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Advances in Science & Research Open Access Proceedings icsinPpr|Dsuso ae icsinPpr|Dsuso ae | Paper Discussion | Paper Discussion | Paper Discussion | Paper Discussion Drink. Water Eng. Sci. Discuss.,Drinking 5, 495–514, 2012 Water Drinking Water www.drink-water-eng-sci-discuss.net/5/495/2012/ DWESD doi:10.5194/dwesd-5-495-2012 Engineering and Science Engineering and Science © Author(s) 2012. CC Attribution 3.0 License. 5, 495–514, 2012 Open Access Access Open Discussions

This discussion paper is/has been under review for the journal Drinking Water Engineering and Fluoride in the

Science (DWES). Please refer to the corresponding final paper in DWES if available. Discussions Earth System Earth System drinking water of Science Science M. A. Tahir and H. Rasheed Open Access Open Fluoride in theAccess Open Data drinking water ofData Pakistan and the possible risk of crippling fluorosis Title Page

Abstract Introduction M. A. Tahir and H. Rasheed Conclusions References Pakistan Council of Research in Water Resources, Kheyaban-e-Johar, H-8/1, , Pakistan Tables Figures Received: 3 February 2012 – Accepted: 7 February 2012 – Published: 7 September 2012 Correspondence to: M. A. Tahir ([email protected]) J I

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495 icsinPpr|Dsuso ae icsinPpr|Dsuso ae | Paper Discussion | Paper Discussion | Paper Discussion | Paper Discussion Abstract DWESD To explore the possibility of fluoride toxicity, seven hundred and forty seven (747) wa- ter samples were collected from surface and ground water sources of sixteen major 5, 495–514, 2012 cities of Pakistan, adopting a uniform sampling design with distribution of samples 5 as: (79), (46), (30), Khushab (50), (51), Fluoride in the (30), (53), (60), (60), (55), (38), drinking water of Risalpur (35), (81), Ziarat (21), Loralai (21), Mastung (37). The comparison of Pakistan analytical findings with WHO Guidelines of Drinking Water for Fluoride (i.e. 1.5 ppm) has concluded that 16 % of the monitored water sources have fluoride concentration M. A. Tahir and −1 10 beyond the permissible, safe limit of 1.5 mg l , falling in the concentration range of 1.6– H. Rasheed 25 mg l−1. The highest fluoride contamination (22 %) has been detected in the Balochis- tan province followed by 19 % in Punjab province. Comparatively higher fluoride levels of >20 % in groundwater sources such as hand pumps has supported the possibil- Title Page

ity of increased ground water contamination, as excessive fluoride concentrations are Abstract Introduction 15 expected to come from calcium-poor aquifers and from areas where fluoride-bearing minerals are common or where cation exchange of sodium for calcium occurs. Field Conclusions References observations have also indicated the prevalence of fluoride-associated health implica- Tables Figures tions in the study areas with excessive fluoride in water sources. The findings in this study have provided a bidirectional vision for epidemiological investigations as well as J I 20 for mitigating the issues in the affected vicinities of fluoride-rich areas.

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3 Per capita water availability in Pakistan has decreased from 5000 m per annum in Full Screen / Esc 1951 to 1100, which is just above the internationally recognized scarcity rate. It is pro- 3 jected that water availability will be less than 700 m per capita by 2025 (Pak-SCEA, Printer-friendly Version 25 2006). Recent estimations of the availability and use of groundwater of an acceptable quality have also indicated the heavy over-exploitation of water resources, resulting in Interactive Discussion 496 icsinPpr|Dsuso ae icsinPpr|Dsuso ae | Paper Discussion | Paper Discussion | Paper Discussion | Paper Discussion the deteriorated quality as well as quantity of the groundwater (Pakistan Water Part- nership, 2000). Findings of several studies conducted in the country to obtain an exact DWESD evaluation of the drinking water quality have disclosed the presence of a few potentially 5, 495–514, 2012 toxic substances in the groundwater with a higher concentration accelerated by human 5 activities. The major reasons for poor water quality may be the untreated disposal of municipal and industrial effluents and the excessive use of fertilizers and insecticides. Fluoride in the In addition, of the total diseases prevalent in the country, 40 % are water borne and drinking water of 20–40 % of hospitalizations are due to such water borne diseases (PCRWR, 2008). Pakistan Therefore, considering the demand of the time, the Pakistan Council of Research in M. A. Tahir and 10 Water Resources (PCRWR) launched a National Water Quality Monitoring Programme (2001–2006) in the country and the findings of this mega water quality monitoring pro- H. Rasheed gram for 23 major cities of Pakistan has revealed the prevalence of four major water quality tribulations, such as bacteriological contamination (68 %), arsenic (24 %), nitrate Title Page (13 %) and fluoride (5 %), in the surface or groundwater sources of Pakistan, specifi- 15 cally in the cities Kasur, Loralai, Quetta, Bahawalpur, Karachi, Faisalabad and Ziarat Abstract Introduction (Kahlown et al., 2001). Fluoride is an important water quality parameter and has beneficial effects on the Conclusions References

