1 s2.0 S0048969721073095 Main

Science of the Total Environment 810 (2022) 152233
Contents lists available at ScienceDirect
Science of the Total Environment

journal homepage: www.elsevier.com/locate/scitotenv
Review
Global diagnosis of nitrate pollution in groundwater and review of

removal technologies
E. Abascal, L. Gómez-Coma, I. Ortiz, A. Ortiz
⁎
Department of Chemical and Biomolecular Engineering, University of Cantabria, Av. Los Castros 46, 39005 Santander, Spain
H I G H L I G H T S G R A P H I C A L A B S T R A C T
• 272 regions worldwide are analyzed to a

rigorous diagnosis of nitrate pollution.
• Groundwater bodies can be contaminated
by NO− 3 (>50 ppm) along with other
pollutants.
• Agriculture, industry, sewage, septic tanks
& landfills are the main pollution sources.
• The catalytic reduction has high nitrate
conversion (98–100%) and no waste
generation.
• Nowadays, the number of groundwater
treatment plants is still very limited.
A R T I C L E I N F O A B S T R A C T
Article history: Clean water and sanitation for the world population is one of the most important challenges established by the Sustain-
Received 23 September 2021 able Development Goals of the United Nations since worldwide, one in three people do not have access to safe drinking
Received in revised form 3 December 2021 water. Groundwater, one of the main sources of fresh water, has been considerably damaged by human activities. Nev-
Accepted 3 December 2021
ertheless, while numerous plants are globally aimed at removing pollutants from surface waters, a much scarcer num-
Available online 9 December 2021
ber of facilities have focused on groundwater remediation. Nowadays, there is increasing concern about the presence
Editor: José Virgílio Cruz of nitrates (NO− 3 ) in groundwaters as a consequence of the intensive use of fertilizers and other anthropogenic sources,
such as sewage or industrial wastewater discharge. In this context, the selection and development of highly effective
Keywords: and low-cost solutions for the sustainable management of groundwater resources need to be addressed. Thus, this
Groundwater work collects data from the literature regarding the presence of nitrates in groundwater, and, simultaneously, it re-
Nitrates (NO−
3 ) views the main alternatives available to remove NO− 3 from groundwater sources. A total of 292 sites have been ana-
Pollutants lyzed categorized by continents, carefully discussing the possible origins of nitrate pollution. In addition, a
Diagnosis discussion is carried out of the different technologies currently employed to treat groundwater, highlighting the prog-
Water treatments
ress made and the main challenges to be overcome. Finally, the review gathers the data available in the literature for
Removal technologies
nitrate treatment plants at full-scale.
Contents
1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
2. Nitrate sources . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
3. Nitrates in groundwater bodies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
⁎ Corresponding author.
E-mail address: [email protected] (A. Ortiz).
http://dx.doi.org/10.1016/j.scitotenv.2021.152233
0048-9697/© 2021 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.
0/).
E. Abascal et al. Science of the Total Environment 810 (2022) 152233
3.1. Asia . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
3.2. America . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
3.3. Europe . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
3.4. Africa . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
3.5. Summarize of nitrate pollution worldwide. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
4. Alternatives to nitrate removal . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 16
5. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18
CRediT authorship contribution statement . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19
Declaration of competing interest . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 20
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 20
Appendix A. Supplementary data . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 20
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 20
1. Introduction In contrast, the inordinate use of fertilizers and pesticides in agriculture

produces high number of pollutants and water degradation. Thus, fertilizers
The supply of high-quality drinking water constitutes the Sustain- abuse as a source of nutrients and the excessive use of chemicals, such as
able Development Goal (SDG) 6 by 2030 established by United Nations insecticides and antibiotics, increase the pressure exerted on aquatic
General Assembly in 2015 (United Nations, 2016). However, water systems altering their autochthonous fauna and facilitating species in-
bodies are continuously facing a reduction in terms of quality and quan- vasions. In general, fertilizers are composed primarily of nitrogen, phos-
tity. Besides, despite three-quarters of our planet is made up of water, phorus, and potassium compounds, among others, to provide nutrients
only 2.5% is freshwater, distributed as follows: 68.7% in glaciers, to plants and crops. As a result of the agriculture activities, such com-
30.1% groundwater, and just 1.2% is surface water (USGS Water pounds end up in surface water and groundwater bodies, raising the
Science School, 2013). Recent estimations indicate that almost 50% concentration of nitrates in water, which are then returned to the soil
of drinking water and approximately 40% of irrigation water come through irrigation (Andreo-Martínez et al., 2020). In this sense and ac-
from aquifers. Thus, urgent actions are required to slow down the dete- cording to recent studies (Ayers and Westcot, 1985) nitrate concentra-
rioration of water bodies (Díaz-Alcaide and Martínez-Santos, 2019; tions above 22 mg/L (ppm) may affect sensitive crops (i.e. sugar beets
Majkić-Dursun et al., 2019) since, at present, around 66% of the world's or grapes), while other crops, such as maize, remain unaffected by con-
population already suffers from severe water shortages at least one centrations below 132 mg/L. The risk of nitrate leaching is closely re-
month a year (Mekonnen and Hoekstra, 2016). This is mainly due to lated to the excessive use of fertilizers, occurring after or during harvest
the following factors: and within the crop cycle. An elevated concentration may affect the pro-
duction of several crops, which can lead to over-stimulation of growth,
i) An increase in the population growth from 5.3 to 7.7 billion between
delayed maturity or poor quality. Nitrates can affect human health by in-
1990 and 2020, and an expected growth to 9.7 billion by 2050
ducing methemoglobinaemia, thyroid effects or cancer, and irreparable
(United Nations, 2019)
damage in the aquatic system, to the point of provoking fish die-offs
ii) Pollution and degradation of available water resources due to in-
(Martínez et al., 2017; Tokazhanov et al., 2020; World Health
creased industrial activity since the mid-18th century. In fact, this
Organization, 2012).
factor is responsible for human health issues, ecosystem damage
Cost-effective and energy-efficient treatments are necessary for remov-
and impacts on food production, economic activity and develop-
ing nitrates, and therefore, to contribute to achieve the SDG and the quality
ment (Bond et al., 2018), along with the discharge of untreated
standards established by WHO and FAO organizations. This review aims to
wastewater (80% of the total wastewater) (Bond et al., 2018;
collect data relevant to discriminate the quality of groundwater bodies
Daesslé et al., 2020)
worldwide. In addition, the different technologies available so far to re-
iii) Climate change (Bond et al., 2018; Lorite et al., 2018) contributes to
move nitrates are analyzed, emphasizing their advantages and drawbacks.
low rainfall and hence provokes water stress worldwide, especially
The work is also complemented with the most representative both pilot
in regions with desertic climates (Lorite et al., 2018; World Health
and full-scale plants installed with these technologies, with details on
Organization, 2012). Moreover, in recent years many countries
their location and their capacity and efficiency. Thus, this review brings
have suffered chronic droughts, as well as irregular and violent rain-
fall leading to disastrous floods and drylands (Bouderbala, 2019;
World Health Organization, 2012). In this respect, the World Health
Organization (WHO) points out that the effects will be particularly Table 1
acute in arid areas and areas with growing populations (World Drinking water and irrigation water standards established by WHO and FAO,
Health Organization, 2012). Also, and due to the lack of rainfall, respectively.
crops require constant intensive irrigation and an increase in exter- Parameter WHO FAO
nal agents, which in turn rise water extraction, with a consequent (World Health Organization, 2012) (Misstear et al., 2017)
increase in the Water Stress Index (Lorite et al., 2018). Nitrates (mg/L) 50 22
Calcium (mg/L) 300
Magnesium (mg/L) 300
As summarized in Table 1, the WHO and the Food and Agriculture Sodium (mg/L) 200 69
Organization of the United Nations (FAO) have established quality stan- Potassium (mg/L) 12
dards for drinking water and for irrigation. Accordingly, different Sulphates (mg/L) 250
thresholds are considered for nitrates (NO−3 ), calcium (Ca
2+
), magne- Chloride (mg/L) 200 107
Bicarbonates (mg/L) 91.5
sium (Mg2+), sodium (Na+), potassium (K+), sulphate (SO2− 4 ), chlo- Fluorides (mg/L) 1.5
ride (Cl − ), bicarbonate (HCO− −
3 ) and fluoride (F ), as well as Conductivity (μS/cm) 2500
conductivity, pH and total dissolved solids. It is important to note that pH 6.5–8.5
FAO's values are stricter than WHO's recommendations in all the com- Total dissolved solids 600 450
(mg/L)
mon parameters quantified.
2
together an updated diagnosis of nitrate pollution in groundwater bodies concentrations are observed in groundwater, they are attributed to
together with the analysis of the different alternative solutions for their domestic sewage pollution (Su et al., 2020). Thus, areas of sewage in-
removal. puts could be differentiated from the other farming inputs by Cl− and
NO− 3 concentrations.
