The appraisal of groundwater specific vulnerability is a global challenge. The high concentration of nitrate in drinking water has detrimental effects on human health. Poor sanitary facilities, excessive use of nitrogen fertilizers, urbanization and industrialization are concerns in groundwater management in recent decades. For this work, samples were collected from hand pump, located along the course of the Subarnarekha River in Jharkhand, India. Collected samples were analysed in laboratory to determine groundwater nitrate concentration of the selected study area and to identify the factors which control the distribution and fluctuation in different hydrological connectivity. Further, analysis of variance (ANOVA) was applied to know the difference in sites. Spatial and temporal variability of nitrate ion in groundwater was observed as 0.4 to 158.6mg/l, 0.2 to 264.6mg/l and 0.2 to 248.7mg/l during the pre-monsoon, monsoon and post-monsoon season, respectively. Agricultural activities are dominant cause of elevated nitrate concentration, and other sources are industries of iron, steel and inorganic chemical (sulphuric acid). Concentration maps were created in SimplexNumerica software for conspicuous visualization of nitrate hot spots. The total area was categorized into safe zone (56%) and unsafe zone (44%). The unsafe zone water is not suitable for direct human consumption.
Nitrate pollution is a serious concern ; it disturbs global water resources due to notable economic and health effects [7, 52, 76, 81]. Recent decades have seen a greater use of nitrogen fertilizers without considering negative effects on soil properties, agriculture yield and agricultural products [49, 50]. It also deteriorates the environment and has dramatically increased environmental pollution. Nitrate has been reported at elevated concentration in groundwater of different parts of the world [1, 8, 17, 35,36,37, 44, 69, 70, 73], and many have identified the cause due to excess uses of chemical fertilizers, animal manure, pesticides [13, 30, 53, 54, 83] for higher agriculture yield  and direct disposal of sewage waste and poor maintenance of sewerage system [17,18,19, 64, 67], industrial and household wastes and urbanization [39, 64, 67, 68].
Nitrate is extremely soluble in water [27, 31, 34, 61], and it can easily migrate to groundwater table through soil by leaching process [15, 47, 50, 61], and there it has high residence time. Nitrate concentration in groundwater depends on the quantity of nitrate added to soil and aquifer’s vulnerability to leaching [3, 43, 56, 72, 80]. Seasonal variations have strong direct relationship with added mineral fertilizers containing high percentage of nitrogen. In last few decades, the trend showed that the excess yield depends on excess input of chemical fertilizers in the field and ultimately enhances the concentration of nitrate in groundwater [50, 51].
In rural and suburban agricultural areas of many states of India, namely Tamil Nadu, Orissa, Jharkhand, Karnataka, Maharashtra, Bihar, Gujarat, Madhya Pradesh and Rajasthan have elevated concentration of nitrate in groundwater . Vulnerability to nitrate pollution depends on factors like rainfall and aquifer depth, and the shallow aquifers are more vulnerable to nitrate pollution compared to deep aquifers . The consumption of water with high concentration of nitrate has potential to cause toxic effects in human and aquatic ecosystems . Children and young livestock are more prone to severe health complications due to consumption of high nitrate containing groundwater . Bureau of Indian Standards  have revised the recommended nitrate level from 100 to 45 mg/l in drinking water because of hazardous in nature. However, the consequence of incessant consumption of high nitrate concentration in water may not physically noticeable as in the case of fluoride and arsenic. The association between nitrate ingestion and cancer is quiet debatable, but nitrosamines that can be formed by the reaction of nitrate with several proteins during digestion are identified to be mutagenic and carcinogenic . Particularly infants are very much sensitive to high concentration of nitrate  and can cause methaemoglobinaemia (blue baby syndrome), gastric, goitre, cancer, metabolic abnormality, birth deformities, hypertension and livestock farming (mouth breathing, muscles tremors, and drooling of saliva) [28, 32, 40, 41, 71].
