THE CONCENTRATION OF FLUORIDES IN TAP WATER AND COMMERCIAL BOTTLED BEVERAGES IN CAZMA- NORTHEN CROATIA Muini D, Krmek S

ABSTRACT The aim of this study was to measure the concentration of fluorides in tap water in Northern Croatian town azma and commercially available bottled drinks. For assessment of drinking habits the questionnaire was conducted. Among 200 randomly chosen patients of The Community Health Centre Cazma. The results showed that the tap water was most consumed, then milk, concentrates, carbonated beverages, beer and vine. Fluoride content in tap water from public supply was assessed by ionic chromatography and was 0,313 mg F-/l. Fluoride content in commercial drinks was assessed by fluoride-selective electrode and was the highest in carbonated mineral water (0,34 - 1,5 mg F-/l), then in some ice tea drinks (0,060,74 mg F-/l) Non-carbonated waters, carbonated soft drinks and noncarbonated soft drinks had very low fluoride concentration and it was <0,01 mg F-/l, 0,02 mg F-/l and 0,06-0,15 mg F-/l, respectively. Low pH of those drinks (2,36 -2.68 in carbonated drinks and 3,08-3,64 in juices) in combination with added sugars and low concentration of fluorides could have cariogenic potential. The results obtained in this investigation could be used in planning preventive measures.

INTRODUCTION According to the World Health Organization (WHO) caries still presents an important public health issue in the majority of industrialized countries, where it affects 60-90% of schoolchildren and the vast majority of adult population. (1). In the countries with growing incidence of caries, WHO recommends various methods of topical fluoridation. In groups exhibiting very high caries prevalences endogenous methods such as drinking water fluoridation showed certain advantages. The fluoridation of salt or milk is recommended as an alternative to water fluoridation (1,2). In planning water fluoridation as a caries protective measure it is important to consider other ways of fluoride intake to avoid exceeded exposure to this micronutrient and its adverse affects. When estimating the overall intake of fluorides it should be considered that the alimentary habits are nowadays quite changed, in the sense that considerable quantity of consumed alimentary products, water, and drinks in general, is highly fabricated and consumed in distant regions. It is, therefore, possible that the consumption of fluorides via beverages in a certain population is not at all in correlation with its concentration in tap water. In order to get the reliable information about the overall intake of a certain substance, in this case fluoride, it is necessary to make a detailed analysis of all alimentary products and the quantities consumed by an individual (3-5). It is also necessary to test fluorides absorption from different fluoride containing oral hygiene products. (4,6). Beverages are frequently consumed during the day and certainly contribute to overall daily intake of fluorides a lot, which makes the analysis fluorides in them an important step in obtaining data about consumed fluoride and proposing preventive measures including fluoride supplements. The content of fluorides in natural waters depends on their concentration in soil, geologic formation of the area through which water flows, the quantity of precipitation, and the intensity of water evaporation. The value of fluorides in natural water is between 0,01 5,0 mg F-/l or 0,52 M -0,26 mM (7). The concentration of fluorides in surface waters depends on the location and vicinity of fluorides source, and their concentration in unpolluted fresh water varies from 0,01 to 0,3 mg F-/l, while in unpolluted sea water fluoride concentration ranges from 1,2 to 1,5 mg F-/l (8).

