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Quality Assessment of Various Bottled Water Marketed in Algeria: Health-Related Effects

Short title: Chemical quality of bottled water marketed in Algeria

Wahiba Bencheikh*1, Zhor Hattab2,Yamina Berredjem3 and Louis J. Lopes4

1Department of Biology, University of Badji-Mokhtar, Annaba,Algeria (E-mail: [email protected])

2Department of Chemistry, University of Badji-Mokhtar, Annaba,Algeria

3Departement of Science &Technology, University of Mohammed Cherif Messaadia, Souk_Aharas, Algeria

4 Departement of Industrial Engineering, University of San Diego State, California, USA.

*Corresponding author:[email protected] ABSTRACT

Forty-two different brands between mineral & spring waters were purchased from varied markets in Algeria, they analyzed for their bacteriological quality & chemical major elements. The results showed that all the brands presented good bacteriological quality (Absence of E. coli, Total coliforms, Ps. aerugenosa, enterococci & anaerobic spores). Piper diagram shown that (76.19%) of the samples were classified as Earth Alkaline water, where (80%) of them belong to dominant 𝐻𝐶𝑂3. By comparing the results with the WHO standards we found that only (16.67%) of the brands are compliant with the standards: Ain Bouglez, Righia, &Besbassa as spring waters, Texanna, El Goléa, Salsabil&Lalla Khadidja as mineral waters, those last two they have not enough TDS to consider them as mineral waters like mentioned in their labels, which confirmed by dendrogram classification. Otherwise, whenthe results comparewith the Algerian standards, all the brand waters turned to be compliant with them except for Arwa. Consumers must be very wary about the consumption of bottled water, especially if they already have health issues because they cannot make a choice only from the labels which are mostly different from the real chemical composition.

Keywords: Algeria, health-related effects, mineral water, Piper diagram, spring water.

HIGHLIGHTS

 Labels do not necessarily identify the real concentration of chemical components.

 Nitrate value exceeds in the bottled water: Arwa by 60 mg/L.

 Algerian standards of drinking water are very lenient compared with the World Health Organization standards.

 The 42 bottled water brandswere classified into 16 types with 70% similarity between them, using dendrogram classification.

GRAPHICAL ABSTRACT

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INTRODUCTION

Water is necessary for life and continuity, particularly safe drinking-water that guarantees significant health benefits; World Health Organization guidelines define safe drinking-water as it does not represent any significant risk to health over a lifetime of consumption (WHO 2017). People believe the idea that bottled water is healthy, cause of its richness by minerals which confer health benefits (Baba et al. 2008; Ward et al. 2009; Sharaf et al., 2021). Murakami et al. (2015) proved in their study that serum glycol-albumin levels were significantly decreased after Bicarbonate Mineral Water consumption (BMW) it tends to lower blood sugar levels, which may prevent and/or improve type 2 Diabetes. Whilst, nitrate may have the effect of protecting the gastrointestinal tract from variousgastrointestinal pathogens, because nitrous oxide and, acidified nitrite have antibacterial properties (WHO 2017). Also, potassium maintains the normal osmotic pressure in cells with sodium; it is a cofactor for many enzymes, a sufficient loss of potassium can result in Hypocalcaemia, which causes: cardiac arrhythmia, muscle weakness, nausea, vomiting, and low muscle tone in the gut. Longer-term hypocalcaemia causes a predisposition to hypertension, (Udhayakumar et al. 2016). Wherefore Osteoporosis patients should select water with high calcium, and magnesium concentrations to help with their skeletal fragility (Chiarenzelli &

Pominville 2008).