2. Nitrate sources Besides, the presence of nitrates due to the use of chemical fertilizers
implies the co-existence of other ions in groundwater, such as F−, SO2− 4 ,
Nitrate is considered the most widespread pollutant in groundwater and K+ (Roy et al., 2020). In this regard, Varol and Şekerci (2018) re-
induced by its high solubility in water and the difficulty to be fixed in ported that the use of certain chemical fertilizers may be the source of
the soil (Bhatnagar and Sillanpää, 2011). Although nitrogen compounds some heavy metals (i.e. arsenic) in groundwater (Varol and Şekerci,
are present in the environment from natural sources e.g., coming from 2018). Mazhar and Ahmad (2020) concluded that the presence of cad-
igneous rocks, atmospheric deposition and symbioses of some plants, mium (Cd 2+ ) and zinc (Zn 2+ ) is also due to the use of fertilizers
along with cyanobacteria and some heterotrophs (Gutiérrez et al., (Mazhar and Ahmad, 2020). Moreover, Escherichia coli, Enterococci,
2018); the main problem of nitrates is the dramatic increase in recent and Total Coliforms are also present in groundwater when nitrate pollu-
years due to anthropogenic actions. On the other hand, the main anthro- tion is associated with domestic leaks, mainly latrines and septic tanks
pogenic sources of nitrate pollution are nitrogen-rich fertilizers used for (Kapembo et al., 2016).
agricultural purposes, discharge of poorly treated domestic, and indus- Regarding the strong seasonal fluctuations, two opposite effects could
trial wastewaters, livestock manure, and leachate from landfill sites occur depending on the characteristics of the terrain: i) an increase in ni-
(Gutiérrez et al., 2018; Tokazhanov et al., 2020). In this sense, in the trate concentration during the rain period due to rainwater infiltration
Mediterranean area, where agriculture is the predominant economic ac- (Varol and Şekerci, 2018) and, ii) a decrease in NO− 3 concentration in the
tivity, nitrate pollution is mainly caused by the use of nitrogen-rich fer- wet season because ions are diluted in the rainfall (Abu-alnaeem et al.,
tilizers. This issue affects shallow wells, due to their location close to the 2018; Roy et al., 2020).
surface, where nitrate pollution occurs (Heaton et al., 2012; Re et al., In terms of the interest aroused from the literature through studies,
2017). In contrast, in developing countries the main source of nitrates regarding groundwater and nitrates pollution, Fig. 2 shows the biblio-
in groundwater is the lack of adequate sanitation (Kapembo et al., metric graph of articles published on groundwater pollution and nitrate
2016). presence from the late 1960s to the present. As depicted in Fig. 2, the in-
The nitrate cycle explains the generation of nitrate by natural pathways terest in the study of the health of groundwater has experienced an ex-
or by anthropogenic actions as shown in Fig. 1. Firstly, N2 is leached and ponential growth since the early 80s. While in the 70–80 decade, the
fixed in the soil by bacteria. Consequently, in a second step, the fixed nitro- scientific community published an average of 100 articles per year,
gen suffers ammonification, and the ammonia reacts and converts to ni- this number has steadily increased with 2742 articles published in
trites or nitrates. These compounds, in turn, may leach to groundwater or 2020 in this field. In the case of the publications focused on the presence
suffer denitrification by some bacteria or plants and return to the atmo- of nitrates in groundwater, the number of published articles has
sphere in the form of nitrogen gas (Gutiérrez et al., 2018). increased from 20 manuscripts published in 1990 to 280 articles pub-
Contrarily, many works highlighted a close relation between nitrates lished in 2021 highlighting the growing interest and concern regarding
and chloride (Cl−) concentration, caused by sewage infiltration (Rezaei this topic.
et al., 2017; Vystavna et al., 2017). In this context, Vystavna et al., 2017 Thus, groundwater health and specifically the presence of nitrates in
and Rezaei et al., 2017, have determined that denitrification processes groundwater is nowadays of great concern and is necessary to be thor-
occur when the ratio NO− 3 /Cl
−
decreases. Su et al., 2020 reported that oughly considered. In this framework, two different aspects need to be ad-
− −
a high NO3 /Cl ratio may suggest pollution from fertilizers and rain- dressed: i) collecting the data reported so far, and ii) making a comparison
water, while low ratios correspond to manure pollution (Su et al., of technological alternatives for nitrates removal to help in the decision-
2020). Moreover, when high NO − 3 /Cl
−
molar ratios and high Cl− making process of future nitrate mitigation strategies.
Fig. 1. Nitrogen cycle.
3
3000
2500
2000
Documents
1500
1000
500
0
1968 1972 1976 1980 1984 1988 1992 1996 2000 2004 2008 2012 2016 2020
Year
Groundwater polluon Nitrates in groundwater
Fig. 2. Bibliometric analysis of articles published in the field of groundwater pollution and nitrate presence.
(Scopus source, updated at 16th November 2021).
3. Nitrates in groundwater bodies In the next sections, a discussion of the results will be held continent by
continent, emphasizing the most striking values as well as the main source
Groundwater hydrochemistry has been largely considered in several of nitrate contamination in that region. In addition, the location of nitrate
works, especially in the last few years (Ahmed et al., 2019; Awomeso pollution regions has been numbered in each figure from the lowest to
et al., 2020; Bojarczuk et al., 2019; da Silva Peixoto et al., 2020; Devaraj the highest average value to facilitate the discussion. When the information
et al., 2020; Erdogan et al., 2020; Gil-Márquez et al., 2019; Hepburn was available, in addition to the average value, the minimum and maxi-
et al., 2020; Rodriguez-Espinosa et al., 2020). This discipline studies the mum values reported in the literature have been included. The detailed ref-
main ions present in groundwater; which presence is mainly determined erences of each pushpin are included as supporting information (SI) which
by the geology and mineralogical composition of the environment, the contains a complete characterization in terms of NO− 3 , Ca
2+
, Mg2+, Na+,
+ 2− − −
water residence time, and the rock-water interactions, among others K , SO4 , Cl , HCO3 of each point analyzed along the manuscript. For
(Islam et al., 2019). Numerous works have been reported worldwide, tak- a clearer visualization of the data assessed among the continents, both the
ing groundwater samples from wells, boreholes, and springs, that are manuscript and the SI contain the maps and the graphics including average,
mostly used for irrigation or domestic purposes. maximum, and minimum values reported by the authors.
Fig. 3 shows the extended concentration of nitrate differentiated with
colours. Blue pushpins indicate that the mean value is under 50 ppm, the 3.1. Asia
threshold established by WHO to guarantee good quality of groundwater.
In contrast, yellow pushpins show the locations where, despite the average The Asian continent is the one that shows the greatest variability in the
is accordance to WHO standards, some measurements are above 50 ppm. data, as can be seen in Fig. 4, which is divided in two parts. The first part in-
Orange colour reflects the groundwater bodies with more than 25% of cludes all the regions studied (Fig. 4a), and the second one reports the mean,
the samples with nitrate concentration higher than 50 ppm, and finally, maximum and minimum values of each point (Fig. 4b). In the aforemen-
red colour pushpins indicate the locations where groundwater is highly pol- tioned figure, the data of 93 regions are collected. For the vast majority of
luted, and therefore the quality of this water is prohibited for utilization the areas, the maximum value exceeds the WHO standard (50 ppm) despite
without previous treatment according to the standards established by the the average value being within the standards. Specifically, in 19 regions, de-
WHO. For a clearer visualization of the data, Table 2, summarizes the 292 spite the mean value is in concordance to the standards recommended by
points studied as a function of nitrate pollution. In this context, 94 samples WHO, more than 25% of the samples have values above 50 ppm.
were studied in Africa, 93 in Asia, 71 in Europe, and 34 in America. Al- A total of 20 regions located in India, Palestine, and Saudi Arabia, and
though Oceania continent has reported an article in the field of groundwa- other areas of China and Pakistan show a mean value above 50 ppm
ter health, it does not provide data about nitrates (Hepburn et al., 2020). (Abu-alnaeem et al., 2018; Alslaibi et al., 2017; Devaraj et al., 2020; Feng
Regarding contaminated areas, 30 regions in Africa, 20 in Asia, and 9 in et al., 2020; Jehan et al., 2019; Kumari and Rai, 2020; Musaed et al.,
Europe are in a critical situation. Besides, Europe presents the highest 2020; Pant et al., 2020; Roy et al., 2020). In particular, as shown in
percentage of regions polluted with more than 25% of samples above Fig. 4, it is also possible to verify that 11 samples have maximum values
50 ppm of nitrates. On the other hand, despite the data corresponding to above 300 ppm and 5 of them (points 81, 84, 86, 89, and 92, Fig. 4) have
Asia showing 45 regions without nitrate pollution, 19 areas present con- maximum values greater than 600 ppm. (Feng et al., 2020; Kumari and
tamination in at least 25% of the samples. In this regard, despite the num- Rai, 2020; Musaed et al., 2020; Pant et al., 2020).