Human activities led to the increased level of fluoride in surface waters. Skjelkvle (9) found that some Norwegian water flows in the vicinity of aluminum industry, may contain more than 10 times as concentration of fluorides as natural waters in the area. Other major source of fluorides is phosphate fertilizers industry, which increases the natural concentration of fluorides more than 100 times, then the industry producing chemicals such as hydrogen fluoride, calcium fluoride, sodium fluoride and sulphor hexafluoride, brick, ceramics and glass industry, the usage of pesticides containing fluorides (8,10,11). Plants contain different amounts of fluorides which is partly dependent on the soil at which they grow. The concentrations of fluorides in fruit and vegetables used in human nutrition range from 0,02 mg F-/kg of dry matter (plums) to 1 mg/kg dry matter (spinach) (7). The plant with the highest fluoride level is tea (Folium Theae), and dependent on the area of growth contains from 15,0 to 189,7 mg F-/kg (on average 70 mg F-/kg). Meat contains from 0,2 to 2,0 mg F-/kg, and fish from1,0 to 27,0 mg F-/kg (7) In the last few decades, the prevalence of dental fluorosis increased significantly, especially in the communities with community water fluoridation. That is why there has been a growing interest in identifying the sources of fluoride contributing to this trend. (3) In 1988 Lopez and Navia (12) have developed a method of analyzing dietary fluoride and have reported the fluoride content of a number of food and beverage samples. In the last few decades a number of studies have reported on the fluoride content in a large number of food and beverages in different communities and in different countries (3-6). In Croatia, the prevalence of caries is very high, oral hygiene is bad, even among highly educated population, and the main reason for teeth extraction is caries (1315). The objective of this study was to determine the fluoride content of tap water and commercially available beverages in the town of Cazma in Northern Croatia and through the questionnaire about the consumed daily quantities get an insight into the consumption of fluorides by the population of Cazma by drinking.

MATERIALS AND METHODS The questioner about beverage consumption habits was carried out in order to obtain the necessary information about the drinking habits. On the basis of the data obtained from the questionnaire, the sample for the analysis could be formed (and average daily consumption quantity of fluoride calculated). (Figure 1). Figure 1. Questionnaire about the drinking habits of the population of Cazma

Sex:

Age:______ level of education: 1 elementary, 2 high

school, 3 baccalaureate; 4 university Encircle a number and a letter before a drink and quantity you consume on a daily basis: 1. a. b. c. d. e. 2. a. b. c. d. e. 3. a. b. c. d. e. 4. a. b. c. d. e. 5. a. b. c. d. 6. a. b. c. d. e. Tap water One glass Two glasses Three glasses Four glasses Five and more glasses Carbonated soft drinks One glass Two glasses Three glasses Four glasses Five and more glasses fruit concentrates (syrupy and powdery) One glass Two glasses Three glasses Four glasses Five and more glasses milk One glass Two glasses Three glasses Four glasses Five and more glasses beer One glass Two glasses Three glasses Four glasses wine One glass Two glasses Three glasses Four glasses Five and more glasses something else, name

7.

The questionnaire was carried out among the patients of the Community Health Center Cazma chosen by random choice. 200 patients between the ages of 11-84, of both genders, participated in the questionnaire. The sample of potable tap water was collected from the water supply system into a plastic container. Commercial bottled non carbonized water (plain and aromatized), carbonated and natural fruit juices, tees were obtained from a local groceries. The concentration of fluorides in tap water was determined by ion chromatography (method HR EN ISO10304-1:1998). Fluoride working solutions were made by diluting the stock fluoride solution of the concentration of 20 mg F-/L (Dionex, 7681-49-4, grad, zemlja) with deionized glass-distilled water. Concentrations of standards and the areas under the curve are listed in Table1. Table 1. standard fluoride solutions and their areas under the curve Standard solutions Standard 1 Standard 2 Standard 3 Standard 4 Standard 5 mg F-/L 0,05 0,1 0,5 1 2 Areas under the curve 10659 14718 70854 163716 322906

The solution that served as mobile phase in determining anions in aqueous solutions was prepared using carbonate and hydrogencarbonate 0,5M solutions (REFERENCA) Prior to any measurement, the chromatograph's (ime, grad, zemlja) good working order had to be confirmed according to the manufacturers instructions. It was automatic and lasted 1-3 minutes after the instrument had been turned on. Then, after half and hour time, the instrument's electro conductance stabilized at the value bellow 20 S/cm. The sample (2-5 ml) was then placed in the injector using disposable syringe and the 0,5 ml of the sample was injected and analyzed. The chromatography was stopped after 5 minutes, after the fluorides peak had been recorded. The fluoride content in commercial bottled drinks was determined using an ion selective electrode. The electrode records the activity of a specific ion dissolved in a 5