Salt minerals are vital for human body as they can be toxic if consumption is excessive, and this may in some cases be baneful (Stanhope 2018). Prolonged consumption of water with high EC (Electrical conductivity) and TDS (Total Dissolved Solids) may cause hypertension, heart attack, gastrointestinal irritation, and renal calculi (Udhayakumar et al. 2016; Rahman

& Rahaman 2018). Furthermore if serum calcium level rises to 160mg/Lmay cause coma, and death; too high magnesium causes nausea, muscular weakness, and paralysis when it reads a level of about 400 mg/L(Udhayakumar et al. 2016). Therefore, patients with kidney stone issues can benefit from avoiding hard or mineralized waters. And those suffering from hypertension should monitor their sodium intake, and avoid waters with high sodium content (Chiarenzelli & Pominville 2008). Excess in chlorine and sodium is harmful to people suffering from cardiac, circulatory, and kidney diseases. High sodium levels may cause hypertension with congestive heart failure (Udhayakumar 2016). Nitrate is themain contaminant in water, capable ofcausing acute toxicity problems; it may be a sign of other contaminants (Fortunato et al. 2020). It is lately cancerous as reduction to nitrite can occur in the organism with primarily gastric cancers. The ingestion of water that contains nitrate over 50 mg/L to 100 mg/L may give rise to infantile methaemoglobinaemia. (WHO 2017), simultaneous gastrointestinal infections may alter human thyroid gland function by competitively inhibiting thyroidal iodide uptake, leading to altered thyroid hormone concentrations, and functions, (Ward et al. 2009; WHO 2017) nitrate in water may also be relatedto theoccurrence of childhood diabetes.

With all these facts, the consumer remains confused about choosing the best for his body, especially with the existence of many brands in the market. According to Algerian ministry of trade in 2016, the number of bottled waterprocessing units is forty-two, in operation (42 Brands between mineral, and spring waters), and thirty-one planned units (concession granted). Consumers in Algeria always believe that bottled water is healthy and safe regardless of spring or mineral water. Mostly they are keen to take it with their medication during treatment, and whenever they can especially, for the elderly, pregnant women &

children.

Our study aims to give the opportunity to get acquainted with the quality of bottled water soldin the Algerian market.In this study, we analyzed the major components of bottled waters; their conformity with the international and local standards; and whether they pose a risk to the consumer’s health.

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METHODS

Over a span of two years (from 2018 to 2020), 42 different brands of spring water, and mineral water samples were purchased from various supermarkets in Algeria. The brand name, manufacturing and expiry dates, batch number, the chemical contents and the address of manufacture were documented in proforma. The water samples were coded and stored in the dark at room temperature and quickly analyzed in the laboratory. The water samples were analyzed just after its opening first for its bacteriological quality then for its chemical contents. The analyses were achieved according to APHA (2017)& Rodier et al.(2009) methods.

Bacteriological analysis

The under groundwater is naturally protected from the contamination of pathogenic bacteria, but there are many microorganisms in surface water. The contamination of spring and mineral water can happen during bottling. The bacteriological quality measured by the indicator organisms, in particular: Total coliforms, Escherichia coli, Pseudomonas aeruginosa, enterococci, and sulfite-reducing anaerobic spores, using the membrane filtration method (the media used in the analysis provided by Conda pronadisa).

Physicochemical analysis

ThepH, EC, and salinity measurements were determined by using pH meter (HACH, sens pH3) and, conductivity meter (HACH, sens IONTM+EC7) respectively. The water samples’

chemical constituents such as chloride𝐶𝑙, magnesium 𝑀𝑔2+, and bicarbonates 𝐻𝐶𝑂3 were analyzed by titrimetry 𝐶𝑙using standard AgNO3,𝑀𝑔2+concentration was esteemed by standard EDTA while carbonate and bicarbonates were estimated by titration withHCl. The dry residues at 180°C were determined by drying method using oven (BINDER 300°C) and the loss on ignition at (525°C±25) was determined by furnace (Nabertherm B180). The calcium, potassium, and sodium were analyzed by flame photometer (PFP7 JENWAY). A UV-Visible spectrophotometer (SHIMADZU UV-1800) was used to determine the sulfate 𝑆𝑂42− and nitrate 𝑁𝑂3 concentrations.

Data analysis

The physicochemical data were studied by graphic treatment with Piper class scatter plot using (Grapher 17 software) for better understanding of samples’ hydrogeochemical quality.

Comparethe results with WHO’s drinking water standards and Algerian standards (using Graphpad prism8) to determine which of our water samples are conform to the norms and which may have health risks. Finally, the water samples were classified to unknown groups depends on its similarity of their physicochemical results using clusters dendrogram by Statistica software.