However, many districts of Jharkhand state have excess iron, lead and arsenic along with fluoride and nitrate concentration in their groundwater. Jharkhand Report  highlights that water quality of shallow hand pumps is of poor quality for consumptive uses. The study area is noticeable for mining and in past few case studies has assessed water quality for drinking and irrigation uses [17, 19]. Jharkhand is one of the leading producers of coal, kyanite, gold, silver, bauxite and feldspar. The tribal population is high in this area, and they are economically poor and do not have adequate potable water. Therefore, the risk to negative health hazards is more to the marginalized local inhabitant. Rural areas have limited water supply network. In rural areas and mining affected areas, mostly tribal and weaker section of society directly consume water without appropriate treatment.
This work will be useful as many previous research work in Jharkhand, India, was mostly focused on heavy metals [5, 9, 16, 17, 21,22,23]. Approximately 8% households have access to sanitation in the rural areas, and remaining excreting in the open area in Jharkhand and waste management practices are not very common in majority of rural Jharkhand. The purpose of the work was to determine groundwater nitrate concentration and to identify the factors which control the distribution and fluctuation in different seasons.
Methods and Materials
River Subarnarekha (latitudes of 21°, 33′ N to 23° 32′ N and longitudes of 85° 09′ E to 87° 27′ E) is a river of the south Chotanagpur plateau of Jharkhand state, India (Fig. 1). It originates from the village, Nagri Ranchi (23.4° N, 85.4° E), situated at 756 m above sea level. Its drainage basin includes the states of Jharkhand (catchment area=18,950 km2), West Bengal (catchment area =13,590 km2) and Orissa (catchment area=3200 km2), and it flows into the Bay of Bengal . Soils of the areas are gravel, sandy loams, alluvium and black. In upland areas (reddish and porous) and in the lowlands (heavier and darker), soils are present. The basin is dominated by red soils (>83%) in lower valleys and coastal plains, alluvial deposits are spread over 11%, and remaining 4% of the basin has infertile latosols (mainly laterites) . The area gets average annual precipitation of 1800 mm; the major contribution is from southwest monsoon in the month of June, July, August and September. Climate of area is tropical with warm summer and mild winter. The mean monthly temperature ranges from 40.5 (May) to 9.0°C (December). The highest recorded temperature is 47.2°C and the lowest is 2.8°C (http://indiawris.nrsc.gov.in/wrpinfo/index.php?title=Subernarekha).
General Hydrogeological Description
The lithology of the region includes rocks of the Precambrian and Tertiary ages, and the Quaternary alluvial plains. The Precambrian formations typically cover Jharkhand and West Bengal regions, and Tertiary and alluvial plains cover Orissa. The Precambrian formations mostly consist of gneisses, mica schists, phyllites, dolomites and granites (Fig. 2) and deposits of coal, iron and bauxite ore . Geological formations have ability to store and transmit water.
Only fractured aquifers were recognized, and groundwater occurs under unconfined condition in the hard rock areas, where great number of tube wells, hand pumps and open dug wells occur at depths of 10–50 m, usually penetrating a few metres into the fractured rock . Subarnarekha River is underlain by folded and fractured Precambrian meta-sediments, mostly mica schists, quartzite and hornblende schists , and shows dominant vertical fracturing. The occurrence and storage of groundwater are entirely controlled by its geological setting . In the Subarnarekha River basin, rock formations are broadly classified into two classes, hard and soft rock. The hard rocks are mainly crystalline and consolidated sedimentary, characterized by very tiny primary porosity. Soft rocks characterized by pebble and loose sand have higher degree of primary porosity and as such are characterized by better water storage capacity. Approximately 83% area of the Subarnarekha basin is hard rocks like granite-schists, mica schists, and gabbro, and the remaining 17% of the basin by soft rocks is characterized by Tertiary grits and gravels and Quaternary alluvial sediments.