solution into an electrical potential, measured by a voltmeter. The indicating electrode is an ion-specific membrane, which together with the reference electrode, and electrolyte solution (sample solution) makes up an electrochemical cell. The voltage measured by the voltmeter is, according to the Nernst equation, theoretically dependent on the logarithm of the ionic activity i.e. concentration: E=E+S log (A), (E measured electrode potential; E- referential potential (constant); A activity of fluoride ions in the solution; S electrode incline) (16). For the measurements of fluoride ion concentration, the microprocessor analyzer ORION EA 940 (Orion Res Inc, USA) with pH electrode tip 91 02 BN (Orion Research Inc, Beverly, USA) and fluoride ion-selective electrode type 96-09 (Thermo Fisher Scientific, Beverly, MA, USA) were used.. Before the analyses, carbonated beverages were maintained at room temperature for 12 h for decarbonation (17). The pH of the electrode was calibrated with two buffer solutions of pH 4,24 and 6,90, respectively. 4,5 ml of each sample or standard were mixed with 0,5 ml of Total Ionic Strength Buffer (TISAB II), and the pH of each sample was measured before and after TISAB adding. TISAB contains reagents that release fluorides from the complexes with metal ions (Fe, Al, Mg) and maintains pH around 5-6, which is very important since the fluoride ion selective electrode reacts to the changes in the concentration of OH- ion (16). The measurements were performed by placing the samples directly under the electrode (18). The resulting millivolt readings were recorded in triplicates for each sample, and the fluoride concentration was calculated from the standard curve (concentrations of standards were 0,19 -1,9 mg/L). For making standard working solutions, the stock solution (Orion) (0,1 M (1 900 mg F/L) and deionized glass distilled water were used. The electrode incline was 96%. During the measurements, standards and samples were mixed at a constant rate using a magnetic mixer and a magnetic stick. Between the mixer and the vessel a piece of polystyrene was placed in order to keep the temperature constant during measurement.

RESULTS 6

The data about drinking habits of 200 patients was obtained from questioner. Demographic data is shown in Figures 2 and 3. Is can be noticed that females were more represented in all age groups except in the group +65 years. The majority of the examinees had high school level of education. Moda bi se moglo napisati tono koliko je bilo enskih, koliko mukih u postocima i koliko je posto svake pojedine strune spreme. u tom sluaju bi se izbacile ove dvije slike. Ja na alost ne mogu iitati konkretne postotke iz slika

Slika 2. Distribution according to the gender and age.

Slika 3. Distribution according to the level of education 7

Concentr Carbona Tap Gender M Arith. mean Number Std. dev. Arith. mean Number Std. dev. Number Std. Dev. water. 1,94 80 0,905 1,98 121 0,707 1,97 201 0,790 ted drinks 0,76 80 0,917 1,03 121 0,991 0,93 201 0,969 ates diluted by tap water 0,69 80 0,866 1,03 121 0,718 0,90 201 0,796 Milk 1,96 80 1,174 1,87 121 1,064 1,91 201 1,107 Beer 0,98 80 1,102 0,16 121 0,466 0,48 201 0,878 Wine 0,79 80 1,133 0,12 121 0,346 0,38 201 0,829 Hard liquors 0,16 80 0,538 0,04 121 0,300 0,09 201 0,415

Non mineral waters 0,04 80 0,249 0,04 121 0,238 0,04 201 0,242

Nonaromatized min. w. 0,19 80 0,695 0,05 121 0,338 0,10 201 0,514 coffee 1,19 80 1,370 1,72 121 1,043 1,51 201 1,209

carbonated carbonated

Total. Arith. mean

Table 3. The average daily beverage consumption expressed in glasses per person- male of female (coffee is expressed in cups)

From Table 3 it can be noticed that water is most consumed in both, males and females (almost 2 glasses per day), followed by milk, whereas bottled noncarbonated mineral waters are drank rarely.