teeth at low concentrations in drinking-water. However, excessive exposure to fluoride Tables Figures in drinking-water or in combination with exposure to fluoride from other sources, can 20 give rise to a number of adverse effects which may range from mild dental fluoro- J I sis to crippling skeletal fluorosis as the level and period of exposure increases. Many countries in the world especially Iraq, Iran, Syria, Turkey, India, Algeria, Morocco, the J I southern parts of the USA and former USSR have also reported higher fluoride con- Back Close centration in their groundwater (Edmunds et al., 1996 and Mangla, 1991). 25 Ali et al. (2002) investigated the presence of fluoride in drinking water of Lahore city Full Screen / Esc and found it to be within safe limits. However, adjoining areas like Mangamandi with higher fluoride concentrations in the water sources have also shown reported health Printer-friendly Version effects in the form of dental and skeletal fluorosis among the natives due to excessive fluoride intake through drinking water (Ali et al., 2002). A similar case was reported in Interactive Discussion

497 icsinPpr|Dsuso ae icsinPpr|Dsuso ae | Paper Discussion | Paper Discussion | Paper Discussion | Paper Discussion the groundwater of Mastung valley in the Kalat division of Balochistan Province (K. Ali, unpublished data, 1999). DWESD Considering the potential toxicity of higher fluoride concentration appearing as dental 5, 495–514, 2012 or skeletal fluorosis, the Pakistan Council of Research in Water Resources with finan- 5 cial assistance from United Nation’s Children Education Funds (UNICEF) has carried out a detailed investigation on the prevalence of fluoride in drinking water sources of Fluoride in the sixteen major suspected cities of Pakistan. The main objectives of the study were to drinking water of authenticate the reported levels of fluoride and to review the possible associated health Pakistan implications to be disseminated to implementing agencies in order to provide guidelines M. A. Tahir and 10 to the affected communities for locating alternate safe water sources. H. Rasheed

2 Materials and methods Title Page Seven hundred and forty seven (747) water samples were collected from various sur- face or groundwater sources such as hand pumps, tube wells, wells, nullahs, springs, Abstract Introduction

dams, bores, and the water supply of sixteen major cities of the country on the basis Conclusions References 2 2 2 15 of a grid size of 0.25 km for small cities, 9 km for medium cities, and 16 km for big cities as given in Table 1. Tables Figures Following the grids on the city maps, one sample per grid was taken maintaining a distance of 0.5 or 1 km between two monitoring points. Replicating every fifth sample for J I quality control purposes, 298 samples were collected additionally to check the reliability J I 20 and accuracy of the sampling and analytical procedures. Following the Standard Methods, all the samples were collected in 1/2 liter Back Close polystyrene bottles and transported to laboratory in the least possible time (APHA- AWWA-WEF, 1992). Field information regarding sampling was recorded on the sam- Full Screen / Esc pling proforma. All the samples were analyzed for fluoride (mg l−1) using the SPANDS 25 method recommended by Standard Methods based on the comparatively higher sen- Printer-friendly Version sitivity and efficiency of the method (APHA-AWWA-WEF, 1992). A sample of blank, Interactive Discussion known fluoride standard and previously analyzed sample were analyzed after every 498 icsinPpr|Dsuso ae icsinPpr|Dsuso ae | Paper Discussion | Paper Discussion | Paper Discussion | Paper Discussion ten samples to check the reproducibility of method and their results were found in the range of ±5 % deviation from the actual analysis. DWESD 5, 495–514, 2012 3 Results and discussion Fluoride in the Analytical findings were compared with WHO Drinking Water Guideline value for flu- drinking water of 5 oride which also considers the impact of climatic conditions, volume of water intake Pakistan as well as fluoride intake from other sources (WHO, 2004). Thus, considering the an- ◦ nual average of maximum daily air temperature (84 F) of Pakistan, the WHO guideline M. A. Tahir and −1 value for fluoride in the drinking water of Pakistan is considered as 1.5 mg l . The city- H. Rasheed wise status of fluoride as a percentage of contamination out of total monitored sites of 10 each city, is graphically reflected in Fig. 1. Mianawali city has shown the highest con- tamination level of 37 % in Punjab province, Mirpur Khas city (3.6 %) in Province, Title Page Quetta city (14 %) in Balochistan Province and Risalpur city (11 %) in North-West Fron- tier Province (NWFP). Abstract Introduction