During pre-monsoon season, dug wells were inventoried to know about water level scenario. Depth to water level varies 6 to 8 metres below ground level (mbgl) Nagri, Ranchi. Water level varies 2 to 4 mbgl in post-monsoon season in Nagri locality. In the lateritic terrain of Nagri areas, water level even goes up to 11 to 12 mbgl. During summer seasons, dug wells become unsustainable for drinking and irrigation purposes (Ground Water Information Booklet Ranchi District, Jharkhand State, 2013). According to Ground Water Year Book Jharkhand 2015–2016, groundwater level fluctuations on seasonal basis are 1.45–13.80 mbgl in pre-monsoon, 0.75–15.60 mbgl in monsoon and 0.97–19.25 mbgl in post-monsoon in the East Singhbhum district. In Ranchi district, it varies 1.52–12.85 mbgl, 0.85–6.55 mbgl and 2.84–11.80 mbgl, in pre-monsoon, monsoon and post-monsoon, respectively.
Agriculture and Crops
East Singhbhum district is mainly rocky. Soil texture varies from zone to zone. The soil is acidic lateritic and red soil (morum) in nature. Soil fertility status is not so bad but water retention capacity is poor. Weather is dry-hot in summer (maximum temperature 48°C recorded) and very cold in winter (minimum temperature 8°C recorded). The area under irrigated farming is found to be approximately 3%. The total area under crop in the zone is approximately 3.70% lakh ha. The principal crops grown in descending order are paddy, vegetables, maize, linseed, Niger, wheat, moong, gram, Kalai, Marua, Bajra and Arhar (http://east-singhbhum.kvk4.in/). In Jharkhand as a whole, average consumption of fertilizer (2012–2013) is 158.22 kg/ha. Out of that, nitrogen consumption is 89.54 kg/ha, phosphate consumption is 60.91 kg/ha, and potash consumption is 7.77 kg/ha (Department of Agriculture and Cooperation, Government of India, New Delhi. Note: * Gross Cropped are 2010-11).
Global Positioning System of Garmin (GPSMAP-76CSX) was used for location readings. At each of 18 locations, samples were collected in the pre-monsoon, monsoon and post-monsoon season in year 2008. Sampling locations were determined based on land use/land cover activities, namely, mining, industrial, agriculture and urban. A great number of tube wells (usually equipped with hand pumps) and open dug well are generally found in the Subarnarekha River basin, with a characteristic depth of about 40–50 m. Small diameter tube wells are usually found. The significant number of wells shows that the area possibly has a well-distributed fracture network . All the samples were collected directly from the hand pump after allowing the water to run for at least 5–7 min so as to steady the variation in physical parameters . One litre sample was collected in high density polyethylene bottle. Millipore membrane filter (0.45 μm) was used for separation of suspended sediments using vacuum pump before storage and laboratory analysis.
Collected groundwater samples were kept at 4°C temperature to prevent any major chemical change . Nitrate concentration was examined by ion chromatograph (Dionex Dx-120) using anions AS12A/AG12 columns coupled to an anion self-regenerating suppressor (ASRS) in recycle mode. After laboratory analysis, samples digital database of nitrate was developed in SimplexNumerica software, and thematic mapping was performed. SimplexNumerica software offers the possibility of structured data management and access. Descriptive statistic was calculated (minimum, maximum, mean, median, standard deviation and standard error). Subsequently, the statistical test analysis of variance (ANOVA) was applied on datasets to know the existing variability within a group and between groups. ANOVA results are reported as Fcritical = Fcalculated with P level and the null hypothesis rejected if Fcalculated>Fcritical.