Table 4. The results of the variance analysis (one-way ANOVA) differences in beverage consumption with respect to gender (difference is significant if p<0,05)
Sum of squares Tap water Between groups Within groups Total Carbonated soft drinks Between groups Within groups Total Concentrates diluted with tap water Milk Between groups Within groups Total Between groups Within groups Total Beer Between groups Within groups Total Wine Between groups Within groups Total Hard drinks Between groups Within groups Total Non-carbonated mineral waters Between groups Within groups Total Non-carbonated aromatized mineral waters Coffee Between groups Within groups Total Between groups Within groups Total 0,102 124,654 124,756 3,525 184,355 187,881 5,751 121,055 126,806 0,432 244,772 245,204 32,223 121,967 154,189 21,735 115,768 137,502 0,707 33,681 34,388 0,001 11,681 11,682 0,916 51,890 52,806 13,605 278,634 292,239 df 1 199 200 1 199 200 1 199 200 1 199 200 1 199 200 1 199 200 1 199 200 1 199 200 1 199 200 1 199 200 13,605 1,400 9,717 0,002 0,916 0,261 3,513 0,062 0,001 ,059 0,012 0,913 0,707 0,169 4,178 0,042 21,735 ,582 37,361 0,000 32,223 0,613 52,574 0,000 0,432 1,230 0,351 0,554 5,751 0,608 9,453 0,002 3,525 ,926 3,805 0,052 Average square 0,102 0,626 F 0,162 Sig. 0,687

Females consume significantly more juice concentrates diluted with tap water and coffee, while males consume significantly more beer, wine and hard drinks.

Table 5. The average consumption of beverages in glasses with respect to age

Concent rates diluted Tap Age 10-17 Arith. mean Number Std. dev. 18-34 Arith. mean Number Std. dev. 35-64 Arith. mean Number Std. dev. 65+ Arith. mean Number Std. dev. Total. Arith. mean Number Std. dev. Carbonat with tap water 1,71 24 0,624 1,29 49 0,612 0,63 95 0,730 0,48 33 0,667 0,90 201 0,796 Milk 1,92 24 1,060 2,02 49 0,878 1,69 95 1,112 2,33 33 1,315 1,91 201 1,107 Beer 0,08 24 ,408 ,41 49 0,705 0,66 95 1,048 0,36 33 0,699 0,48 201 0,878 Wine 0,00 24 0,000 0,00 49 ,000 0,62 95 0,980 0,55 33 0,971 0,38 201 0,829 Hard liquors 0,00 24 0,000 0,02 49 0,143 0,17 95 0,577 0,03 33 0,174 0,09 201 0,415 water. ed drinks 2,54 24 0,588 2,02 49 0,692 1,87 95 0,828 1,73 33 0,761 1,97 201 0,790 1,87 24 0,741 1,41 49 0,864 0,75 95 0,899 0,03 33 0,174 0,93 201 0,969 Non mineral waters 0,29 24 0,624 0,02 49 0,143 0,00 95 0,000 0,00 33 0,000 0,04 201 0,242 Nonaromatized min. w. 0,04 24 0,204 0,18 49 0,635 0,04 95 0,289 0,21 33 0,857 0,10 201 0,514 coffee 0,37 24 0,770 1,49 49 1,139 1,86 95 1,260 1,33 33 ,854 1,51 201 1,209 carbonated carbonated

The concentration of fluorides in tap water measured by ion chromatography was 0,3137 mg/L . The results of the analysis of fluorides concentration by fluoride selective electrode in different samples of commercially available beverages are shown in Table7. The concentration was the highest in carbonated mineral waters (0,34 1,5 mg F-/l), then in some ice teas (0,06 -0,74 mg F-/l). Commercial bottled non carbonated waters contained very low concentrations of fluorides (below 0,01 mg F-/l), as well as carbonated (0,02 mgF-/l) and fruit juices (0,06 0,15 mg F-/l). The low pH of the drinks can, together with the low fluoride concentration, act very cariogenic. Table7. pH and concentration of fluorides in commercial drinks
Product Manufacturer pH of the beverage pH after adding Cons of F- (mg/L)