RESULTS

Bacteriological quality

The bacteriological results showed thatall samples are exempt from pathogenic bacteria. No colonies detected in Cetrimide medium.The test results ofPs. aeruginosa, E. coli, Total coliforms, Enterococci & anaerobic spores were also negative. These outcomes indicate that all samples were completely conforming to the Algerian drinking water standards (Interministerial Decree 2016) and the WHO standards.

Chemical quality

The physicochemical results of water samples are summarized in Tables 1 & 2.

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Table1: Physicochemical parameters of mineral water samples.

p H

EC TDS 𝑪𝒂𝟐+𝑴𝒈𝟐+𝑵𝒂+ 𝑲+ Sali nity

𝑪𝒍 𝑺𝑶𝟒𝟐− 𝑯𝑪𝑶𝟑𝑵𝑶𝟑 Dry resid ues 180˚

Los s- on- igni tion Brands

µs/c m

mg/L mg /L

mg/

L

mg /L

mg /L

mg/

L

mg/

L

mg/

L

mg/

L

mg /L

mg/L

mg/

L LallaKha

didja

7.

8

282.3 1

242.4 6

24 14.

9

03 0.7 116 35.4 5

30 122.

03

2.3 0

41 6 Texanna 7.

5

337.7 4

269.8 4

18 8 20 3.2 147.

3

35.4 5

20.3 152.

54

2.3 6

98 54 Guedila 7.

5

819.5 654.7 5

54 35 30 2.4 356 70.9 1

108.

09

305.

1

4.6 7

400 90

Ifri 7.

3

888.6 752.2 3

10 0

44 50 1.9 374 99.3 80 305.

1

22.

13

406 72

Alma 7.

4

1135.

64

961.4 13 0

57 18 5.5 481 141.

81

100 335.

6

23.

5

602 243 Lavita 7.

3

1853.

95

1569.

43

16 0

112 17 0

2.7 810 184.

36

127.

5

762.

71

17.

3

979 123 ElGoléa 7.

8

326.2 1

280.2 16 11 33 14 142.

3

35.4 5

44 91.5 3

9.8 3

192 146 Salsabil 7 256.5

3

220.3 2

24 3 25 4.2 120.

8

71 6.7 76.3 10.

23

155 135 Saida 7 1214.

02

1028 66 56 69 2.8 530 127.

63

120.

5

274.

6

38.

2

501 27 Baniane 7.

25

930.8 1

788 63 50 31.

5

2.9 403 49.6 3

148 293 3.2 535 321 Mouzaia 7.

3

1765.

23

1494.

33

10 0

100 15 5

3 763 156 200 714 18.

5

705 91 Thevest 7.

7

885.1 749.2 3

84 40 10 2.5

3.2 439 78 205.

38

238 2.4 541 248 Toudja 7.

6

432.6 346 41.

7

12.

33

27 1 231 63.8 2

16 171 0.9 3

262 120 Messergh

ine

8 713.9 3

570.4 1

22 15 73 1.2 342 132 79 213.

6

5.5 4

368 305 Youkous 7.

7

438.4 350.2 53

37 7 25 2.8 172.

7

45 36 170 3.5 342 136 ManbaaE

lghezlane 7.

44

955.5 809 11 5

19 80 1 385 120 160 270 22 719 202 WHO

(1996, 2017)

6.

5- 8.

5

400 Min 250 Max6 00

10 0

30 20

0

- 150 250 250 500 50 - -

Algerian Standard s (Ex.D 2014)

6.

5- 8.

5

2800 - 20

0

- 20

0

12 - 500 400 50 1500 -

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Table 2:Physicochemical parameters of spring water samples.

p H

EC TD S

𝑪𝒂𝟐+𝑴𝒈𝟐+𝑵𝒂+ 𝑲+ Sali nity

𝑪𝒍 𝑺𝑶𝟒𝟐−𝑯𝑪𝑶𝟑𝑵𝑶𝟑 Dry resid ues 180˚

Loss -on- ignit ion

Brands µs/c

m

mg/

L

mg /L

mg /L

mg /L

mg /L

mg/

L

mg/

L

mg /L

mg/

L

mg /L

mg/

L

mg/

L Ain-

Bouglez 7.

5

131.

