𝑂^_ + 𝐶𝑎⁺² (4)

𝐶𝑎𝐶𝑂₃ = 𝐶𝑎⁺² + 𝐶𝑂^_2 (5)

𝑀𝑔𝐶𝑂₃ = 𝑀𝑔⁺² + 𝐶𝑂^_2 (6)

Table 2. Matrix of the correlation coefficients of the physicochemical of water samples (source: own study)

Parameter	T°C	pH	CE	HCO3-	Fe	Cl-	NO2-	NO3-	SO4-	Ca++	Mg++	Na+	K+
T°C	1
pH	0,086	1
CE	0,290	0,734	1
HCO3-	0,299	0,786	0,969	1
Fe	0,262	0,188	0,062	0,053	1
Cl-	0,314	0,677	0,977	0,916	0,078	1
NO2-	0,126	0,383	0,693	0,578	0,042	0,745	1
NO3-	0,053	0,005	0,015	0,069	0,375	0,038	0,021	1
SO4--	0,114	0,653	0,772	0,776	0,055	0,689	0,351	0,036	1
Ca++	0,243	0,772	0,984	0,988	0,068	0,940	0,623	0,021	0,804	1
Mg++	0,242	0,673	0,944	0,917	0,058	0,895	0,641	0,076	0,775	0,931	1
Na+	0,349	0,684	0,973	0,932	0,039	0,985	0,706	0,009	0,665	0,942	0,871	1
K+	0,351	0,646	0,841	0,821	0,166	0,851	0,593	0,055	0,515	0,808	0,768	0,852	1

Binary Ratios and Geochemical Processes

The Ca ^{+ 2}/Mg ^{+ 2}ratio provides information on the origin of these elements Ca + 2 and Mg + 2 from the dissolution of calcite and dolomite. If this Ca + 2 / Mg + 2 ratio ≤ 1, there is a dissolution of dolomite, on the other hand a higher ratio testifies to the dissolution of calcite, when it is greater than 2, it indicates the dissolution of silicate minerals .The application of this classification to groundwater in the Annaba-El Tarf region (Fig.4), shows that the majority of water samples analyzed (52.9%) have ratios greater than 2, thus translating dissolution of silicates followed by that of calcite (26.7%) and dolomite (20.6%).

Saturation Index

To better understand the process of mineralization of groundwater in the Annaba-El Tarf region by the dissolution / precipitation of certain minerals. The calculation of saturation indices was carried out for the waters of the boreholes of (Bouteldja, El Tarf, Les Saline and Barrahal). The calculation of saturation indices was carried out for the waters of the boreholes of (Bouteldja, El Tarf, Les Saline and Barrahal). The values of the saturation indices for each sample as well as the hydrochemical facies are presented in Table 3.

When:

IS <0, the solution is undersaturated with respect to the mineral (Dissolution of the mineral)

IS = 0, the solution and the solid phase are at equilibrium (Equilibrium)

IS> 0, the solution is supersaturated with respect to the mineral (Precipitation)

Table 3. Groundwater saturation indices for the Annaba-El-Tarf region.

locality	N°	Facies	carbonate minerals			evaporitic minerals
locality	N°	Facies	Calcite CaCO3	Dolomite CaMg (CO3)2	Aragonite CaCO3	Anhydrite CaSO4	Gypsum CaSO4 :2H2O	Halite NaCl
Bouteldja	1	CS	-3,51	-6,55	-3,65	-4,07	-3,84	-7,51
	2	CS	-3,16	-6,63	-3,31	-3,43	-3,18	-7,44
	3	CS	-2,72	-5,07	-2,87	-3,43	-3,18	-7,9
	4	CS	-3,46	-7,21	-3,61	-3,37	-3,13	-7,66
	5	CS	-3,82	-8,28	-3,97	-3,55	-3,31	-7,93
	6	CS	-3,51	-7,58	-3,65	-3,52	-3,28	-7,7
	7	CS	-3,52	-7,32	-3,67	-3,16	-2,92	-7,62
	8	CS	-3,36	-6,75	-3,51	-3,42	-3,18	-7,76
	9	CS	-3,78	-7,12	-3,93	-3,56	-3,32	-7,78
	10	CS	-3,3	-6,77	-3,45	-3,36	-3,12	-7,73
	11	CS	-3,29	-6,52	-3,44	-3,39	-3,15	-7,49
	12	CS	-4,48	-8,34	-4,63	-4,15	-3,9	-7,68
	13	CS	-3,88	-7,14	-4,03	-3,59	-3,34	-7,63
	14	CS	-4,52	-9,41	-4,67	-3,45	-3,22	-7,61
	15	CS	-3,5	-7,11	-3,65	-3,3	-3,06	-7,61
	16	CS	-3,76	-7,45	-3,9	-3,57	-3,33	-7,69
	17	CS	-3,77	-7,51	-3,92	-3,48	-3,25	-7,78
	18	CS	-3,88	-8	-4,03	-3,62	-3,39	-7,7
	19	CS	-3,13	-5,95	-3,28	-3,64	-3,4	-7,76
	20	CS	-4,07	-7,86	-4,21	-3,73	-3,5	-7,93
	21	BS	-2,48	-4,88	-2,63	-3,3	-3,05	-7,32
	22	BS	-3,68	-6,96	-3,83	-3,29	-3,07	-7,25
Les Saline	23	CS	0,53	1,07	0,39	-1,44	-1,21	-5,49
	24	CS	0,39	0,48	0,24	-1,3	-1,07	-5,51
	25	CS	0,26	0,47	0,11	-1,28	-1,04	-5,53
	26	BS	0,32	0,27	0,18	-2,03	-1,8	-5,56
	27	CS	0,19	0,26	0,04	-1,77	-1,53	-5,17
Barrahal	28	BC	0,31	0,72	0,17	-2,7	-2,48	-5,79
	29	SS	0,84	1,59	0,69	-1,16	-0,93	-5,88
	30	CS	0,29	0,52	0,14	-1,61	-1,38	-5,55
El-Taref	31	CS	-3,23	-6,37	-3,38	-3,39	-3,14	-7,64
	32	BC	0,24	-0,22	0,09	-1,97	-1,73	-6,99
	33	CS	-2,76	-5,4	-2,91	-3,42	-3,18	-7,45
	34	CS	-3,44	-7,12	-3,59	-3,31	-3,08	-7,53