10

TISAB JANA Non-carbonated waters Jamnica d.d, 7,65 Getaldieva 3, Zagreb, BISTRA Croatia Coca-Cola, Beverages, 6,96 M. Sachasa 1 Zagreb, JANA JAGODA Croatia Jamnica d.d, Getaldieva 3; Zagreb, JANA LIMUN Croatia Jamnica d.d, Getaldieva 3, Zagreb, Croatia JAMNICA Carbonated waters Jamnica d.d, 8,35 Getaldieva 3; Zagreb, MIVELA Croatia Nova sloga Kneginje Milice 81/1 STUDENAC Trstenik, Serbia Podravka d.d. A. Starevia 32 DONAT MG Koprivnica Croatia Droga Kolinska Kolinska cesta 1 Ljubljana, Slovenia Carbonated soft drinks Coca-Cola, Beverages, 2,68 M. Sachasa 1 Zagreb, Croatia Product Manufacturer pH of the beverage
FANTA Coca-Cola, Beverages, M. Sachasa 1 Zagreb, COCA COLA Plastina boca 2,86

4,86

0.080

5,09

0,092

3,21

5,02

0,050

3,29

4,96

0,052

4,93

0,632

7,34

4,96

0,378

7,00

5,15

1,500

7,89

5,65

0,015

SPRITE

4,91

0,020

pH after adding TISAB 4,93

Cons of F- (mg/L)
0,020

Croatia Coca-Cola, Beverages,

M. Sachasa 1 Zagreb,

2,36

4,99

0,018

11

COCA COLA Limenka

Croatia Coca-Cola NBC,

Trestev Strasse 91, Vienna, Austria Tees

2,43

4,99

0,018

ICE TEA STUDENA

Podravka d.d. A. Starevia 32 Koprivnica Croatia Eurobev d.o.o. Borongajska cesta 104, Zagreb, Croatia Podravka d.d. LERO d.o.o. Tome Striia 8, Rijeka, Croatia Coca-Cola, Beverages, M. Sachasa 1 Zagreb,

3,33

4,95

0,180

ETERNA

2,84

4,89

0,062

GREEN TEA

3,34

4,88

0,375

VITAO

3,07

4,93

0,738

Croatia
Fruit soft drinks VINDIJA JABUKA Vindija d.o.o. Meimurska 6 VINDIJA BRESKVA Varadin, Croatia Vindija d.o.o. Meimurska 6 VINDIJA BOROVNICA Varadin, Croatia Vindija d.o.o. Meimurska 6 MARASKA NARANA Varadin, Croatia Maraska d.d. Biogradska c. 64A MARASKA MULTIVITAMIN Zadar, Croatia Maraska d.d. Biogradska c. 64A Zadar, Croatia 3,27 4,92 0,080 3,64 4,88 0,064 3,08 4,69 0,116 3,47 5,01 0,099 3,26 5,00 0,146