Overall, only 16 % of the total 747 samples were found to be unsafe, whereas the Conclusions References 15 remaining 84 % were declared to be safe. This overall distribution of Fluoride for 747 locations monitored in the selected 16 cities is shown as Fig. 2. Tables Figures Table 2 provides details of quantitative summaries of each water quality variable, namely the minimum, maximum, median (middle value of the ordered data), mean, J I the first and third quartiles, Q1 and Q3 respectively (which are the 25th and 75th per- J I 20 centile values of the ordered data), the total number of observations recorded (Count). Comparing means and medians, we see that the means of Fluoride are substantially Back Close greater than their medians (except for Jhelum city). The distributions of the data for these variables are highly skewed to the right. Full Screen / Esc An overall comparison of four provinces indicated a higher percentage contamination 25 in Balochistan Province followed by Punjab Province. The province-wise distribution is Printer-friendly Version also given in Figs. 3–6 to provide an idea of the range of fluoride concentration within Interactive Discussion each province. 499 icsinPpr|Dsuso ae icsinPpr|Dsuso ae | Paper Discussion | Paper Discussion | Paper Discussion | Paper Discussion The results of this perspective survey have finally led to recognition of the fact that fluoride is a considerable issue in quite a few places in Pakistan. Observations of the DWESD sampling team have also disclosed the possible signs and symptoms including Skeletal 5, 495–514, 2012 and Dental Fluorosis among the few individuals of the communities associated most 5 probably to the excessive fluoride level in their drinking water. In the same way, deaths of the native people at locations with excessive fluoride due to an unknown chronic Fluoride in the disease symptomized by bone and joint deformities have also been reported by teams drinking water of of the World Health Organization (WHO) and other NGOs in the year 2000. Experts Pakistan found prominent signs of “Dental Fluorosis” in the native areas, where the possibility M. A. Tahir and 10 of chronic fluoride toxicity was confirmed further by the epidemiological and laboratory investigation into the problem areas by a joint team of Pakistan Council of Research H. Rasheed in Water Resources (PCRWR), World Health Organization (WHO), National Institute of Health (NIH), Federal Ministry of Health and Sindh Provincial Health Department in the Title Page year 2005. 15 Fluoride is likely to produce Crippling Skeletal Fluorosis leading to Osteosclerosis, Abstract Introduction Ligamentous and Tendinous Calcification, hypersensitivity and other immunological ef- fects (USNRC, 1993). In addition, fluoride has an effect on the kidneys, muscular and Conclusions References

nervous system and there are some reports about the relationship between erythro- Tables Figures cyte abnormalities and serum fluoride levels with excessive fluoride intake and there- 20 fore leading to death after prolonged illness. Prolonged exposure to 10–20 mg fluo- J I ride/person/day for 10–20 yr can lead to Crippling Skeletal Fluorosis, leading to Os- teosclerosis, Ligamentous and Tendinous Calcification and extreme boney deformities J I (USNRC, 1993). Health impacts from long-term use of various ranges of fluoridated Back Close water have been summarized in Table 3. 25 Fluoride in drinking water increases the risk of hip fractures in women, as evidence Full Screen / Esc has suggested that fluoride may be associated with some gender- dependent mecha- nisms or risk factors for hip fractures (Kurttio et al., 1999). A large number of epidemi- Printer-friendly Version ological studies showed that fluoride is carcinogenic, a bone seeker and is associated with hip fractures and brittle bones (Yelena et al., 2001). It has also been found that Interactive Discussion