Evaporitic minerals

The average values of the groundwater saturation indices are greater than zero in the waters of Barrahal and Salines, minerals tend to precipitate, and the dissolution process is observed only in the waters of Bouteldja and El-Tarf (Fig 5). The dissolution of carbonate minerals (calcite, dolomite and aragonite) is an important process for controlling concentrations of Ca2+, Mg2+ and HCO3- in groundwater. The CO2 enrichment of water infiltrated into the aquifer promotes the dissolution of carbonate by releasing Ca2 + and HCO3- ions in solution (Saadia et al. 1999; Jalali 2009)

The presence of carbonate minerals partly explains the strong electrical conductivities (Fig 6). The graphic representation of carbonate minerals (calcite, aragonite and dolomite) vs pH (Fig 6), illustrates that the evolution of these minerals is proportional to the evolution of pH .This increase in pH is due to the alkalinity produced by the dissolution of carbonates.

Evaporitic minerals

The calculated values of the saturation indices for anhydrite, gypsum and halite are less than zero for all samples (Table 3). The waters are undersaturated with respect to the main evaporitic minerals (halite, gypsum and anhydrite), which induces a dissolution of these minerals. The high contents of Cl- ,Na+, Ca2 +, Mg2 +, SO 2- and their good correlations with the electrical conductivity observed in water can be explained by the dissolution of halite and gypsum (Katz,1998; Saravanan et al.2015). Fig 8 and Fig 9 shows the correlation of the saturation indices of evaporitic minerals with the electrical conductivity and the pH respectively.

Saturation indices for carbonate and evaporitic minerals

The graphical representation of saturation indices as a function of Sulphates explains the process of precipitation / dissolution in the aquifers of north eastern Algeria. Sulphates have been used in the diagrams for their content but also for their contribution in the different processes of dissolution - precipitation. Fig 10 shows the saturation indices for calcite, dolomite, gypsum and halite as a function of sulphate concentrations.

Dissolving gypsum (Fig 10 (c)), all samples are in an undersaturated state, indicating that CaSO4 is a probable source of

Ca² ⁺ and SO₄2-.

The dissolution of halite takes place in the same way as gypsum (Fig 10 (d)); all samples are in a strictly undersaturated state, indicating that NaCl is the source of Na+ and Cl-. This shows that the evaporite formations are of the gypsum- saliferous type.

The representation of the saturation indices (SI) as a function of calcite, aragonite and dolomite (Fig 11 (a) and (b)) follow a positive linear trend which allows saying that the mineral phases are in the process of change with a similar tendency due to the same hydrogeochemical processes.

The integration of statistical approaches and geochemical methods were applied to investigate the regional factors and processes governing the chemical composition of groundwater on the north-eastern Algeria (Annaba-El Tarf). In general, the dominant hydrogeochemical facies of groundwater were the sodium chloride (82%), seconded by bicarbonate-sodium - calcium 14.7%.

The flow converges to the North—Eastern of Algeria. The chemistry of the groundwater of this plain is controlled both by the dissolution of the minerals of the evaporate rocks and those of the carbonate rocks, weathering of silicates and marine influence. The combination of statistical and hydrogeochemical analysis confirms the existence of these two families. The carbonate minerals (calcite, dolomite and aragonite) are saturated for some samples and undersaturated for others; therefore the waters are undersaturated with respect to the main evaporitic minerals (halite, gypsum and anhydrite).

Acknowledgments:

We would like to express my deepest appreciation to Editorial Assistant Environmental Earth Sciences and We thank anonymous reviewers for their valuable comments.

Authors’ Contributions:

Formal analysis and investigation specific to Dr Bounab Samia, Dr Sedrati Nassima wrote the main manuscript text, Dr Khammoudj Kaddour prepared all figures and tables and Dr Majour habiba prepared guideline manuscript.

All authors reviewed the manuscript.

Data availability

All relevant data are included in the paper or Supplementary Information.

Funding sources

The authors did not receive support from any organization for the submitted work.

No funding was received to assist with the preparation of this manuscript.

No funding was received for conducting this study.

No funds, grants, or other support was received.

Declaration of competing interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

The authors have no relevant financial or non-financial interests to disclose.

The authors have no conflicts of interest to declare that are relevant to the content of this article.

All authors certify that they have no affiliations with or involvement in any organization or entity with any financial interest or non-financial interest in the subject matter or materials discussed in this manuscript.

The authors have no financial or proprietary interests in any material discussed in this article.

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No competing interests reported.

Contribution Of Hydrogeochemical And Statistic Tools To The Acquisition Of Water Quality In The North-Eastern Of Algeria: Annaba-El Tarf

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Version 1

Abstract

Figures

1. Introduction

2. Materials And Methods

3. Results And Discussion

Conclusion

Declarations

References

Additional Declarations

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Version 1