Descriptive statistics are presented in Table 1. The permissible limit of nitrate as recommended by WHO  is 50mg/l; at ten sampling locations, nitrate concentration was below the prescribed limit of WHO  in all three seasons. Nitrate concentration ranged from 50 to 250 mg/l at six locations (1, 3, 6, 10, 15 and 16) in all the season; diffused source is the main the reason of elevated concentration. The probable sources of nitrate in groundwater are seepage/runoff from fertilized agricultural lands, municipal and industrial waste water, animal feedlots, septic tanks, urban sewerage drainage and decaying plant debris. The natural source as geological formations and route of groundwater flow may also affect nitrate concentration . From spatial distribution map, minimum nitrate concentration was observed at Khuddi Village (in Ranchi) (0.4mg/l), and maximum concentration was 158.6 mg/l at Govindpur location (in Purbi Singhbhum).
The pre-monsoon samples have average concentration as 48.66 mg/l. Total eight locations (44%) have nitrate concentration greater than the WHO  limit of 50 mg/l (Fig. 3). Location no. 6 is near a cemetery, which may contribute to nitrate pollution . Location no. 1 and no. 15 are located in agricultural land where fertilizers are often applied to crops for higher crop yield, and location no. 1 has 88.5 mg/l nitrate. Local farmers are growing vegetable crops, namely, carrot, tomato, green pepper and cucumber, and they apply higher amounts of nitrogen-based fertilizers for higher yield. The growth of urban areas is high in the region, and four locations fall within the urban/residential areas and in new construction sites. The disposal of untreated sewage waste and domestic waste water from urban residential areas has contributed to nitrate ion pollution. Sewage generation in urban areas and treatment capacity available are 1270 million litres per day (mld) and 117.24mld, respectively, in (source: Government of India Ministry of Environment, Forest and Climate Change, Lok Sabha unstarred question no.2541, Updated on 28th May, ).
The pre-monsoon (a) followed by the monsoon (b) and followed by the post-monsoon (c) has the overall order of increasing trend of nitrate (NO3-Post-monsoon> NO3- Monsoon> NO3-Pre-monsoon). This may be true for overall seasonal mean values, but Fig. 3 shows that it is not true at every site. The increasing trend of nitrate concentration in the groundwater of different seasons is governed by interactions of different factors. Spatial distribution maps of nitrate concentration in the pre-monsoon (Fig. 4a), monsoon (Fig. 4b) and post-monsson (Fig. 4c) samples. The minimum and maximum concentration was observed as 0.2 mg/l and 264.60 mg/l with the average value 48.34 mg/l in monsoon season. It was measured as maximum at location no. 6 as 264.60 mg/l in the monsoon, and it is higher as compared to the pre-monsoon season. Nitrate concentration at locations no. 7 and 8 increased greatly with respect to the pre-monsoon and exceed from recommended WHO  limit. Nitrate distribution in groundwater is mainly governed by the source, thickness and composition of the vadose zone, precipitation, irrigation, groundwater flow, aquifer heterogeneity, dissolved oxygen concentrations and electron donor availability and dispersion . Evaporation increases the concentration of nitrate, whereas rainfall leads to dilution of nitrate in soil and lower groundwater concentration . Spatial distribution of the post-monsoon season is expressed in Fig. 4c. The minimum concentration was 0.2 mg/l at Sakchi (in Purbi Singhbhum), and the maximum (248.7 mg/l) was measured at Govindpur (in Purbi Singhbhum) with average value of 48.8 mg/l (Table 1). Elevated nitrate concentration was reported 44% of the total analysed water samples. Sampling locations at Hatia Bridge, Tatanagar, Govindpur, Mushabani, Kandra and Saraikela have concentration >50 mg/l in all three seasons. These regions are dominated by agriculture activities.
Analysis of Variance
The F critical value is given in the one-way ANOVA (Table 2). In this case, the p value is 0.99 and alpha level is 0.05. The p value is larger than alpha so null hypothesis is not rejected. The F value (0.000327) is less than an F critical (3.17); this also means that null hypothesis is not rejected and no significant difference exists. The greater p values suggest that all the results are not significant. Statistical similarity among sites does not mean that all sites have similar kinds of activities. Therefore, it is very challenging to identify the exact source of pollution. Very few sites have high level of nitrate pollution in different seasons. Therefore, these sites have temporal variability in nitrate concentration.