ber of polluted regions in Asia is higher than in Europe, 19 and 16 In India, there are numerous available samples, and the variability of
respectively, in terms of percentage of polluted regions, Europe counts the data is striking since while some of the areas studied have mean values
with more areas with concentrations of nitrates above 50 ppm. For its below 50 ppm, other regions have averaged values between 59 and
part, America only reports 5 regions with more than 25% of samples with 215 mg/L (points 75, 76, 77, 79, 82, 84, 88 and 92, Fig. 4) (Devaraj
NO− 3 concentration above WHO recommended value. Finally, the manu- et al., 2020; Pant et al., 2020; Roy et al., 2020). It is important to note
scripts addressing the African continent highlight 34 regions with average that this last value is more than fourfold higher than the standard recom-
values below 50 ppm. mended by WHO. Birbhum (points 44 and 45, Fig. 4), Solapur (points 66
4
Fig. 3. Locations and nitrate concentration [NO− 3 ] in groundwater bodies (Abboud, 2018; Abderamane et al., 2013; Abou Zakhem et al., 2017; Abou Zakhem and Hafez,
2015; Abu-alnaeem et al., 2018; Ahmed et al., 2019; Aladejana et al., 2020; Ali et al., 2019; Alslaibi et al., 2017; Anim-Gyampo et al., 2018; Ruiz-García et al., 2019;
Ashun and Bansah, 2017; Asmael et al., 2015; Atikul Islam et al., 2017; Awomeso et al., 2020; Barbieri et al., 2019; Batsaikhan et al., 2018; Bello et al., 2019;
Benkaddour et al., 2020; Benmarce and Khanchoul, 2019; Beyene et al., 2019; Bicalho et al., 2019; Blázquez-Pallí et al., 2019; Bojarczuk et al., 2019; Bon et al., 2020;
Boudjana et al., 2019; Bouteraa et al., 2019; Bretzler et al., 2017; Bucci et al., 2017; Canora et al., 2019; Carasek et al., 2020; Carvalho et al., 2019; Celestino et al., 2019;
Chandrajith et al., 2014; Charizopoulos et al., 2018; Costa et al., 2015; Ćuk et al., 2020; Daesslé et al., 2020; Danni et al., 2019; da Silva Peixoto et al., 2020; de Oca
et al., 2019; Devaraj et al., 2020; di Lorenzo et al., 2012; Dippong et al., 2019; Egbi et al., 2019; el Gammal and Ibrahim, 2017; el Ghali et al., 2020; Elumalai et al., 2019;
Erdogan et al., 2020; Erostate et al., 2018; Esteller et al., 2017; Fan et al., 2020; Feng et al., 2020; Ferchichi et al., 2018; Ferrante et al., 2018; Gamazo et al., 2018;
Gamboa et al., 2019; Gevera and Mouri, 2018; Gil-Márquez et al., 2019; Giménez-Forcada et al., 2017; Gomez et al., 2019; Gorgij et al., 2019; Gromadzka et al., 2015;
Heaton et al., 2012; Hossain and Patra, 2020; Islam et al., 2018, 2019; Ismail et al., 2019; Jehan et al., 2019; Kapembo et al., 2016; Karakuş, 2019; Karroum et al., 2017;
Kattan, 2018; Kawo and Karuppannan, 2018; Khanoranga and Khalid, 2019; Kshetrimayum and Thokchom, 2017; Kumari and Rai, 2020; F. Liu et al., 2020; J. Liu et al.,
2020; T. Liu et al., 2020; Loh et al., 2020; Loomer et al., 2019; Lorette et al., 2018; Majkić-Dursun et al., 2018; Masocha et al., 2019; Mazhar and Ahmad, 2020; Melki
et al., 2019; Mendes et al., 2019; Mirčovski et al., 2018; Moni et al., 2019; Moratalla et al., 2009; Mostaza-Colado et al., 2018; Mouassa et al., 2020; Mudzielwana et al.,
2020; Mukanga et al., 2016; Mukate et al., 2019; Musaed et al., 2020; Mushtaq et al., 2018; Muzenda et al., 2019; Ncibi et al., 2020; Nguyen et al., 2015; Nikolenko
et al., 2019; Nyilitya et al., 2020; Ogrinc et al., 2019; Opoku et al., 2020; Ossa-Valencia and Betancur-Vargas, 2018; Owamah, 2020; Panno et al., 2019; Pant et al., 2020;
Papazotos et al., 2019; Pedretti et al., 2019; Quenet et al., 2019; Quino-Lima et al., 2020; Rashid et al., 2020; Re et al., 2017; Rezaei et al., 2017; Rodriguez et al., 2020;
Roy et al., 2020; Rufino et al., 2019; Sánchez-Gutiérrez et al., 2020; Sarker et al., 2018; Sedlazeck et al., 2017; Sefie et al., 2018; Silva et al., 2017; Slavinskienė and
Jurevičius, 2016; Smedley et al., 2018; Snousy et al., 2020; Strauhal et al., 2016; Sunkari et al., 2019; Swift Bird et al., 2020; Talib et al., 2019; Taucare et al., 2020;
Thakur et al., 2015; Tolera et al., 2020, 2017; Torres-Martínez et al., 2020; Tran et al., 2020; Tzoraki et al., 2018; Ujević Bošnjak et al., 2012; Varol and Şekerci, 2018;
Vystavna et al., 2015; Yetiş et al., 2019; Zaki et al., 2019; Zango et al., 2019; Zhang et al., 2020).
and 71, Fig. 4), and Bareilly (points 31 and 51, Fig. 4), all of them located in Fig. 4), where in most cases, the authors attributed this fact to sewage dis-
India, they report mean values in the range between 7 and 47 mg/L. Never- posal and farming inputs (Abu-alnaeem et al., 2018; Barbieri et al., 2019;
theless, these regions have also more than 25% of samples of nitrate con- Musaed et al., 2020). Palestine also shows mean values below 50 ppm in
centration above 50 mg/L (Hossain and Patra, 2020; Mazhar and Ahmad, some regions (points 7, 8, 60, 73, and 74, Fig. 4) (Alslaibi et al., 2017).
2020; Mukate et al., 2019). Regarding the possible causes of contamination In the Asian continent, the NO− 3 pollution is primarily due to septic
in this country, some authors highlight the poor maintenance of septic tanks and agriculture inputs leakage. Moreover, many authors emphasize
tanks and boreholes, sewage discharge, and fertilizers (Barbieri et al., the high variability due to the strong influence that the rainy season has
2019; Devaraj et al., 2020; Roy et al., 2020). on the groundwater quality of this continent (Amanambu et al., 2020;
Contrarily, the mean values are between 50 and 220 mg/L in Palestine Nguyen et al., 2015). In this continent, water scarcity is recognized as one
(points 80, 83, 85, 87, 90, 91, and 93, Fig. 4) and Saudi Arabia (point 86, of the most important concerns in many countries especially in the Middle
Table 2
Sources of nitrates categorized by continents.
Continent Asia America Europe Africa Total
Number of regions with [NO−3 ] average > 50 ppm 20 1 9 30 60

Number of regions with [NO− −
3 ] average < 50 ppm and more than 25% of samples with NO3 concentration > 50 ppm 19 4 16 10 49
Number of regions with [NO3−] average < 50 ppm and less than 25% of samples with NO3− concentration > 50 ppm 9 2 6 7 24
Number regions with [NO−3 ] average < 50 ppm 45 27 39 34 145
Total number of regions 93 34 71 94 292
5
Fig. 4. a) Studied regions in Asia. b) Mean value and range of nitrate concentration in Asian groundwater bodies (Ahmed et al., 2019; Alslaibi et al., 2017; Asmael et al., 2015;
Atikul Islam et al., 2017; Batsaikhan et al., 2018; Chandrajith et al., 2014; Costa et al., 2015; Fan et al., 2020; Islam et al., 2018, 2019; Ismail et al., 2019; Khanoranga and
Khalid, 2019; Kshetrimayum and Thokchom, 2017; J. Liu et al., 2020; T. Liu et al., 2020; Mazhar and Ahmad, 2020; Moni et al., 2019; Mushtaq et al., 2018; Nguyen et al.,
2015; Sarker et al., 2018; Sefie et al., 2018; Talib et al., 2019; Thakur et al., 2015). Detailed references are included in Table S1 of the Supplementary Information.
6
East, and consequently, the use of fertilizers is continuously growing, farming areas together with human or livestock wastes. On the other
encouraging the presence of nitrates in groundwater (Alaei Shahmirzadi hand, poor living conditions and unsuitable sanitary and sewage disposal
et al., 2018). practices constitute an additional source of NO− 3 pollution in developing
The different information collected is summarized in Table 3, which countries such as Mongolia (Batsaikhan et al., 2018). Finally, despite
shows the source of nitrate pollution classified into five categories: septic Malaysia has NO− 3 values within the WHO recommended standards, the
tanks, sewage, agriculture, landfills, and industrial activities. Besides, impact of intensive human activities and deforestation in certain areas
three levels of risk have been determined and associated to the categories, has provoked an increase in nitrate contamination (Sefie et al., 2018).
low ( ), medium ( ), or high ( ) along the different countries considered in In a different way, the high values of nitrates in different regions
the study. Green colour has been established when the category is of “no (e.g., Pakistan) are attributed to the solubility of minerals, such as feldspar,
concern” in the country, meaning there is no risk evidence so far. Medium biotite, muscovite, calcite, and dolomite (Jehan et al., 2019; Khanoranga
risk has been considered when some regions in a country present concern- and Khalid, 2019). In this line, Khanoranga and Khalid (2019) highlighted
ing values of nitrate, and the category is considered as a “potential influ- that the composition of Balochistan province area groundwater is greatly
ence”. Finally, the highest level of risk has been set up when any region influenced by the geological composition and anthropogenic activities
in the country reports nitrate pollution, and the evidence indicates that like agricultural occupations and brick kiln factories carried out in the vi-
this category has a “significant contribution”. cinity of the study area (Khanoranga and Khalid, 2019).
Agriculture is the main activity that causes the high nitrate values in China, for its part, has different hypotheses to justify the increment of
Saudi Arabia, Myanmar and Jordan (Abboud, 2018; Kshetrimayum and nitrates in groundwater. For example, in a recent article, high values are de-
Thokchom, 2017; Musaed et al., 2020; Pincetti-Zúniga et al., 2020). Con- fined as non-point sources of contamination (Feng et al., 2020). In particu-
cerning nitrates and phosphates in groundwater in Sri Lanka, Bangladesh, lar, Feng et al. (2020) emphasized the risk associated with irrigation of
Vietnam, and Nepal, recent works pointed to the agriculture inputs and la- farmland employing sewage, and excessive nitrogen fertilizer usage. In
trines that penetrate the sandy aquifers as potential contamination activi- this regard, Tolera et al. (2017) and Kim and Park (2016) reported ground-
ties (Chandrajith et al., 2014; Islam et al., 2018; Lee et al., 2018; water contamination by nitrate from non-point sources (application of fer-
McArthur et al., 2012; Nguyen et al., 2015; Thakur et al., 2015). In the tilizers and animal wastes) as a serious concern in South Korea (Kim and
case of Iraq and the Gaza coastal (Palestine) recent works reported a clear Park, 2016; Tolera et al., 2017).
concern for agricultural fertilizers, industrial waste, and municipal sewage
(Abu-alnaeem et al., 2018; Ismail et al., 2019; Mostaza-Colado et al., 2018). 3.2. America
In contrast, the information available for Iran explains that in this country,
the nitrate concentration is regularly low (Rezaei et al., 2017). Still, it can In this section, the different regions of the American continent are dis-
achieve abnormal values subsequently of draining or overflow from the cussed, where 34 areas are collected. Fig. 5 illustrates all the regions studied
in this continent (Fig. 5a) and the mean values sorted by size, including the
Table 3 minimum and maximum data (Fig. 5b). Although up to 11 countries have
Main causes of nitrate pollution in Asia. been studied in this continent, only one of the references reported an aver-
age value of nitrates higher than 50 ppm (point 33, Fig. 5). This region is
Fortaleza (Brazil) which informed a concentration above WHO's limits,
with a mean value of 51.3 mg/L (da Silva Peixoto et al., 2020). In this
way, the high values of nitrates in Brazil are referred mainly to septic
tanks and sewage discharge and to a lesser extent to agriculture inputs
and industrial wastes (da Silva Bellettini et al., 2019; da Silva Peixoto
et al., 2020; Rezende et al., 2019; Suhogusoff et al., 2019). Besides, da
Silva Peixoto et al. (2020) attributed this contamination to two different
sources: (i) sewage discharge and (ii) low natural recharge from precipita-
tion (da Silva Peixoto et al., 2020). In contrast, da Silva Bellettini et al.