9

139 .45

<1 5

2.1 10 1 55 42.

54 18.

3

30.

5

8.4 9

36 2 Hassia 7.

3

763.

4

609 .94

63 12 23 2.5 334 219 .8

35.

07 30.

5

31.

17

322 86 Tazliza 7.

7

741.

5

592 .43

60 29 50 10.

3

315 106 .35

13 6

91.

52 19.

47

366 74 El

Ghadir 7.

6

941.

2

796 .8

69 17 45 2.9 406 63.

82 14 8

366 .1

35.

11

510 136 Ouwis 7 992.

1

839 .85

63 30.

5

51 1.3 435 78 17 6

274 .6

12.

30

534 125 Lajdar 7.

8

712.

54

569 .3

60 35 40 2.9 310 42.

54

62 305 .1

8.4 2

359 59 Righia 7.

6

132.

85

140 .5

<1 5

0 32 2 52.2 35.

45

0 156 .2

3.5 2

109 109 Fezguia 7.

7

594.

5

475 57 5 23 1.2 260 28.

4

54 274 .6

23.

9

361 76 Mileza 7.

44 103 0

872 63 33 56 1.5 440 21.

3

21 5

396 .6

2.6 0

539 84 Nestle-

Purelife 7.

64 538.

9

430 .55

45 13 41.

5

1.5 226 28.

4

47 207 .5

5.8 8

160 14 Togi 7.

5

669.

72

535 .1

60 18.

7

35 2.2 281 56.

72

34 274 .6

8.4 8

276 0 Ovitale 7.

5

716.

9

572 .75

69 23 35.

25

2.6 303 56.

72 15 6

219 .7

16.

03

361 66 BirEssal

am

7.

4

872.

9

738 .91

69 22 41.

25

2.1 371 28.

4

11 1

341 .7

3.3 8

501 33 Soumma

m

7.

5

177 2

150 0

15 0

70 11 0

3.2 770 304 .9

26 0

347 .8

33.

03

835 141 Arwa 7.

2

133 8.55

113 3.1

12 5

43 66 1.3 579 163 .1

23 7

329 .5

60 581 79 MontDju

rdjura 7.

2

800.

31

639 .42

69 17.

9

63 2.5 378 85.

1

50 311 .2

20.

76

501 317 Ifren 7.

4

441.

8

353 42 5.9 26.

25

2 226 28.

36 30.

4

201 .35

2.6 0

116 1 Ayris 7.

6

469.

7

375 .3

48 6.5 7 1 248 49.

63

45 201 .35

4.7 7

266 99 Star 7.

35 739.

2

590 .6

10 5

13 20 1 399 78 49 286

.8

31.

36

543 201 Gueriou

ne

7 547.

34

437 .31

54 2.5 14 1 261 142 60 135 .6

17.

76

404 305 Besbassa 7.

7

345.

34

275 .92

69 1.7 45 1 135.

4

60 12 70 11.

27

279.

9

120

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SidiRach ed

7.

55 608.

21

485 .94

80 5 50 2 241 60 35 207 35 526.

5

141 El-

Kantara 7.

56 713.

83

570 .33

70 3 35 1.2 284 55 75 300 22 562 160 DjebelA

mour

7.

63 656.

4

524 .4

45 6 30 <0 .2

262 45 10 0

240 43.

85

307 120 Lajdar 7.

8

712.

54

569 .3

60 35 40 2.9 310 42.

54

62 305 .1

8.4 2

359 59 Taya 7.

5

473.

5

378 .3

50 11 65 1 187.

1

117 99 65 28 490 200 Messad 7.

6

769.

2

614 .6

75 7 60 1 307 170 16 0

120 1.1 9

600 322

The chemical contents of water depend on the composition of rocks from which it is extracted and by geochemical processes (Van der Aa 2003). The hydrogeochemical was evaluated by Piper trilineardiagram shown in Figure 1.

Figure 1: Piper Trilinear diagram showing the type of water samples.