500 icsinPpr|Dsuso ae icsinPpr|Dsuso ae | Paper Discussion | Paper Discussion | Paper Discussion | Paper Discussion the crippling malady of fluorosis not only affects the bones and teeth, but every tis- sue and organ of the body, leading to death after prolonged illness (Susheela et al., DWESD 2001). USNRC has concluded that fluoride is likely to produce hypersensitivity and 5, 495–514, 2012 other immunological effects. Fluoride is mainly excreted from the kidneys (USNRC, 5 1993). Thus, it is reasonable that those with impaired renal function might be at greater risk of fluoride toxicity than others. However, there is much evidence that the amount of Fluoride in the fluoride absorbed and retained by the body is mainly dependent on nutrition, especially drinking water of for children. The study mentioned has clearly indicated that most of the water sources Pakistan of the sixteen cities of the country are found free of the presence of excessive fluoride M. A. Tahir and 10 and therefore from the possibility of potential fluoride toxicity. In total, 16 locations have a fluoride level of >10 mg l−1, which is suspected to cause cases of crippling fluorosis H. Rasheed and needs detailed epidemiological study. The analytical findings of Balochistan and Punjab Provinces give rise to the prediction that fluoride is more commonly found in the Title Page groundwater as depicted graphically in Fig. 7. However, detailed monitoring of the con- 15 taminated regions and surroundings are highly recommended to formulate a mitigation Abstract Introduction strategy. Most of the fluoride found in groundwater is naturally occurring from the breakdown Conclusions References

of rocks and soils or weathering and deposition of atmospheric volcanic particles. Flu- Tables Figures oride can also come from runoff and infiltration of chemical fertilizers in agricultural ar- 20 eas, septic and sewage treatment system discharges and liquid waste from industrial J I sources. Pakistan is an agricultural country and 96 % of its total water resources are being used by the agricultural sector, Fertilizer consumption has increased threefold J I during the past 30 yr in the country. It reached one million nutrient tonnes in 1980– Back Close 1981, two million tonnes in 1992–1993 and three million tonnes in 2002–2003 and 25 thus, may be an important contributing factor to increased fluoride contamination (FAO, Full Screen / Esc 2007). Moreover, fluorides are found at significant levels in a wide variety of minerals, including fluorspar, rock phosphate, cryolite, apatite, mica, hornblende and others (Mur- Printer-friendly Version ray, 1986). Fluorite (CaF2) is a common fluoride mineral of low solubility occurring in both igneous and sedimentary rocks. Rock phosphates are converted into phosphate Interactive Discussion

501 icsinPpr|Dsuso ae icsinPpr|Dsuso ae | Paper Discussion | Paper Discussion | Paper Discussion | Paper Discussion fertilizers by the removal of up to 4.2 per cent fluoride (Murray, 1986). In ground wa- ters, however, low or high concentrations of fluoride can occur, depending on the na- DWESD ture of the rocks and the occurrence of fluoride-bearing minerals. Concentrations in 5, 495–514, 2012 water are limited by fluorite solubility, so that in the presence of 40 mg l−1 calcium, it −1 5 should be limited to 3.1 mg l (Hem, 1989). Balochistan Province of Pakistan is rich in mineral deposits and diverse mineralogy and in this region, higher fluoride concen- Fluoride in the trations may therefore be expected in groundwater from calcium-poor aquifers and in drinking water of areas where fluoride-bearing minerals are common. Fluoride concentrations may also Pakistan increase in groundwater in which cation exchange of sodium for calcium occurs. High M. A. Tahir and 10 groundwater fluoride concentrations associated with igneous and metamorphic rocks such as granites and gneisses have been reported from India, Pakistan, West Africa, H. Rasheed Thailand, China, Sri Lanka, and Southern Africa. In China, endemic fluorosis has been reported in all 28 provinces, autonomous regions and municipalities except Shanghai. Title Page Both shallow and deeper ground water are affected; in general the deeper ground wa- 15 ters have the higher concentrations. To cover up the gaps, institutional arrangements, Abstract Introduction capacity- building efforts, legislations and policy development with reference to water quality monitoring and surveillance activities as well as diagnosis and management of Conclusions References

water related diseases are highly required to be managed in order to resolve water Tables Figures quality problems such as excessive fluoride and its possible health implications.