(2019) reported that the coal mining industry without proper wastewater
treatment contributed to high nitrates concentration in the Carboniferous
region (Brazil) (da Silva Bellettini et al., 2019).
Most of the sources are represented in blue colour, indicating no pollu-
tion in terms of nitrates, highlighting several areas of Mexico, Chile, Costa
Rica, the USA, Colombia, and Argentina which have the maximum values
within the WHO limits (points 1–16, Fig. 5). Nevertheless, in other regions
located in Mexico, such as Mezquital and Toluca Valley, the mean values
are in the range 2–36 mg/L; but more than 25% of the samples analyzed re-
port values above 50 mg/L of NO− 3 (points 14, 16, 18 and 31, Fig. 5) (de
Oca et al., 2019; Esteller et al., 2017).
Besides, in two regions located in Illinois (United States of America)
(point 24, Fig. 5) and Bolivia (point 29, Fig. 5), although some measure-
ments reflect a certain degree of contamination, less than 25% of the values
exceed 50 ppm (Panno et al., 2019; Quino-Lima et al., 2020). Specifically,
in the case of Bolivia, as illustrated in Fig. 5, although the average value ful-
fills the standard, some samples are above 200 mg/L, provoking a cause of
great concern in this region (point 29, Fig. 5) (Quino-Lima et al., 2020). The
authors attribute the contamination to human activities, such as insufficient
treatment of urban wastes and intensive agriculture (Quino-Lima et al.,
2020).
Regarding the main causes of nitrate pollution, Table 4 summarizes the
different risks associated with the different activities analyzed. For exam-
Risk of contamination: ( ) low, ( ) medium, ( ) high.
ple, in Argentina, human activities have affected some areas since some
7
Fig. 5. a) Regions studied in America. b) Mean value and range of nitrate concentration in American groundwater bodies (Bucci et al., 2017; Carasek et al., 2020; Celestino
et al., 2019; Daesslé et al., 2020; da Silva Peixoto et al., 2020; de Oca et al., 2019; Esteller et al., 2017; Gamazo et al., 2018; Gamboa et al., 2019; Gomez et al., 2019; Juliana
et al., 2018; Loomer et al., 2019; Mendes et al., 2019; Ossa-Valencia and Betancur-Vargas, 2018; Panno et al., 2019; Quino-Lima et al., 2020; Sánchez-Gutiérrez et al., 2020;
Swift Bird et al., 2020; Taucare et al., 2020; Torres-Martínez et al., 2020). Detailed references are incorporated in Table S3 of the Supplementary Information.
8
Table 4 In the specific case of the USA, Ward et al. (2018) point out that there
Nitrate pollution in America. are many private wells in the United States of America that are not regu-
lated by the Environmental Protection Agency (EPA) (Ward et al., 2018)
and consequently no pollutant areas are reported. In fact, these authors es-
timated that 2% of public-supply wells and 6% of private wells exceeded
the maximum contaminant level (MCL) for nitrate in public drinking
water supplies in the United States. MCL is situated as 10 mg·L−1 as
nitrate‑nitrogen, which is approximately equivalent to the WHO guideline
of 50 mg·L−1. Moreover, an assessment carried out in the United States be-
tween 1991 and 2003 demonstrated that nitrate concentrations were
highest in shallow groundwater beneath agricultural land use or areas
with well-drained soils and oxic geochemical conditions. In contrast,
lower values were found in deep groundwater when these water bodies
were older since the anthropogenic sources had not already caused a signif-
icant impact. In this context, The United States Geological Survey (USGS), a
scientific agency of the government, developed a robust model, based on
nationwide data, to estimate the risk of nitrate contamination in shallow
groundwater across the United States. This model integrates nitrogen in-
puts and aquifer vulnerability using Geographic Information System (GIS)
technology (“Groundwater Quality”, 2019). Nitrogen inputs include com-
mercial fertilizer and manure application rates, atmospheric contributions,
and population densities.
Aquifer vulnerability is represented by soil-drainage characteristics and
the extent to which woodlands are interspersed with cropland. Fig. 6, ex-
tracted from the USGS, represents the areas with the highest risk of contam-
aquifers are increasing the groundwater abstraction rates and the return ve- ination from both natural and human-induced sources (“Groundwater
locity of the sewage or the industrial discharge with poor treatment (Isla Quality”, 2019).
et al., 2018; Lupi et al., 2019). On the other hand, while in Chile, nowadays,
agricultural practices are the major cause of concern for nitrates pollution 3.3. Europe
(Sánchez-Gutiérrez et al., 2020), in Colombia, groundwater at the shallow
levels present anthropogenic contamination from agricultural activities, In the European continent, a total of 71 regions have been collected and
livestock, poor management of solid waste, and the lack of a sewer system discussed. Despite the mean value being under the WHO limit in many
in certain regions (Ossa-Valencia and Betancur-Vargas, 2018). Finally, in areas, 22 regions have maximum values above 50 ppm. In more detail, 16
Guatemala, the risk is associated with fertilizers and urban wastewater of the studied regions have more than 25% of samples with NO− 3 values
(Bucci et al., 2017). above 50 mg·L−1. Fig. 7 depicts the different areas studied (Fig. 7a) and
Fig. 6. Risk of nitrate pollution in groundwater aquifers in USA.

Adapted from (“Groundwater Quality”, 2019).
9
Fig. 7. a) Distribution of nitrate polluted zones in Europe. b) Nitrate concentration in European groundwater bodies (Ruiz-García et al., 2019; Barbieri et al., 2019; Bicalho
et al., 2019; Blázquez-Pallí et al., 2019; Bojarczuk et al., 2019; Boudjana et al., 2019; Canora et al., 2019; Carvalho et al., 2019; Charizopoulos et al., 2018; Ćuk et al., 2020; di
Lorenzo et al., 2012; Dippong et al., 2019; Erostate et al., 2018; Gil-Márquez et al., 2019; Giménez-Forcada et al., 2017; Gromadzka et al., 2015; Heaton et al., 2012; Karakuş,
2019; Lorette et al., 2018; Majkić-Dursun et al., 2018; Mirčovski et al., 2018; Moratalla et al., 2009; Mostaza-Colado et al., 2018; Nikolenko et al., 2019; Ogrinc et al., 2019;
Papazotos et al., 2019; Pedretti et al., 2019; Quenet et al., 2019; Rodriguez et al., 2020; Rufino et al., 2019; Sedlazeck et al., 2017; Slavinskienė and Jurevičius, 2016; Smedley
et al., 2018; Strauhal et al., 2016; Tran et al., 2020; Tzoraki et al., 2018; Ujević Bošnjak et al., 2012; Varol and Şekerci, 2018; Vystavna et al., 2015; Yetiş et al., 2019).
References are detailed in Table S5 of the Supplementary Information.
10
the mean, maximum and minimum values of each point (Fig. 7b). As it is Table 5
drawn in the mentioned figure, the values of Italy (points 65–67, Fig. 7), Pollution sources in Europe.
Malta (points 60, 64 and 70, Fig. 7), Lithuania (point 69, Fig. 7),
Belgium (points 7 and 62, Fig. 7) and Spain (point 68, Fig. 7), contain
high concentration of nitrates, with a mean value between 72 ±
6 mg/L, 104 ± 41 mg/L, 120 mg/L, 62 ± 3 mg/L, and 80 mg/L, respec-
tively (Boudjana et al., 2019; di Lorenzo et al., 2012; Heaton et al.,
2012; Nikolenko et al., 2019; Rodriguez et al., 2020; Slavinskienė and
Jurevičius, 2016). In addition, two additional regions in Duero (Spain)
(point 61, Fig. 7) and Malta (point 70, Fig. 7) also have maximum con-
centration values of nitrates of high concern since they exceed
200 ppm. In the case of Italy, the major concerns in terms of activities
that cause higher nitrate concentration are synthetic fertilizers, mainly
ammonium salts, and runoff processes. Nevertheless, groundwater in
Italy is often locally affected by denitrification processes that reduce
the nitrate content, offering values consistent with legal standards.
Regarding the high values reported, Malta mineral fertilizers, animal
and human sewage waste, and soil cultivation are the main sources of
contamination (Heaton et al., 2012). Contrarily, Lithuania has reported
the maximum worldwide value of nitrate concentration, 2753 mg/L
(point 69, Fig. 7) (Slavinskienė and Jurevičius, 2016). This high concentra-
tion was measured in a groundwater body close to open hydrogeological
systems, where some landfills are located (Slavinskienė and Jurevičius,
2016).