DISCUSSION

The diagramallowed us toclassify the waters samplesusing the main cations 𝐶𝑎2+,𝑀𝑔2+, 𝑁𝑎+, 𝐾+ and, anions𝐶𝑙, 𝑆𝑂42−,𝐻𝐶𝑂3, 𝑁𝑂3 (Piper 1944; Ravikumar et al. 2015; Varol & Şekerci 2018). Only (9.5%) of samples were classified as Normal earth

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alkaline waters: Lalla khadidja, Star, and Ayris with dominant bicarbonate, Alma with dominant bicarbonate &chloride. (14.28%) of samples belong to the alkaline water: El Goléa, Messerghine, Salsabil&Ain Bouglez with dominant bicarbonate, Righia with dominant chloride. Most samples (76.19%) were classified as Earth Alkaline water, where (80%) of them belong to dominant HCO3-

.

The pH of samples varied from 7 to 8, which is within the 6.5-8.5 range recommended for drinking water (Executive Decree 2014; WHO 2017).

The EC values vary from normal: Lalla Khadidja, Texanna, ElGoléa, Salsabil,Ain Bouglez, Righia&Besbassa, into high in both mineral & spring water samples (131.9𝜇c cm-1 − 1853.95𝜇c/cm), The EC value of more than 83% of water samples is higher than the allowable WHO value for drinking water:400𝜇c/cm. However, the EC threshold is 2800𝜇c/cm in Algerian standards (Executive Decree 2014; Tahmasebi et al., 2020), which makes all water samples compliant with the Algerian permissible limit for EC. The EC is proportional to the TDS. Drinking-water becomes significantly andincreasingly unpalatable at TDS levels greater than about 1000mg/L (WHO 2017): Lavita: 1569.43 mg/L, Mouzaia:

1494.33mg/L and Saida: 1028 mg/L, also with the bottled spring water: Soummam: 1500mg/L

&Arwa: 1133.1mg/L, whereas (45.23%) of samples exceeded the allowable limit of TDS:

600mg/L.The US Food and Drug Administration (FDA) describes natural mineral water as water containing at least250 mg/L ofTDS (Ong et al. 2009), which is not carried out with two water samples labeled as natural mineral water: Lalla khadidja: 242.46mg/L&Salsabil:

220.32mg/L.The patability of water samples related toTDS concentrations is shown in Table 3.

Table 3:The patability of water samples based on their TDS concentrations.

TDS Concentrations (mg/L) Drinking water

quality (WHO 1996)

Excellent

<300

Good 300- 600

Fair 600-900

Poor 900- 1200

Unacceptable

> 1200 Mineral water

samples

Lalla khadidja Texanna El Goléa, Salsabil

Toudja Messerghine Youkous

Guedila Ifri, Baniane Thevest Manbaa el ghezlane

Alma Saida

Lavita Mouzaia

Spring water samples

Ain Bouglez, Righia Besbassa

Tazliza Lajdar Fezguia Nestle Pure life

Togi Ovitale Ifren Ayris, Guerioune Sidi Rached El Kantara Djebel Amour Taya

Hassia El Ghadir Ouwis Mileza Bir- Essalam Mont Djurdjura Messad

Arwa Soummam

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The Calcium concentrations exceed the WHO permissible limit (WHO2017) in six samples (they represent 14.28 %), where the upmost concentration is: 160 mg/L, for Lavita mineral water. In the spring waters: Righia&Ain Bouglez the calcium concentrations were below the detection limit. The calcium concentrations of water samples were within the permissible limit of Algerian standards.

The magnesium concentrations ranged from 0 to 112mg/L, (30.95%) of samples exceeded the limit; the highest value detected with Lavita.

The potassium and sodium concentrations of all samples are within the allowable range.

Also, the chloride concentrations were within the WHO permissible limit unless with the spring water Soummam: 304.9mg/L, as well still conform to the Algerian standards, while (80.95%) of samples exceeded the threshold limit of NaClspecified by the WHO at 150mg/L(WHO 1996).

According to WHO standards (WHO 2017), the permissible limit for sulfate is 250 mg/L. We noticed that all water samples were within the threshold limit unless for the mineral water Soummam: 260 mg/Lhowever, it conforms according to the Algerian standards where the permissible limit for sulfate is 400mg/L.

The WHO threshold limit of bicarbonate is 500mg/L, in all samples the bicarbonate values are within the standards, except for one mineral water: Lavita: 762.71mg/L.