20 Acknowledgements. We would like to gratefully acknowledge the contributions of the technical J I and non-technical staff of the National Water Quality Laboratory, PCRWR, who were involved in sampling, laboratory analysis and coordination. The authors are grateful to Muhammad El- J I Feteh and Tameez Ahmad from the WES Programme, UNICEF Pakistan, for financial assis- Back Close tance for this study. Full Screen / Esc

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502 icsinPpr|Dsuso ae icsinPpr|Dsuso ae | Paper Discussion | Paper Discussion | Paper Discussion | Paper Discussion References DWESD Ali, A. K., Whelton, H., and O’Mullane, D.: A map of natural fluoride in drinking water in Pakistan, Internat. Dent. J., 52, 291–297, 2002. 5, 495–514, 2012 APHA-AWWA-WEF: Standard methods for the examination of water and wastewater, Amer- 5 ican public health association, American water works association and water environment federation, 18th Edn., Washington, DC, 1–33:4–82, 1992. Fluoride in the Edmunds, W. M. and Smedley, P. L.: Groundwater geochemistry and health: an overview, in: drinking water of Environmental geochemistry and health, edited by: Appleton, J. D., Fuge, R., and McCall, G. Pakistan J. H., Geological society special publication No. 113, 91–105, 1996. 10 FAO: The Fertilizer sector, in: FAO corporate document repository, http://www.fao.org/docrep/ M. A. Tahir and 007/y5460e/y5460e07.htm#TopOfPage, last access: 15 December 2004, 2007. H. Rasheed Hem, J. D.: Study and interpretation of the chemical characteristics of natural water, Water Supply Paper 2254, 3rd Edn., US Geological Survey, Washington, D.C., 263 pp., 1989. Kahlown, M. A., Tahir, M. A., and Hifza, R.: Water Quality Status of Pakistan, Pakistan Council Title Page 15 of Research in Water Resources, Islamabad, Pakistan, Technical report Series 121-2006, 79–80, 2001. Abstract Introduction Kurttio, P. N., Gustavsson, N., Vartiainen, T., and Pekkanen, J.: Exposure to natural fluoride in well water and hip fracture: A cohort analysis in Finland, Am. J. Epidemiol., 150, 817–824, Conclusions References 1999. Tables Figures 20 Mangla, B: India’s dentists squeeze fluoride warnings off tubes, New Scientist, 131, p. 16, 1991. Murray, J. J.: Appropriate use of fluorides for human health, World Health Organization, Geneva, 1986. J I Pak-SCEA: Pakistan; Strategic country environmental assessment report: Rising to the chal- lenges, South Asian Development and Social Development Unit, the World Bank, 50 pp., J I 25 2006. Pakistan Water Partnership: Framework for action for achieving the Pakistan water vision 2025, Back Close Islamabad, 2000. Full Screen / Esc Susheela, A. K., Das, T. K., Gupta, I. P., Tandon, R. K., Kacker, S. K., Ghosh, P., and Deka, R. C.: Fluoride ingestion and its correlation with gastro-intestinal discomfort, Journal Fluoride, 30 25, 7–12, 1992. Printer-friendly Version

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503 icsinPpr|Dsuso ae icsinPpr|Dsuso ae | Paper Discussion | Paper Discussion | Paper Discussion | Paper Discussion The Network for Consumer Protection in Pakistan and Action-aid Pakistan: Drinking water is- sues in Pakistan. A seminar on Drinking Water Issues in Pakistan 9th December 2003, Is- DWESD lamabad, Pakistan, 2002. USNRC: US National Research Council, Health effects of Ingested fluoride, National academy 5, 495–514, 2012 5 press, Washington, D.C., 1993. WHO: World Health Organization, Guideline for Drinking-Water Quality, second Edn., Vol. 2, Health criteria and other supporting information, World Health Organization, Geneva, 2004. Fluoride in the Yelena, V., Marina, T., Viktor, A., and Rein, M.: Fluoride in drinking water, Tallinn Technical drinking water of University, Estonia, 2001. Pakistan

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Table 1. Sampling criteria and number of samples collected from four provinces of the country. Fluoride in the

2 drinking water of Sr. No. Province City Grid Size (km ) No. of Sample Pakistan 1 Punjab Lahore 3 79 Kasur 0.5 46 M. A. Tahir and Faisalabad 3 30 H. Rasheed Khushab 0.5 50 Chakwal 0.5 51 Mianwali 0.5 30 Title Page Jhelum 0.5 53 Bahawalpur 3 60 Abstract Introduction