12

DISCUSSION Recent epidemiologic data show that dental caries remains a public health problem in many developing countries, where significant increase in dental caries prevalence was recorded in schoolchildren and adults (2,19,20). Croatia is among the countries with bad oral health including high caries prevalence (12,14,15, 21). Although in the 1970ies and 1980ies there was a decreasing trend in caries prevalence the research in the last few decades showed negative oral health trends (12,14). In Croatia, the factors contributing to negative trends in oral health suspended preventive dentistry in the process of privatization of dental profession, and war in the early nineties, which has caused many setbacks. On the global level such a trend in caries prevalence is attributed to the increasing consumption of sugar and inadequate exposure to fluorides (2) For this reason it was recommended that caries be controlled by applying well known and established fluoride implementation methods, with the emphasis on public health approaches including: water, salt and milk fluoridation, the development of affordable fluoride toothpastes, topical application of fluorides, (re)introduction of educational programs in schools (tooth brushing, dental floss usage, nutrition, paying regular visits to dental office) (2). The increasing consumption of commercial noncarbonated mineral waters and soft drinks certainly added a new variable in explaining and estimating the incidence of caries. The main reasons why people choose bottled waters over tap water is the concern about the microbiologic safety, avoiding potential chemical pollutants and chlorine added for disinfection, the taste of water suits better, and the belief that bottled water is healthier than tap water (22). It was found that the level of fluorides in bottled water is significantly lower than in tap water (22), which is in concordance with the results of our study where the concentration of fluorides in commercial waters was (0,050 0,080 mg/L F- ), and in tap water (0,313 mg/L F-). The level of fluorides in tap water was below the recommended value in caries preventive activities, and the recorded low value of fluorides in commercial waters does not whatsoever contribute to caries incidence decrease in individuals consuming them. The fluoride concentration was declared in only a few products and the values 13

recorded in our study corresponded to the declared vales. It was reported that in the USA less than 5% of the products had the concentration of fluoride declared, while in Canada, where the declaring of fluoride content is obligatory, all products had the fluoride concentration stated in the declaration (23, 24). Wienberger (23) investigated the accuracy of the declared values and reported that they are not correct in all cases. Besides low fluoride concentration value in tap water and commercial drinks, the factor contributing to increasing DMFT index is the increasing consumption of low molecular carbohydrates, especially among children. In some parts of Croatia DMFT among 12 year olds reaches 9,5, and is in correlation with the concentration of fluorides in tap water (25). According to the WHO report from 2003 DMFT index among 12-year olds was 2,7 4,4 (20). Decrease in caries incidence in pre-school children of lower economic status in Brazil was recorded after the fluoridation of tap water had been done (26). The majority of the population in our study consumed tap water. The tap water in Croatia has never been fluoridated, and is much below the level recommended in preventive measures. Anyway, the majority of water from water supply systems is not consumed, but used in household for other purposes or lost. Together with the fact that adding fluoride is more expensive than adding chlorine for disinfection, along with the reports on he increased prevalence of fluorosis, does not make it the most preferable choice in public health measures. According to some reports, net daily consumed quantity of sugars remained the same over the years, but the form in which they are consumed changed today they are mostly consumed via soft drinks (27). The pH of soft drinks in this study was very low (pH=3,08 3,64), much lower than pH 5,5, which is considered the critical acidity value for hydroxilapatite demineralization, although the loss of tooth mineral content can occur in a less acidic environment (28). The fluoride content of soft drinks was also very low (0,06 0,14 ppm F-) which makes them even more cariogenic. If the pH were higher than 4,5, and the fluoride ions available in low concentration, fluorohydroxiapatite would precipitate in surface layer, while the hidroxyapatite in deeper enamel layers would dissolve. With growing pH above 5,5, and available fluoride ions, remineralization of enamel and dentine would take place. Hydroxilapatite crystals with incorporated fluoride in remineralization process are less soluble than calcium hydroxilapatite (29). 14