The nitrate maximum limit is given by 50 mg/Laccording to WHO and Algerian standards.

The nitrate originates from organic matter degradation. Due to agricultural activities, it can reach groundwater and/or occasionally natural vegetation (WHO 2017; Adamou et al. 2020) only the spring water Arwa exceeded the permissible limit by 60 mg/L.

The loss on ignition measurement allowed us to determine approximately the organic matter in dry residues due to decompositions and volatilizations of mineral salts. Organic matter is the causeof such aesthetic concerns as color, taste & odor (Rodier et al. 2009). The highest organic matter concentrations were observed with: Lavita: 856 mg/L&Soummam: 694 mg/L, while the lowest concentration was with: Righia spring water: 0 mg/L. Generally, we estimated a high organic matter in all water samples except for Lalla Khadidja, El Goléa, Salsabil&Ain Bouglez.

We can observe clearly in Figure 2,Whether or not the samples comply or not with both Algerian standards and the WHO drinking water guidelines.

Figure 2:The chemical composition of water samples compared with WHO& Algerian standards.

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The Algerian standards’ limits are very high which allows all the water types to be within the range even with their high mineralization except for Arwa.

Conversely, the WHO drinking water standards are strict; allow only a few brands of bottled waters to be safely usedas potable water. Consequently, only 16.67% werecompliant with the norms: Ain Bouglez, Righia&Besbassa as spring water, Texanna&El Goléa as mineral water.

Salsabil and Lalla Khadidja were compliant with the drinking water standards, but not as natural mineral water as indicated on their labels because their TDS concentrations were below the minimum level.

As wellFigure 2 allowed us to notice the overlapping in the chemical parameters of spring and mineral water. No uniformity between the same-category brands. We observed water brands labeled as natural mineral waters have low mineralization, per contra spring waters with very high mineralization, as TDS in Soummam is 1500 mg/L. In this regard we readout that, the designation of bottled water as mineral or spring water was done randomly.

Which is approved after classifying all samples into unknown groupsdepends on their similarity of their physicochemical results using clusters dendrogram (Figure 3).

Figure 3:Dendrogram of 42 bottled water samples.

This classification is called Q-mode classification (Belkhiri et al. 2010) Ain Bouglez was very close to Righia, had equally distant, which means they are similar; this is because both springs water filled from the same area. From this point, we could count sixteen clusters with (70 %) of similarity, starting from the top of dendogram: 1 (Ain Bouglez&Righia) 2 (from Nestle life pure to Texanna) 3 (Messad) 4 (from Hassia to Ifri) 5 (From Mont Djurdjura to Sidi Rached) 6 (Baniane&Thevest) 7 (Gueriuone) 8 (Taya) 9 (Manbaa elghezlan) 10 (Alma) 11 (Arwa) 12 (Saida) 13 (Messerghine) 14 (Soummam) 15 (Lavita) &16 (Mouzaia).

We noticed that the mineral water: Toudja, Youkous, ElGoléa, Lalla Khadidja are situated on the range close to spring water,which is consistent with Hazzab (2011) study’s results, same remark with Salsabil&Texanna. As well, some spring waters are situated close to the mineral waters range as Arwa&Soummam.

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CONCLUSIONS

Forty-two water brandswere analyzed; where all were bacteriologically safeas the results shown. The hydrochemical quality showed that 76.19% of samples are Earth Alkaline water with 𝐻𝐶𝑂3dominants mostly. The physicochemical data of 14 parameters compared with WHO and Algerian standards. 83.33% of brands did not conform to the WHO’s drinking water guidelines, which may pose risk to consumers with health issues, infants, young children, debilitated people, & the elderly. We concluded that not all bottled water is safe for all categories of people, the selection between water types must be based on chemical composition mentioned in labels and health condition of the consumer, that’s why we suggest adding some important information on label, such as TDS concentration. Furthermore, 97.62% of samples are compliant with the Algerian standards, the large differences between the local and the international standards; affect theexport trade of bottled water and consumer’s health.

We recommendthat the Algerian standards adapt to international drinking-water standards and apply strict control of the bottled water labels and their updating, whenever required to avoid the falsification and random nomination among spring and mineral water.

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