2 Sindh Karachi 4 60 Conclusions References Mirpur Khas 0.5 55 3 North West Frontier Peshawar 3 38 Tables Figures Province (NWFP) Risalpur 0.5 35 4 Balochistan Quetta 1.5 81 J I Ziarat 0.5 21 J I Loralai 0.5 21 Mastung 0.5 37 Back Close

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Fluoride in the Table 2. Basic statistics of fluoride in water sources of 16 cities. drinking water of Pakistan Sr. No. Cities Count Mean SD Min Q1 Median Q3 Max M. A. Tahir and 1 Chakwal 51 1.02 0.60 0.00 0.59 0.76 1.49 2.63 H. Rasheed 2 Bahawalpur 60 0.67 0.67 0.15 0.30 0.53 0.74 4.58 3 Karachi 60 0.48 0.44 0.05 0.17 0.43 0.54 2.77 4 Mirpur Khas 55 0.74 0.48 0.00 0.28 0.81 1.06 1.80 5 Khushab 50 1.09 1.10 0.04 0.16 1.05 1.50 4.78 Title Page 6 Mianwali 30 1.37 0.47 0.08 1.06 1.36 1.77 2.14 7 Kasur 46 1.11 0.84 0.35 0.54 0.81 1.47 4.10 Abstract Introduction 8 Faisalabad 30 0.89 0.97 0.04 0.36 0.79 1.00 5.16 Conclusions References 9 Lahore 79 2.62 4.46 0.05 0.26 0.51 1.76 19.70 10 Quetta 81 2.47 4.23 0.03 0.45 0.94 2.11 24.48 Tables Figures 11 Ziarat 21 0.39 0.33 0.01 0.14 0.34 0.47 1.51 12 Loralai 21 1.08 0.38 0.08 0.88 1.04 1.18 1.86 13 Mastung 37 1.13 0.41 0.63 0.82 1.08 1.35 2.27 J I 14 Jhelum 53 0.37 0.18 0.05 0.16 0.41 0.50 0.64 15 Peshawar 38 0.29 0.29 0.05 0.10 0.15 0.40 1.10 J I 16 Risalpur 35 1.27 0.27 0.78 1.12 1.30 1.42 2.09 Back Close

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Fluoride in the drinking water of Pakistan

M. A. Tahir and H. Rasheed

Table 3. Health impacts from long-term use of various ranges of fluoridated water.

Title Page <0.5 mg l−1 Dental caries 0.5–1.5 mg l−1 Promotes dental health Abstract Introduction 1.5–4 mg l−1 Dental fluorosis Conclusions References > 4 mg l−1 Dental, skeletal fluorosis −1 > 10 mg l Crippling fluorosis Tables Figures

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507 Following the Standard Methods, all the samples were collected in ½ liter polystyrene bottles and transported to laboratory in least possible time [8]. Field information regarding sampling was recorded on the sampling proforma. All the samples were analyzed for fluoride (mg/l) using SPANDS method recommended by Standard Methods based on the comparatively higher sensitivity and efficiency of the method [8]. A sample of blank, known fluoride standard and previously analyzed sample were analyzed after every ten samples to check the reproducibility of method and their results were found in the range of ±5% deviation than the actual analysis.

3. Results and Discussion

Analytical findings were compared with WHO Drinking Water Guideline value for fluoride which also considers the impact of climatic conditions, volume of water intake as well as fluoride intake from other sources [9]. Thus, considering the annual average of maximum daily air temperature

(84oF) of Pakistan, WHO guideline value for fluoride in the drinking water of Pakistan is considered as 1.5 mg /l. City-wise status of fluoride as percentage contamination out of total monitored sites of each city, is graphically reflected in Figure-1. Mianawali city has shown a highest contamination level icsinPpr|Dsuso ae icsinPpr|Dsuso ae | Paper Discussion | Paper Discussion | Paper Discussion | Paper Discussion of 37% in Punjab province, Mirpur Khas city (3.6%) in Sindh province, Quetta city (14%) in DWESD Balochistan province and Risalpur city (11%) in North-West Frontier Province (NWFP). 5, 495–514, 2012