The fluoride content in commercial beverages of some multinational companies, such as Coca Cola, differs among countries and depends on the fluorides concentration in the local water from which the drinks are made. For instance, is the fluoride concentration in Cola beverages in Mexico is 0,49 ppm (in the range from 0,10 to 1,62 ppm) (31), which is significantly more than in our study. Furthermore, we did not find any significant difference in fluoride concentration of carbonated soft drinks beverage in plastic bottle and tin, which is not in concordance with the results of the study in Mexico (30). Since the fluorides have high affinity towards glass and metals, it is well expected that their concentration would be lower in tin or glass bottle. The reason why we did not record any difference between carbonated soft drinks in plastic or tin lies probably on the fact that the concentrations were very low and difficult to detect. Higher fluoride concentration was found in carbonated mineral waters. One of them contained 1,5ppm of fluorides which is the higher value of that recommended in caries prevention. This fact can be taken into consideration when suggesting preventive measures in adult high caries risk patients. Somewhat higher fluoride concentration was found in ice teas. One product showed the value of 0,7 ppm. This concentration is close to the value recommended in caries prevention (1 ppm or 1 mg/L). Similar concentrations were found in some carbonated soft drinks of fruit flavor and some mineral waters and (0,7-0,9 ppm) (31). Fresh made tea or ice tea can have the concentration of fluorides from 0,5-4 mg/l, and the concentration is dependent on the place of growth of tea plants and the dipping time of tea leaves (32,33). The number of reports on fluoride content in foods and beverages increased in the last few decades, as the reported increase in the prevalence of dental fluorosis together with the reduction in caries prevalence had been related to the community water fluoridation and fluoridated therapeutic products usage (3, 34). It was noticed that at the level of fluorides in drinking water of 1 ppm, 50% of the subjects exhibited mild flourosis. It was also notices that the degree of fluorosis is directly dependent on the fluoride usage (29). Therefore, in order to theoretically organize and implement effective caries preventive measures in a certain community, it is important to have a detailed knowledge about the ways of fluoride intake and its quantity, in order get optimal 15

caries preventive effect of fluoride and avoid undesired conditions such as dental fluorosis (2,34). The results of this study give information about the fluoride sources in different beverages. Together with the additional studies on fluoride intake by other sources, they can be used in planning and implementing caries preventive measures including fluoride supplements in this Northern Croatian town

1. Petersen PE. The World Oral Health Report 2003: continuous improvement of oral health in the 21st century the approach of the WHO Global Oral Health Program. Community Dent Oral Epidemiol. 2003;31 Suppl 1:3-23. 2. Jones S, Burt BA, Petersen PE, Lennon MA. The effective use of fluorides in public health. Bulletin of the World Health Organization. 2005; 83 (9): 670-676. 3. Jackson RD, Brizendine EJ, Hinesley R, Stookey GK, Dunipace AJ. The fluoride content of foods and beverages from negligibly and optimally fluoridated communities. Community Dent Oral Epidemiol. 2002; 30(5): 38291. 4. Martinez-Mier EA, Soto-Rojas AE, Urena-Cirett JL, Stookey GK, Dunipace AJ. Fluoride intake from foods, beverages and dentifrice by children in Mexico. Community Dent Oral Epidemiol. 2003; 31(3): 221-30. 5. Pagliari AV, Moimaz Saliba SA, Saliba O, Botazzo delben AC, Sassaki KT. Analysis of fluoride concentrations in mother's milk substituites. Braz Oral Res. 2006; 20(3): 269-74. 6. Nagpal DI, Damle SG. Comparison of salivary fluoride leveles following use of dentifrices containing different concentrations of fluoride. J Indian Soc Pedod Prev Dent. 2007; 25(1): 20-2. 7. Tomi D, Linir I. Farmakologija za stomatologe. Zagreb: Sveuilina naklada Liber, 1985. 8. Camargo JA. Comparing levels of pollutants in regulated rivers with safe concentrations of pollutants for fishes: a case study. Chemosphere. 1996; 33(1): 81-90.