In Belgium, the concerning values of nitrates are attributed to poor
treatment of household sewage and manure (Nikolenko et al., 2019). In
this line, a recent report from the European Commission to the council
and the European parliament claimed that a high percentage of groundwa-
ter monitored currently shows high NO− 3 concentration, above the maxi-
mum 50 ppm, in Malta, Germany, Luxemburg, Spain, Portugal, and
Belgium (Flanders region).
In contrast, points from 1 to 61 present mean values below 50 ppm. In
this sense, some countries, such as Finland (point 9, Fig. 7), Croatia (point
11, Fig. 7), Serbia (points 17 and 39, Fig. 7), Spain (point 29, Fig. 7),
Macedonia (point 41, Fig. 7), Poland (point 53, Fig. 7), Greece (points 55,
57 and 58, Fig. 7), and Romania (point 56, Fig. 7) have mean values
below 50 mg/L (Bojarczuk et al., 2019; Charizopoulos et al., 2018; Ćuk
et al., 2020; Dippong et al., 2019; Mirčovski et al., 2018; Ogrinc et al.,
2019; Papazotos et al., 2019; Pedretti et al., 2019; Ujević Bošnjak et al.,
2012). Nevertheless, there are areas of special concern where more than a
quarter of the collected samples are polluted. Additionally, Turkey (point
49, Fig. 7), Ukraine (point 37, Fig. 7), United Kingdom (point 24, Fig. 7),
Slovenia (point 34, Fig. 7) and Albania (point 52, Fig. 7) report samples
with nitrate concentration above 50 mg/L (Barbieri et al., 2015; Ogrinc
et al., 2019; Smedley et al., 2018; Varol and Şekerci, 2018; Vystavna Croatia and Cyprus the contamination of groundwater excluded any
et al., 2015). urban or industrial source but underlined the risk of agriculture inputs
As in previous continents, Table 5 shows the risk of nitrate pollution (Nikolaou et al., 2020; Tzoraki et al., 2018; Ujević Bošnjak et al., 2012).
due to the five different activities analyzed in this work. In Europe, the Finally, previous works focused on Serbia, remarked some anthropogenic
primary source of nitrates is leaching of fertilizers, the excess of live- activities of special concern, nitrogen-based fertilizers and manure, and to
stock, and municipal human wastes (Heaton et al., 2012; Rodriguez a larger extent, mixing of sewage and septic tank effluents (Majkić-
et al., 2020). For example, in Spain, France, and Macedonia, intensive Dursun et al., 2019, 2018).
agriculture using NPK fertilizers and the manure used as fertilizer are In the line with the conclusions reported in previous works and col-
the main sources of high nitrate levels (Giménez-Forcada et al., 2017; lected through this work, the European Environment Agency (EEA) has
Mirčovski et al., 2018; Nofal et al., 2019; Rodriguez et al., 2020). A sim- developed a map highlighting the percentage of groundwater body
ilar situation is found in Greece, where the upper values of nitrates are areas that present bad chemical status due to nitrate and total nitrogen
related to intensive agriculture and nitrogen fertilizers (Vasileiou input from organic and inorganic fertilizers (EEA, 2012). Fig. 8 shows
et al., 2019). Regarding Romania, high concentrations have been the areas and the risk associated. Northern Europe countries
found in areas with pig farms and grapevine cultures (Dippong et al., (Norway, Sweden, Estonia, Latvia, and Lithuania) present good quality
2019). In this way, many authors pointed to agricultural activity, poor of groundwater in terms of nitrates presence. However, in general, re-
sewage treatment, and manure as the main anthropogenic sources of gions of central Europe (France, Germany, Poland among others)
pollution in Turkey, Ukraine, the United Kingdom, Slovenia, and have a remarkable percentage of areas with a risk of up to 10% of
Albania (Barbieri et al., 2015; Ogrinc et al., 2019; Smedley et al., groundwater with poor chemical status due to nitrates. Moreover,
2018; Varol and Şekerci, 2018; Vystavna et al., 2015). some areas in the Czech Republic, Slovenia, Netherlands, and Spain
While the discharge of municipal sewage and organic-mineral fertiliza- present a percentage between 70% and 90% classified as bad quality,
tion of agricultural land are the main contributors to the changes in the which is considered a concerning problem to be solved in the near fu-
quality of shallow groundwater in Poland (Bojarczuk et al., 2019), in ture (EEA, 2012).
11
Fig. 8. Map developed by EEA classifying the quality of groundwater (EEA, 2012).
3.4. Africa Kapembo et al., 2016; Muzenda et al., 2019). Previous works focused on
Mozambique and Zimbabwe mainly attributed the high mean values to filtra-
Finally, this section debates the African continent, which presents the tion and leaks from septic tanks and latrines (Arsénio et al., 2018; Barbieri
most concerning situation since one-third of the data reported mean values et al., 2019; Muzenda et al., 2019). In this sense, but in a more dramatic
of nitrate concentration in groundwater above the WHO threshold. In this way, the Democratic Republic of the Congo reports the most concerning sit-
continent, 94 points were collected and analyzed, as illustrated in Fig. 9a; uation worldwide, since there is poor sanitation and people make use of con-
the data reported so far in 15 sites did not allow to obtain average values taminated water for irrigation, domestic and drinking purposes. For example,
(Fig. 9b). In this regard, Africa has several countries in which groundwater in the commune of Bumbu (Democratic Republic of the Congo), above 75%
has been contaminated by nitrate, with mean values ranging from 52 to of people have no access to safe water, and the water sources are shallow
776 mg/L (see Fig. 9). For example, in some regions in the Democratic Re- wells that are located near latrines (Kapembo et al., 2016).
public of the Congo, Mozambique, and Zimbabwe, mean values are between Moreover, Angola (point 63, Fig. 9) and Grand Yaéré, Cameroon (point 51,
189 and 775 mg/L (points 68–81, Fig. 9), 89–172 mg/L (points 64 and 67, Fig. 9) reported average values of 83 and 50 ppm achieving maximum values
Fig. 9), and 72 mg/L (point 59, Fig. 9) respectively (Barbieri et al., 2019; of 132 and 646 mg/L respectively (Bello et al., 2019; Silva et al., 2017). In
12
Fig. 9. a) Regions studied in Africa. b) Nitrate concentration in African groundwater bodies (Abderamane et al., 2013; Aladejana et al., 2020; Anim-Gyampo et al., 2018;
Ashun and Bansah, 2017; Awomeso et al., 2020; Bello et al., 2019; Benkaddour et al., 2020; Benmarce and Khanchoul, 2019; Beyene et al., 2019; Bon et al., 2020; Bouteraa
et al., 2019; Bretzler et al., 2017; Danni et al., 2019; Egbi et al., 2019; el Gammal and Ibrahim, 2017; el Ghali et al., 2020; Elumalai et al., 2019; Erdogan et al., 2020; Ferchichi
et al., 2018; Ferrante et al., 2018; Gevera and Mouri, 2018; Kapembo et al., 2016; Karroum et al., 2017; Kawo and Karuppannan, 2018; Loh et al., 2020; Masocha et al., 2019;
Melki et al., 2019; Mouassa et al., 2020; Mudzielwana et al., 2020; Mukanga et al., 2016; Muzenda et al., 2019; Ncibi et al., 2020; Nyilitya et al., 2020; Opoku et al., 2020;
Owamah, 2020; Re et al., 2017; Silva et al., 2017; Snousy et al., 2020; Sunkari et al., 2019; Tolera et al., 2020; Zaki et al., 2019; Zango et al., 2019). Detailed references appear
in Table S7 of the Supplementary Information.
13
these two countries, the NO− 3 pollution is attributed to latrines and live- 2020). In the same line, Kawo and Karuppannan (2018) pointed out the
stock waste (Bello et al., 2019; Silva et al., 2017). Firstly, Silva et al. presence on nitrates in central Ethiopia due to agricultural inputs, waste
(2017) reported the presence of nitrate probably due to the direct dis- disposal site and several industries (Kawo and Karuppannan, 2018).
charge of nitrogen-rich and untreated domestic effluents in the high- Finally, in the case of Nigeria, NO−
3 comes from weathering of bedrocks,
porosity soil in Angola. Supporting this argument, in Cameroon, Bello leachate from septic tanks and dumpsites, runoff of materials, hardness, nu-
et al. (2019) found NO− +
3 evolution independently of K , thus, excluding trients from agricultural lands, and chlorine pollution (Awomeso et al.,
the use of agricultural fertilizers as potential source and therefore, at- 2020). In summary, Table 6 collects the different activities studied in this
tributing the presence of nitrates in this region to oxidation-reduction work as a function of the risk in each country.
reactions of organic matter associated with septic-tank effluents, animal
or plant production. 3.5. Summarize of nitrate pollution worldwide
Morocco presents nitrate concentrations between 33 and 74 mg/L
(points 48 and 61, Fig. 9) (Benkaddour et al., 2020) and the main source In view of the analysis of nitrate pollution, continent-by-continent, it
of nitrate pollution, is similar to the different areas studied in Europe; the can be concluded that nitrate pollution is a global problem. In this con-
overuse of fertilizers, pesticides, manure, and intensive agriculture and irri- text, if we pay attention to Fig. 10, and according to the analysis made
gation (Benkaddour et al., 2020). country-by-country, most of the regions studied in the Mediterranean
In the case of Ghana, South Tongu and Ada East region (point 63, Fig. 9) area have worried values and therefore is one of the most polluted
and Tunisia (points 52, 53, 55, 60 and 66, Fig. 9) the mean values are areas worldwide in terms of nitrate presence in groundwaters. To have
89 mg/L and 100 ± 38 mg/L, respectively (Egbi et al., 2019; Ferchichi a global vision and to appreciate this fact, Fig. 10 represents the regions
et al., 2018; Melki et al., 2019; Ncibi et al., 2020; Re et al., 2017) because studied in Europe and North Africa, and as can be seen, regarding NO− 3
of the intensive agricultural activities and discharge of domestic and indus- concentration, most of the areas collected show orange or red colour im-
trial sewage (Egbi et al., 2019; Ferchichi et al., 2018; Re et al., 2017). plying that more than 25% of the samples report values above 50 ppm
Other countries with contaminated sites in the African continent are (orange) or mean values higher than 50 mg·L −1 (red), which is the
South Africa (point 23, Fig. 9), Kenya (points 25, 39 and 47, Fig. 9), value established by WHO to determine the polluted areas.