Pearson’s Correlation Analysis
The Pearson’s correlation matrix of the analysed parameters results is presented (Table 3). In general correlation coefficient (r) is classified into three classes as strong (r>0.7), moderate (0.5<r<0.7) and poor (r<0.5). The correlation result shows the interrelation of nitrate with other physicochemical parameters. The pH and F show significant negative correlation with the nitrate, whereas the EC, TDS, Cl, HCO3, SO4, Ca, Mg and Na showed significant positive correlation. The silica and K does not have significantly weak correlation. This suggests that pH has no influence on the release and assimilation of NO3 in studied waters. Further, it indicates that nitrate has specific sources compared to other. The major source of the nitrate concentration in sampled water is generally linked to excess input of chemical fertilizer (NPK) in the agriculture field for high crop yield and weak sewage management system. The maximum nitrate concentration was observed in the Govindpur location where poor hydrological connectivity, nitrification process and poor waste disposal management are dominant reason for enhancing the nitrate enrichment. High porosity and permeability, shallow aquifer and construction of non-cemented septic tanks in rural areas are further deteriorating the groundwater quality.
Principal Component Analysis
Principal component analysis (PCA) helps to identify the hidden factors [65, 66, 82] which control the water chemistry and useful in predicting and establishing the possible sources of pollutant in water, even though it has high subjectivity. The Varimax with Kaiser normalization rotation method was applied to extract the principal components (PCs) loading of different studied ions. Three PCs were extracted (at initial eigenvalue ≥1), and their %cumulative variability was explained at 84.326% (Table 4). PC1 explains 59.907% of the total variance (Table 4). In PC1, the quality parameters, namely, TDS, EC, Ca, NO3, Mg, Cl, SO4, Na and HCO3, identified (Table 5) are mainly responsible for controlling geochemistry of groundwater. The high loading due to TDS, EC, Ca, Mg, Na and Cl attributed to the natural process, whereas high loading due to NO3 and SO4 is articulated to anthropogenic inputs compared to natural processes. Gautam et al.  also reported high nitrate concentrations because of leaching and anthropogenic activities. The high loading of F (0.873) in PC2 which explained 16.652% of the variability and % cumulative variability (73.559%) in the groundwater of study area. The PC 3 has high loading K factor (0.884), and it explained the 10.767% variability and total variability (84.326%). Hence it has been given least preference in regulating groundwater chemistry of the study area. Potassium, an important fertilizer, is strongly held by clay particles in soil. Therefore, leaching of potassium through the soil profile and into groundwater is important only on coarse-textured soils. Potassium is common in many rocks. Many of these rocks are relatively soluble, and potassium concentrations in groundwater increase with time. Important anthropogenic sources of sodium include road salt and animal wastes.
Jharkhand is a rich land of the natural resources. Uranium ore is mined and processed by Uranium Corporation of India Ltd. (UCIL) for use as fuel in the country’s nuclear power reactors through four underground mines, one opencast mine, two processing plants and a by-product recovery plant, all in East Singhbhum district of the State. Jharkhand accounts for about 36% rock phosphate, 28% coal, 26% iron ore (hematite), 30% apatite, 22% andalusite, 18% copper ore and 5% silver ore resources of the country. East Singhbhum region has rich deposits of copper ore. Hindustan Copper Limited (HCL) is situated in the Ghatshila, East Singhbhum district, Jharkhand, which manufactures copper right from the stage of mining to beneficiation, smelting, refining and casting of refined copper metal into downstream saleable products. Ghatshila is best known for the HCL mines because they are Asia’s first copper mines and the world’s second deepest mines. Bihar Sponge Iron Ltd. is the first merchant sponge iron plant in Chandil, Saraikela Kharsawan, and Tata Steel Ltd. is multinational steel-making company in Jamshedpur .