16

9. Skjelkvale BL. Water chemistry in areas with high deposition of fluoride. Sci Total Environ. 1994; 152(2): 105-12. 10. Zingde MD, Mandalia AV. Study of fluoride in polluted and unpolluted estuarine environments. Estaur Coast Shelf Sci. 1988; 27(6): 707-12. 11. Fuge R, Andrews MJ. Fluorine in the UK environment. Environ Geochem Health. 1988; 10(3,4): 96-104. 12. Lopez H, Navia JM. A method to assay fluoride in foods, beverages and diets. Caries Res. 1988; 22(4): 2106. 13. Juri H, Klari T, agar M, Bukovi D Jr., Jankovi B, palj S. Incidence of caries in children of rural and subrural areas in Croatia. Coll Antropol. 2008; 32 (1): 131-6. 14. Urek mm, Uhac I, Mihaljevic ZV, Leovic D, Blecic N, Kovac Z. Oral health status in war veterans with post-traumatic stress disorder. J Oral Rehabil. 2007;34: 18 15. Kalauz A, Prpi-Mehii G, Katanec D. Razlozi za ekstrakcije zuba: ogledna studija. Acat Stom Croat. 2009; 43(2): 110-6. 16. Campbell AD. Determination of fluoride in various matrices. Pure & Apll Chem. 1987; 695(5): 695-702. 17. Heilman J, Kiritsy M, Levy S, Wefel J. Assessing fluoride contetnt level of carbonated soft drinks. Am J Dent Assoc. 1999; 130(11): 1593-9. 18. Community Dent Oral Epidemiol 2002; 30: 38291 19. Bagramian RA, Garcia-Godoy F, Volpe AR. The global increase in dental caries. A pending public health crisis. Am J Dent. 2009; 22(1): 3-8. 20. The world oral health report 2003. Geneva: WHO; 2003. Available from: HYPERLINK "http://www.who.int/oral_health" 21. Kraljevic SS, Boras VV, Panduric J, Zilic IA. Oral health among institutionalised elderly in Zagreb, Croatia. Gerodontology 2005; 22; 238241. 22. Cochrane NJ, Saranathan S, Morgan MV, Daspher SG. Fluoride content of still bottled water in Australia. Austr Dent J. 2006; 51(3): 242-4. 23. Weinberger SJ. Bottled drinking waters: are the fluoride concentrations shown on the labels accurate? Int Paediatr Dent. 1991; 1(3): 143-6. 24. Johnson SA, DeBaiase C. Concentration levels of fluoride in bottled drinking water. J Dent Hyg. 2003; 77(3): 161-7. 17

25. Dadi . Korelacija izmeu sadraja fluorida u vodama Hrvatske i rairenosti karijesa [dissertation]. Zagreb: Stomatoloki fakultet Sveuilita u Zagrebu; 2000. 26. Carvalho J C, Figueiredo MJ, Vieira EO, Mestrinho HD. Caries trends in Brazilian non-privileged preschool children in 1996 and 2006. Caries Res. 2009; 43(1): 2-9. 27. Moynihan P. The interrelationship between diet and oral health. Review. Proc Nutrit Soc. 2005; 64(4): 571-80. 28. Birkhed D. Sugar content, acidity and effect on plaque pH of fruit juices, fruit drinks, carbonated beverages and sport drinks. Caries Res. 1984; 18(2): 1207. 29. Fejerskov O, Kidd E. Dental caries: The disease and its clinical menagment. 2nd ed. New York: Willey Blackwell; 2008. 30. Jimanez-Farfani MD, Hernandez-Guerrero, Loyola-Rodrigez JP, LedesmaMontes. Fluoride content in bottled waters, juices and carbonated soft drinks in Mexico City, Mexeico. Int J Paed Dent. 2004; 14(4): 260-6. 31. Clovis J, Hargreaves JA. Fluoride intake from beverage consumption. Community Dent Oral Epidemiol. 1988; 16(1): 11-5. 32. Emekli-Alturfan E, Yarat A, Akyuz S. Fluoride levels in various black tea, herbal and fruit infusions consumed in Turkey. Food Chem Toxicol. 2009; 47(7): 1495-8. 33. Hayacibara MF, Queiroz CS, Tabchoury CP, Cury JA. Fluoride and aluminum in teas and tea-based beverages. Rev Saude Publica. 2004 Feb; 38(1): 100-5. 34. Machiulskiene V, Baelum V, Fejerskov O,Nyvad B. Prevalence and extent of dental caries, dental fluorosis, and developmental enamel defects in Lithuanian teenage populations with different fluoride exposures. Eur J Oral Sci. 2009; 117(2): 154-60.

18