Fluoride in the 40 drinking water of 35 Pakistan

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%age Samples exceeding 1.5 mg/l of Fluoride of mg/l 1.5 exceeding Samples %age 0

e r r ab s ar tta rat bad pur wal chi pu a rali ng asu l sh tu K ala ak helum Que Zi Lo Lahor J Kara r Kha shaw Khu Ch Mianwali pu Risala Mas J I Fais ahawa Pe B Mir Cities of Pakistan J I

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508 Figure-1: Distribution of fluoride in sixteen cities of four provinces

In overall, only 16% samples out of total 747 were found to be unsafe whereas; remaining 84% were icsinPpr|Dsuso ae icsinPpr|Dsuso ae | Paper Discussion | Paper Discussion | Paper Discussion | Paper Discussion declared to be safe. This overall distribution of Fluoride for 747 locations monitored in selected 16 DWESD cities is shown as Figure-2. 5, 495–514, 2012

26 25 Fluoride in the 24 23 drinking water of 22 21 Pakistan 20 19 M. A. Tahir and 18 17 H. Rasheed 16 (mg/l) 15 14 13 Title Page 12 11 10 Abstract Introduction Concentration 9 8 Conclusions References 7

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Fig. 2. VariationFigure-2: of fluoride Variation concentration of fluoride (mgconcen l−1tration) in the (mg/l) monitored in the sites.monitored sites Full Screen / Esc

Table-2 provides details of quantitative summaries of each water quality variable, namely the Printer-friendly Version minimum, maximum, median (middle value of the ordered data), mean, the first and third quartiles, Interactive Discussion Q1 and Q3 respectively (which are the 25th and 75th percentile values of the ordered data), the total number of observations recorded (Count). Compari509ng means and medians, we see that the means of Fluoride are substantially greater than their medians (except for Jhelum city). The distributions of the data for these variables are highly skewed to the right.

Table-2: Basic Statistics of Fluoride in Water Sources of 16 Cities Sr. No. Cities Count Mean SD Min Q1 Median Q3 Max 1 Chakwal 51 1.02 0.60 0.00 0.59 0.76 1.49 2.63 2 Bahawalpur 60 0.67 0.67 0.15 0.30 0.53 0.74 4.58 3 Karachi 60 0.48 0.44 0.05 0.17 0.43 0.54 2.77 4 Mirpur Khas 55 0.74 0.48 0.00 0.28 0.81 1.06 1.80 5 Khushab 50 1.09 1.10 0.04 0.16 1.05 1.50 4.78

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6 Mianwali 30 1.37 0.47 0.08 1.06 1.36 1.77 2.14 7 Kasur 46 1.11 0.84 0.35 0.54 0.81 1.47 4.10 8 Faisalabad 30 0.89 0.97 0.04 0.36 0.79 1.00 5.16 9 Lahore 79 2.62 4.46 0.05 0.26 0.51 1.76 19.70 10 Quetta 81 2.47 4.23 0.03 0.45 0.94 2.11 24.48 11 Ziarat 21 0.39 0.33 0.01 0.14 0.34 0.47 1.51 12 Loralai 21 1.08 0.38 0.08 0.88 1.04 1.18 1.86 13 Mastung 37 1.13 0.41 0.63 0.82 1.08 1.35 2.27 14 Jhelum 53 0.37 0.18 0.05 0.16 0.41 0.50 0.64 15 Peshawar 38 0.29 0.29 0.05 0.10 0.15 0.40 1.10 icsinPpr|Dsuso ae icsinPpr|Dsuso ae | Paper Discussion | Paper Discussion | Paper Discussion | Paper Discussion 16 Risalpur 35 1.27 0.27 0.78 1.12 1.30 1.42 2.09 DWESD An overall comparison of four provinces indicated a higher percentage contamination in Balochistan 5, 495–514, 2012 province followed by Punjab province. The province-wise distribution is also given in Figures 3-6 to provide an idea of range of fluoride concentration within each province. Fluoride in the drinking water of Pakistan Range of Fluoride contaminated samples in Punjab province 25 M. A. Tahir and H. Rasheed 20

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Figure-3: Range of fluoride contaminatedSl samples (>1.5mg/l)−1 in Punjab Province Fig. 3. Range of fluoride contaminated samples (>1.5 mg l ) in Punjab Province. J I