The high concentration of mineral nitrogen in shallow groundwater was found alarming [49, 51]. This may be accounted to leachate generated from landfill site which is affecting the many factors as fertilizer or build-up of soil organic matter and through surface runoff into the subsoil and groundwater [33, 49, 63, 79]. Therefore, it requires control of the fertilizer use and good agricultural practices [38, 55]. Natural sources as soil texture  and precipitations [6, 12, 14, 49, 62, 79] may be significantly influenced the high agricultural nitrate leaching. Hence taking measures is highly recommended to guarantee the better groundwater quality in the vicinity.
It was also observed that the nitrate concentration (the value ranges from 0.2 to 265 mg/l) was very high than the limit prescribed by WHO 50mg/l that indicates that the source of nitrate is not anthropogenic but is geogenic. Most nitrate contamination sources are easily defined, particularly if there is a single known source such as a cattle feed lot, but in some areas, particularly rural locations that have been urbanized, distinguishing between human (anthropogenic) and natural (geogenic) sources is somewhat more complicated. Sources of anthropogenic nitrate contamination to groundwater are septic systems, sanitary sewage effluent releases, domestic animal wastes and home and farm usage of nitrogen fertilizer [49, 68]. Nitrate contamination also occurs from the degradation of cyanide (CN–) an industrial pollutant, particularly common to historic gasworks sites. The geogenic sources include those that are desert-derived such as desert deposits (which also contain natural perchlorate); caliche and Playa Lake evaporate deposits, and desert vadose zone soils. Motzer  reported that naturally occurring vadose zone nitrogen reservoir had the potential to become mobilized, thereby leaching large amounts of nitrate to groundwater.
The primary objective of the study was to assess nitrate pollution in groundwater along a course of the Subarnarekha River and to distinguish the spatio-temporal variability (pre-monsoon, monsoon and post-monsoon seasons), and identification of source, respectively. The results outline that nitrate concentration was found higher at Hatia Bridge, Tatanagar, Govindpur, Mushabani, Kandra and Saraikela region in all three seasons compared to prescribed limit of nitrate in groundwater recommended by the World Health Organization. Water quality of shallow hand pumps is considered poor due to leaching of nitrate. ANOVA shows seasonal variability in nitrate, whereas PCA shows the anthropogenic source of nitrate pollution. The risk arises when the marginalized sections of the society do not have the proper drinking water facility. The area is having higher tribal population; these tribal people are weaker section of the society. Nitrate at higher concentration at these locations requires special treatments of groundwater for nitrate removal before its consumptive and other uses. The average nitrate concentration for all the seasons shows that 56% of observed groundwater samples are safe. The well-pronounced hydrological connectivity and dominant denitrifying biological processes are the main reason of low nitrate concentrations at few sites. The regular monitoring is recommended as essential precautionary step for the unsafe locations to monitor the further degradation of water quality and decline of water level and to create awareness among inhabitants of the region. Groundwater planners, resource manager and local authorities need to install long-term monitoring system and adopt measures of rainwater harvesting to combat the problems more efficiently and effectively.
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All the authors are thankful to two anonymous reviewers and Editor in Chief for their valuable suggestions and recommendations. Also, first author (SKG) is very much grateful to Dr Abhay K Singh and Dr J K Tripathi for providing research facilities and valuable support throughout the research. The SKG is thankful to the CSIR, New Delhi, India, for providing the financial support (09/263 (0703)/2008-EMR-I) and DST N-PDF (File No: PDF/2017/002820) and altogether acknowledges the technical and administrative staff of School of Environmental Sciences for their technical supports.
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Gautam, S.K., Singh, S.K. & Rawat, K.S. Intrinsic Vulnerability Evaluation of Groundwater Nitrate Pollution Along a Course of the Subarnarekha River in Jharkhand, India. Water Conserv Sci Eng (2021). https://doi.org/10.1007/s41101-021-00102-3
- Nitrate pollution
- Subarnarekha River