Ethiopia (point 28, Fig. 9), Nigeria (points 36, 44 and 46, Fig. 9) and Besides, apart from the five categories of contamination studied
Chad (point 43, Fig. 9) (Abderamane et al., 2013; Aladejana et al., 2020; through this manuscript, different catastrophic events that occurred during
Ashun and Bansah, 2017; Awomeso et al., 2020; Elumalai et al., 2019; the past decades have changed the presence of nitrates in groundwater in
Kawo and Karuppannan, 2018; Nyilitya et al., 2020). the affected areas. For example, the groundwater around the Union Carbide
In the specific case of Algeria, there are two areas with a mean value factory in Bhopal has been contaminated with excessive levels of nitrate,
under 50 ppm, but some samples contain nitrate concentrations higher chloride, and heavy metals (“Water Contamination Crisis - Bhopal's
than this value (points 42 and 45, Fig. 9) (Bouteraa et al., 2019; Mouassa Second Disaster - The Bhopal medical appeal”, 2021). In the case of Beirut,
et al., 2020). Nevertheless, several points only reported mean values, in 2020, 2750 tons of ammonium nitrate inadequate storage caused an ex-
which are in most cases above 50 mg/L (points 82–91, Fig. 9) (Benmarce plosion creating an important number of pollutants being released to the
and Khanchoul, 2019). The presence of nitrates was attributed as in environment. Compared with a similar incident in Tianjin (China), coffer-
Kenya to the intensive agriculture and to livestock activity in this area dams and cement encasements should be built to prevent nitrates leakage
(Benmarce and Khanchoul, 2019; Mouassa et al., 2020; Nyilitya et al., to soil and groundwater, or nitrate contamination is likely to be distributed
in groundwater in five years (ur Rehman et al., 2021). Regarding the Cher-
nobyl accident, two regions of Belarus assessed the hazard of nitrates since
Table 6
Nitrate risk pollution in Africa. two regions reported similar radiation values but, the incidence of pediatric
thyroid cancer was different, being the main difference the nitrate contam-
ination in drinking water, 40 vs. 185 ppm (Drozd et al., 2018).
Regarding the existing regulation of nitrates worldwide, the world
health organization developed a report in 2015 using data from members
of the WHO International Network of Drinking-water Regulators, WHO re-
gional and country office contacts, through internet searches or purchased
from the relevant standards organizations considering 104 countries and
territories. Nitrates was one of only three inorganic parameters with a
value set by all countries and territories. For example, at the European
level, there exists a Directive (2006/18/EC) based on the protection of
groundwater against pollution and deterioration, fixing as quality standards
a maximum of 50 mg·L−1 of nitrates concentration. Besides, in 1991, the EU
introduced the Nitrates Directive (91/676/EEC), which aimed to reduce
water pollution caused or induced by nitrate from agricultural sources.
This Directive also defines Vulnerable Nitrate Zones where it is necessary
to establish and implement action programs to reduce water pollution
from nitrogen compounds. In the case of the United States of America, the
Environmental Protection Agency (EPA) has established a limit for nitrates
and nitrites in drinking water (10 parts per million (ppm) for nitrates and
1 ppm for nitrites), and the Food and Drug Administration (FDA) has recom-
mended limits for nitrates and nitrites in bottled water (same thresholds as
the EPA) and foodstuffs (sodium nitrate lower than 500 ppm in the finished
meat product, sodium nitrite below 200 ppm in the finished meat product
and potassium nitrate as curing agent in the processing of cod roe in an
amount less than 200 ppm in the finished roe).
This manuscript contains in-depth analysis developed using more than
272 regions worldwide, despite the focus on specific areas, which could not
necessarily apply to more extensive zones, allows us to conclude: i) the
14
Fig. 10. Location and nitrate concentration in groundwater bodies in the Mediterranean area. (Abboud, 2018; Abou Zakhem et al., 2017; Abou Zakhem and Hafez, 2015; Abu-
alnaeem et al., 2018; Alslaibi et al., 2017; Ruiz-García et al., 2019; Asmael et al., 2015; Benmarce and Khanchoul, 2019; Bicalho et al., 2019; Blázquez-Pallí et al., 2019; Bojarczuk
et al., 2019; Boudjana et al., 2019; Bouteraa et al., 2019; Canora et al., 2019; Carvalho et al., 2019; Charizopoulos et al., 2018; Ćuk et al., 2020; Danni et al., 2019; di Lorenzo et al.,
2012; Dippong et al., 2019; el Gammal and Ibrahim, 2017; el Ghali et al., 2020; Erostate et al., 2018; Ferchichi et al., 2018; Gil-Márquez et al., 2019; Giménez-Forcada et al., 2017;
Gorgij et al., 2019; Heaton et al., 2012; Karakuş, 2019; Karroum et al., 2017; Kattan, 2018; Lorette et al., 2018; Majkić-Dursun et al., 2018; Melki et al., 2019; Mirčovski et al., 2018;
Moratalla et al., 2009; Mostaza-Colado et al., 2018; Mouassa et al., 2020; Ncibi et al., 2020; Nikolenko et al., 2019; Papazotos et al., 2019; Quenet et al., 2019; Re et al., 2017;
Rezaei et al., 2017; Rodriguez et al., 2020; Rufino et al., 2019; Sedlazeck et al., 2017; Smedley et al., 2018; Snousy et al., 2020; Strauhal et al., 2016; Tran et al., 2020; Tzoraki
et al., 2018; Ujević Bošnjak et al., 2012; Varol and Şekerci, 2018; Vystavna et al., 2015; Yetiş et al., 2019; Zaki et al., 2019).
primary anthropogenic sources of nitrate are the use of fertilizers and the dis- Also, this pollution, far from being solved, shows an increasing trend
charge of non-treated domestic and industrial wastes, ii) at many points, the that demands drastic and urgent solutions to prevent this problem.
nitrate contamination is associated with other contamination by fluorine, sul- Thus, immediate actions are required before natural water bodies are
phates, potash, phosphates and some heavy metals such as zinc, cadmium or entirely spoiled, especially in developing countries with water short-
arsenic, and iii) nitrate pollution is mainly concentrated in the Mediterranean ages. Although there are different sources of nitrates pollution in
area and some regions of South Asia, where agriculture is an essential source groundwater bodies, the challenge of water remediation can be facili-
of income but also the presence of NO− 3 is a big concern in some developing tated by using similar technologies that enable the transfer of knowl-
African countries, due to the lack of adequate sanitation. edge and inter-site adaptation.
Table 7
Different technologies available to remove pollutants present in water bodies.
Technology Substances to be removed Ref
Precipitation and coagulation Phosphorous, fluoride, arsenic, ferrocyanide, and heavy metals. (Ballinas et al., 2004; Sharma and Bhattacharya, 2017)
Softening Hardness ions (Sharma and Bhattacharya, 2017)
Distillation Toxic chemicals, heavy metals, bacteria, viruses or parasites. (Sharma and Bhattacharya, 2017)
Adsorption Eliminate compounds that add either colour, taste, or odor to water, such (Sharma and Bhattacharya, 2017)
as VOCs, chlorine, heavy metals, organics.
Ion exchange Anions or cations based on resin type. (Sharma and Bhattacharya, 2017)
Reverse osmosis Salts, pesticides, microbes. (Sharma and Bhattacharya, 2017; Yang et al., 2019)
Electrodialysis Dissolved ionic particles. (Akhter et al., 2018; Sharma and Bhattacharya, 2017)
Catalytic processes Organic compounds, formic acid or nitrates. (Guate et al., 2019; Rezvani et al., 2019; Sharma and
Bhattacharya, 2017; Tokazhanov et al., 2020)
Bioremediation Heavy metals, sediments, pathogens, or dissolved organic chemicals. (Kozyatnyk and Klymenko, 2016; Sharma and Bhattacharya, 2017)
Magnetic separation Oil, suspended solids and some ions with difficulties to coagulate. (Sharma and Bhattacharya, 2017)
Disinfection (UV or chlorine) Bacteria and viruses. (Sharma and Bhattacharya, 2017)
Active carbon filtration Dissolved organic carbon (Sharma and Bhattacharya, 2017)
Filtration (UF, NF, gravel, sand…) Suspended solids, dyes or organic matter (Rashid et al., 2021)
Oxidation (mechanical, thermal, with ozone) Colour, odor, organic compounds, and inorganic compounds (Radu and Racoviteanu, 2021)
Clarification Total suspended solids (TSS) (Ortiz et al., 2015)
Aeration/air stripping Transferring of volatile components of a liquid into an air flow (Radu and Racoviteanu, 2021)
15
4. Alternatives to nitrate removal in the world dedicated to groundwater treatment. On this basis, Table 8
summarizes the facilities dedicated to this purpose as well as their daily ca-
As mentioned above, apart from nitrates, groundwater could contain pacity and the pollutants removed by these techniques. If we take as a basis,
different ions which must be removed before use. In this sense, nowa- a daily treatment flow greater than 1000 m3, we find that there are only 13
days, numerous water treatment technologies have been developed, ac- plants implemented in the world: five in the USA, five in Italy, and one in
cording to the pollutants, infrastructure, affordability, and acceptability Australia, India and Poland, respectively. Regarding the processes carried
(Hosseini et al., 2016; Sharma and Bhattacharya, 2017). In fact, the out in these plants, reverse osmosis (RO), filtration, and ultrafiltration
most common technologies to remove pollutants are summarized in (UF) are the most popular technologies employed in the United States of
Table 7. America. Besides, Italy has numerous plants located all over the country,
Currently, there are numerous technologies implemented at the indus- able to remove a wide variety of pollutants. On the other hand, iron, man-
trial scale to remove different pollutants from water, and particularly, to ganese, and inorganic compounds stand out among the contaminants that
treat surface waters. But, there is a scarce number of demonstration plants are also removed. Also, the pilot situated in Australia has installed thermal
Table 8
Characteristics of groundwater treatment plants.