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Fluoride in the drinking water of Range of Fluoride Contamianted Samples in Sindh Province Pakistan 3 M. A. Tahir and 2.5 H. Rasheed 2

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5 Conclusions References Fluoride (mg/l) Fluoride

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J I Fig. 5. RangeFigure-5: of fluoride Range of contaminated fluoride contaminated samples samples (>1.5 mg(>1.5mg l−1)/l) in in Balochistan Balochistan Province Province. Back Close

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Interactive Discussion

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DWESD 5, 495–514, 2012

Fluoride in the drinking water of Range of Fluoride Contaminated Samples in NWFP Pakistan 2.5 M. A. Tahir and 2 H. Rasheed

1.5 Title Page 1 Abstract Introduction 0.5 Fluoride (mg/l) Conclusions References

0 Tables Figures 01234

Samples J I

Fig. 6. Range ofFigure-6: fluoride contaminatedRange of fluoride samples contamin (ated>1.5 samples mg l−1 (>1.5mg/l)) in NWFP. in NWFP J I The results of this perspective survey have finally led to recognition of the fact that fluoride is a Back Close

considerable issue in few places of Pakistan. Observations of the sampling team have also disclosed Full Screen / Esc

the possible signs and symptoms including Skeletal and Dental Fluorosis among the few individuals Printer-friendly Version of the communities associated most probably to the excessive fluoride level in their drinking water. In Interactive Discussion the same way, deaths of the native people at locations with excessive fluoride due to an unknown 513 chronic disease symptomized by bone and joint deformities have also been reported by teams of

World Health Organizations (WHO) and other NGOs in the year 2000. Experts found prominent signs

of “Dental Fluorosis” in the native areas, where the possibility of chronic fluoride toxicity was

confirmed further by the epidemiological and laboratory investigation in the problem areas by a joint

team of Pakistan Council of Research in Water Resources (PCRWR), World Health Organizations

(WHO), National Institute of Health (NIH), Federal Ministry of Health and Sindh Provincial Health

Department in the year 2005.

Fluoride is unlikely to produce Crippling Skeletal Fluorosis leading to Osteosclerosis, Ligamentous

and Tendinous Calcification, hypersensitivity and other immunological effects [10]. In addition,

fluoride has an effect on the kidneys, muscular and nervous system and there are some reports about

the relationship between erythrocyte abnormalities and serum fluoride levels with excessive fluoride

intake and therefore leading to death after prolonged illness. Prolonged exposure to 10-20 mg

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DWESD 5, 495–514, 2012

Fluoride in the 25 drinking water of Pakistan 20 M. A. Tahir and H. Rasheed 15

Title Page 10 Abstract Introduction

5 Conclusions References

Tables Figures %age samples exceeding 1.5 mg/L 1.5 Fluoride exceeding samples %age 0 Hand Pum p Dug We ll Tube We ll Sur face Karez Spring Dam Rivers water J I supplies Types of water sources monitored J I

Back Close Fig. 7. DistributionFigure-7: of fluoride Distribution in surface of fluoride and in groundwater surface and groundwater sources. sources Full Screen / Esc

Most of the fluoride found in groundwater is naturally occurring from the breakdown of rocks and Printer-friendly Version

soils or weathering and deposition of atmospheric volcanic particles. Fluoride can also come from Interactive Discussion

runoff and infiltration of chemical fertilizers in agricultural areas, septic and sewage treatment system 514 discharges and liquid waste from industrial sources. Pakistan is an agricultural country and 96% of its

total water resources are being used by agriculture sector, Fertilizer consumption has increased

threefold during the past 30 years in the country. It reached one million nutrient tonnes in 1980-81,

two million tonnes in 1992-93 and three million tonnes in 2002-03 and thus may be an important

contributing factor of increased Fluoride contamination [14]. Moreover, fluorides are found at

significant levels in a wide variety of minerals, including fluorspar, rock phosphate, cryolite, apatite,

mica, hornblende and others [15]. Fluorite (CaF2) is a common fluoride mineral of low solubility

occurring in both igneous and sedimentary rocks. Rock phosphates are converted into phosphate

fertilizers by the removal of up to 4.2 per cent fluoride [15]. In ground waters, however, low or high

concentrations of fluoride can occur, depending on the nature of the rocks and the occurrence of

fluoride-bearing minerals. Concentrations in water are limited by fluorite solubility, so that in the

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