Region Process Capacity Pollutants removed Opening Ref
(m3/day) year
Asia India biofilm reactor, flocculation, precipitation, 528 BTEX, MIBK, chlorinated 2011 (“Züblin Umwelttechnik GmbH -
deferrization, lamella separator, gravel compounds, phenols, Groundwater Treatment Plant”, 2021)
filter, filtration activated carbon, sludge nitroaromatics, anilines,
treatment, thickener, chamber filter press pesticides, hydrocarbons
New Delhi Aeration, lime softening, coagulation, 4536 bicarbonate hardness n. a. (Pillai et al., 2019)
flocculation, clarification, pH adjust, UF, removal, suspended
disinfection (UV or chlorine) particles, colloids and
harmful microorganisms
Saudi Buraydah, Coagulation, UF, Sand filtration, RO TDS, Fe, Mn n. a. (Haider, 2017)
Arabia Qassim region
America Canada White Rock Pre-oxidation with ozone, filtration, Mn, As 2019 (“Water Treatment Plant | White Rock,
adsorption BC”, 2021)
Ecuador RO 336 2013 (“Industrial Reverse Osmosis Equipment
87,000 GPD - Ecuador - Pure Aqua, Inc.”,
2020)
Haiti RO, activated carbon 216 Salts n. a. (“Groundwater Treatment Plant 57000 GPD
- Haiti - Pure Aqua, Inc.”, 2021)
USA Jordan, Utah RO, UV 26,496 TDS and Chemical 2011 (“Southwest Groundwater Treatment Plant
impurities - Flatiron”, 2021)
Lary Lane, Filtration, chemical compounds for 5904 Fe, Mn, As 2015 (“Lary Lane Ground Water Treatment Plant
Exeter NH co-precipitation, pH adjustment and | Town of Exeter New Hampshire Official
disinfection Website”, 2020)
Jacksonville NF, bio scrubbing system, disinfection, pH 15,142 2011 (“City Water Plant | Jacksonville, NC -
(North Carolina) adjust Official Website”, 2021)
Scottsdale RO, airstripping technology Trichloroethylene In (“City of Scottsdale - City Construction
(Arizona) construction Projects - Thomas Groundwater Treatment
Facility and Improvements to the Central
Groundwater Treatment Facility”, 2021)
Santa Mónica Pretreatment, RO, aeration 32,160 Mehtyl tert-butyl ether 2010 (“Santa Monica Public Works - Santa
(California) Monica Water Treatment Plant”, 2021)
Davie (Florida) Ion exchange 37,848 n. a. (“Water Treatment | Davie, FL”, 2020)
RO, aeration, disinfection n. a.
Orrington UF, granular activated carbon 312 Hg 2012 (“Groundwater Treatment Plant |
(Maine) beyondholtrachem”, 2021)
Europe Italy Porto Marghera Filtration, activated carbon 1320 Heavy metals, organic n. a.
chlorinated compounds
and aromatic compounds
Porto Torres Physico-chemical treatment, filtration, 1200 Heavy metals, organic n. a.
activated carbon chlorinated compounds
and aromatic compounds
Assemini Ion exchange 1320 Heavy metals, organic n. a.
chlorinated compounds
and aromatic compounds (“Trattamento Acque di Falda”, 2021)
Portovesme Physico-chemical treatment, activated 9600 Heavy metals, inorganic n. a.
carbon compounds and aromatic
compounds
San Gavino Physico-chemical treatment, activated 864 Heavy metals, organic n. a.
Monreale carbon compounds and
inorganic compounds
(sulphates)
Porto Torres Mechanical oxidation, UF 4800 n. a.
Poland Drzenin Aeration, filtration 1080 Fe, Mn 1977 (Jakubaszek, 2019)
Oceania Australia Botany Air stripping, thermal oxidizer, filtration, 6000 chlorinated 2006 (Orica, 2020)
biological aerated filters, granular hydrocarbons
activated carbon, filtration, RO
16
oxidizers within other processes and the Botany plant removes chlorinated the screening effects (Richards et al., 2010). Regarding the materials
hydrocarbons (Orica, 2020). The Orrington plant (Maine, United States of employed in ion exchange, Purolite A 520E has been considered the
America), although it has a small daily treatment capacity, is worth to men- most effective ion exchange resin to remove nitrates (Samatya et al.,
tion because the main element that is removed is mercury (“Groundwater 2006).
Treatment Plant | beyondholtrachem”, 2021). Membrane technology, along with ion exchange, has less efficiency than
Among the different technologies available to remove nitrates, no one is the catalytic process in the degradation of pollutants but has lower costs, au-
fully implemented or stands out clearly from the others. Table 9 summa- tomatization is more accessible, and has fewer control needs. For its part, ad-
rizes the main advantages and drawbacks of the technologies existing in sorption has been analyzed by several authors and the different adsorbents
each type of approach. In this way, despite the scarcity of data regarding ni- studied are carbon-based sorbents, natural sorbents (i.e. zeolite or clays), ag-
trate removal values, great efforts are being made at the laboratory level to ricultural wastes (i.e. sugar bagasse), industrial wastes (i.e. red mud),
find out the optimal figures of merit for each technology with associated biosorbents (i.e. bamboo power) or miscellaneous sorbents (i.e. double lay-
strengths and weaknesses. ered hydroxides, silica or alumina). In this sense, double layered hydroxides
There are two foremost approaches, i) the separation of nitrates from or modified chitosan report higher uptake of nitrate than conventional ad-
the water (reverse osmosis, ion exchange, and electrodialysis) and ii) the sorbents such as carbon-based sorbents (carbon nanotubes, activated car-
transformation of nitrates into harmless nitrogen gas (biological denitrifica- bon) or natural sorbents (clay, zeolite) (Bhatnagar and Sillanpää, 2011).
tion, and catalytic methods). Regarding the first alternative, the separation Soías-Viciana et al. (2008) removed nitrates from water using calcinated
requires a second step to remove, concentrate or neutralize the target com- hydrotalcite-type compounds. On the other hand, Chatterjee et al. (2009)
pounds. studied chitosan as adsorbent to remove nitrates. They achieved an adsorp-
In the case of reverse osmosis, the membranes that are commonly tion capacity of 104 mg/g using crosslinked chitosan beans while the re-
employed are polyamide and cellulose triacetate (Hosseini et al., ported adsorption capacity of normal chitosan beans is of 90.7 mg/g
2016). Schoeman and Steyn (2003) achieved, approximately, 98% ni- (Chatterjee et al., 2009). In the case of electrodialysis, Aliaskari and
trate removal using this membrane technology (Schoeman and Steyn, Schäfer (2020) studied this process to remove salinity, nitrates, fluoride
2003). Contrarily, Richards et al. (2010), studied the influence of pH and arsenic. They concluded that the removal of contaminants followed
to remove nitrates concluding that this parameter does not affect the re- the order, nitrate = salinity > fluoride > arsenic. These authors, ob-
tention of nitrates but suffers a decrease in the presence of Na+ due to tained a high nitrate removal with low electrical potential while arsenic
Table 9
Advantages and drawbacks of the main technologies for nitrates removal.
Technology Advantages Drawbacks Ref
Separation Reverse - Compact equipment - Fouling (to reduce it, sulfuric acid and sodium (Archna et al., 2012; Häyrynen et al., 2009; Schoeman and
osmosis - Continuous hexametaphosphate) Steyn, 2003; Sharma and Bhattacharya, 2017; Tokazhanov
operation is possible et al., 2020)
- Not necessary
post-treatments
Ion exchange - Simplicity - Lower affinity of resins to nitrates with respect to sulphates (Kabay et al., 2007a, 2007b; Primo et al., 2009; Samatya
- Effectiveness et al., 2007, 2006; Sharma and Bhattacharya, 2017;
- Selectivity Tokazhanov et al., 2020)
- Recovery
- Relatively low cost
Adsorption - Ease of operation - Necessity of take into account some factors: i) initial (Bhatnagar and Sillanpää, 2011; Sharma and Bhattacharya,
- Simplicity of design nitrate concentrations, ii) other ions present in water, iii) 2017)
- Remove different adsorbent quantity, iv) water pH, v) operation and
types of maintenance and vi) temperature
contaminants,
organics and
inorganics
Electrodialysis - Higher taxes of - Necessary to consider time, temperature, flow rate, and (Aliaskari and Schäfer, 2020; el Midaoui et al., 2002; Sharma
recovery voltage to optimize and Bhattacharya, 2017)
- May remove - Process
contaminants and - Efficiency loss due to the fouling and scaling
desalinate - The need for a pretreatment remineralization requirements
simultaneously
- Environmentally
friendly technology
Transformation Biological - Economical - High levels of nitrate concentration may be difficult to (Chu and Wang, 2013; Ghafari et al., 2008; Martínez et al.,
denitrification - Environmentally reduce 2017; Sharma and Bhattacharya, 2017; Tokazhanov et al.,
friendly technology - Long time 2020; Xu et al., 2018; Yang et al., 2019)
- Bacteria sludge
- High pH requirements
- Low selectivity
- Higher energy requirements
Catalytic - Nitrate conversion - Formation of ammonia (Ghosh et al., 2017; Guate et al., 2019; Liu et al., 2012;
reduction of 98–100% - High operational costs Marchesini et al., 2019; Martínez et al., 2017; Pizarro et al.,
- No waste 2018; Sharma and Bhattacharya, 2017; Tokazhanov et al.,
2020; Zhou et al., 2017)
Electrocatalytic - Versatile - Requirement of certain conductivity (Akbari et al., 2020; Garcia-Segura et al., 2018; Martínez
reduction - Scalable et al., 2017; Sanjuán et al., 2020; Tokazhanov et al., 2020;
Weber et al., 2019)
Photocatalytic - High selectivity - Formation of nitrite and ammonium (Kozyatnyk and Klymenko, 2016; Sharma and Bhattacharya,
method 2017; Zhang et al., 2005)
17
elimination increases with high electrical potential (Aliaskari and scale installations in contrast to catalytic reduction and this technol-
Schäfer, 2020). ogy does not produce ammonia (Rezvani et al., 2019). Only a pilot
However, the use of techniques to transform nitrates to N 2 , has plant located in Borrasa (Spain) has been currently reported in the
the advantage of no waste production. Biological denitrification literature (“Breakthrough in Nitrate-polluted Water Treatment”,
can be heterotrophic or autotrophic. On the one hand, heterotrophic 2021).
bacteria need the presence of organic compounds or hydrocarbons as Regarding pilot plants for nitrates removal based on separation or
energy and carbon source. On the other hand, autotrophic bacteria transformation technologies, there are several plants developed
use inorganic compounds, usually carbon dioxide as carbon source, throughout the world. Nevertheless, these plants, in many cases, are
and electron donors like hydrogen or reduced sulfur compounds as only dedicated to the treatment of surface waters. Table 10, shows
energy source. In this context, autotrophic denitrification using hy- the main pilot or full-scale plants installed to treat nitrates. This
drogen as electron donor is called hydrogenotrophic denitrification table collects the data reported in the bibliography for nitrate treat-
(Ghafari et al., 2008). Lee and Rittmann (2000) developed a hollow ment plants; in many cases, other compounds are removed at the
fiber membrane biofilm reactor capable of removing nitrate using same time. In view of the results, it is important to highlight, i) the
hydrogen as electron donor (Lee and Rittmann, 2000). Zhou et al. treatment capacity of the plants offers high variability, from 18 m 3
(2017) developed a hollow fiber membrane reactor combining bio- per day in Spain using the electrodialysis reversal technology to
film with a palladium catalyst achieving a reduction of nitrates faster 38,400 m 3 in Germany employing biological denitrification, ii) the
than using only biofilm or only the palladium catalyst and they re- lack of data regarding the nitrate removal yield, iii) the high number
ported a selectivity toward nitrogen gas (Zhou et al., 2017). In con- of plants installed in the USA based on the ion exchange technology
trast, catalytic reduction employs a bimetallic catalyst consisting of and, iv) Asia and Africa, with large regions contaminated by nitrates,
a noble metal and a transition metal. These catalysts are usually only have two plants dedicated to nitrates removal. On the other
composed of palladium or platinum and copper, tin or indium. The hand, it is worth to mention the high differences in terms of capacity
reaction occurs with hydrogen as reducing agent and carbon dioxide per day of reverse osmosis plants.
is commonly used as buffer to control pH (Martínez et al., 2017). Al-
though this method achieves high nitrate degradation yields, the 5. Conclusions
chemical catalytic process is not implemented yet at full-scale. Cur-
rently, Marchesini et al. (2019) compared PdIn/SiO 2 and PdIn/ This review collects the quality of different groundwater bodies
Al2O 3 catalysts to reduce nitrates from real water, that is, in the pres- throughout the world in terms of nitrates concentration and reports the
ence of other anions such as sulphate, carbonate or chloride. They treatment options both for this compound and for other critical pollutants,
concluded that for PdIn/SiO 2 the presence of other anions decreases identifying the pilot plants that are currently in operation.
the nitrate reduction yield and the selectivity toward nitrogen gas After analyzing a total of up to 292 points from 146 works reported
while for PdIn/Al 2 O 3 , the presence of other anions only diminishes in the literature, some general conclusions can be drawn: i) The pres-
the selectivity toward nitrogen gas (Marchesini et al., 2019). Control ence of nitrates in groundwater is continuously growing, and in conse-
of pH has been studied by Pizarro et al. (2018) using CO2 as buffer quence, urgent measures are required to avoid the degradation of these
gas. They achieved 100% of conversion using PdIn/Al 2 O 3 catalyst water bodies. ii) Different areas worldwide present values higher than
with and without CO 2 buffer but the selectivity toward ammonia the WHO standards (50 ppm). iii) Nitrate pollution coming from agri-
was 34% and 92% respectively (Pizarro et al., 2018). Additionally, culture and, specifically, from the use of fertilizers and pesticides is a
zero-valent iron (ZVI) has been used as catalyst too. ZVI, in presence common denominator on all continents. iv) In Asia, there is significant
of nitrates, is oxidized to form Fe2+ /Fe 3+ and nitrates are reduced variability in the concentration of NO− 3 because of the strong influence
to form nitrites, nitrogen or ammonia (Dominguez et al., 2018; of the rainy season and the poor treatment of septic tanks. v) In addition
Martínez et al., 2017). Ghosh et al. (2017) achieved 72–100% of ni- to contamination by fertilizers, aquifers in America suffer from waste-
trate reduction with a selectivity higher than 99% toward ammonia water discharged without adequate treatment. vi) In Europe, landfills,
(Ghosh et al., 2017), while Liu et al. (2012) reached 90% nitrate re- industrial activities, and sewage have an outstanding contribution to
duction with nitrogen gas as the main product, together with 20% nitrate presence in groundwater. vii) In Africa, apart from the different
selectivity toward ammonia and a small number of nitrites (Liu reasons previously summarized, pollution is mostly due to the poor
et al., 2012). health conditions in many countries (e.g., the presence of septic tanks
The electrocatalytic reduction of nitrates to nitrogen or ammonia without treatment).
is another alternative. The reaction occurs in the cathodic surface Nowadays, there is a high number of plants dedicated to surface
which acts as a catalyst too. The main configurations to remove ni- water treatment, nevertheless, the number of plants for groundwater
trates using this technology are single chamber cell, where cathode treatment is still very limited. Regarding the different treatments to re-
and anode are in the same compartment and in contact with the elec- move nitrates, continue research is necessary since, although there are
trolyte, and dual-chamber cell, where a membrane separates the elec- many technologies available, scarce applications have reached the
trodes (Martínez et al., 2017). Several authors have researched this pilot plant scale. Also, between all the technologies that are currently
process to eliminate nitrates. Weber et al. (2019) achieved 99% and under development, there is not a clear line because all present clear
90% of nitrate conversion with 81% and 78% of selectivity toward ni- advantages and disadvantages. In the case of reverse osmosis, com-
trogen gas using CuSn and CuPd as cathode, respectively (Weber monly used to remove pollutants from surface water, the degradation
et al., 2019). Akbari et al. (2020) secured 90% of nitrate conversion of the membranes by fouling and the fact that nitrate is not converted
with a nitrogen selectivity of 88.8% employing Fe0/Fe3O4 over nickel to nitrogen prevents it from being the most promising technology. On
foam as cathode (Akbari et al., 2020). However, the photocatalytic the other hand, apart from reverse osmosis, biological denitrification
method to remove nitrates is still in its infancy due to the formation and ion exchange are the main treatments implemented at full-scale
of nitrite and ammonium as byproducts; promising results have been to nitrate removal. However, these technologies have the drawback
published by Zhang et al. (2005) who reported 100% selectivity to- of the difficult nitrate removal at high concentration. Catalytic nitrate
ward nitrogen gas with Ag/TiO2 with fine Ag cluster catalyst (Zhang reduction, which still needs further research, is a promising technol-
et al., 2005). ogy for the destruction of nitrates due to the high conversion close to
Regarding transformation techniques, catalytic reduction pre- 98–100%, and no waste generation. Thus, despite there is still a long
sents more advantages than biological denitrification such as high ni- way to achieve full groundwater remediation, the efforts which are
trates removal rates. However, biological denitrification has full- currently being performed will promote short-term responses.
18
Table 10
Nitrate treatment plants at full-scale.
Location Capacity Nitrates removed Opening Ref.
(m3/day) (mg/L) year
Reverse osmosis Bakersfield (California) 654 75–84 n. a. (Jensen et al., 2014)

Brighton (Colorado) 25,075 49–89 n. a.
Arlington Desalter, Riverside (California) 24,982 44–89 n. a.
Yemen 169 n. a. (Shams, 2010)
France 120 n. a.
Zava-Giyani (South Africa) 54.5 n. a.
Milan (Italy) (13 sites) 169–1352 n. a.
Pomaire (Chile) 518 2015 (“Reverse osmosis dwtp for nitrate removal, pomaire,
chile – wes chile – water & energy solutions”, 2021)
Ion exchange Ellsworth (Minnesota) 178 1994
Clear Lake (Minnesota) 178 1995
Edgerton (Minnesota) 519 2002
Adrian (Minnesota) 488 1998
McCook (Nebraska) 25,741 > 125 2006
McFarland (California) 3785 60 1983
(Jensen et al., 2014)
McFarland (California) 3785 64 1987
La Crescenta (California) 10,221 70–100 1987
Grover City (California) 8706 80–130 n. a.
Des Moines (Iowa) 37,854 >55 1992
Glendale (Arizona) 37,854 177 2010
Indian Hills (Colorado) 272.5 53–71 2009
Avondale (Arizona) 10,357 2003
Salinas (California) 16,353 2002
East Valley, San Bernardino Highland (California) 5451 2003
(Shams, 2010)
Yucca Valley (California) 13,627 2002
Pomona (California) 5451 Late 1990s
- (California) 10,902 n. a.
Colina (Chile) 630 n. a. (“Nitrate removal dwtp, colina, chile – wes chile –
water & energy solutions”, 2020)
Electrodialysis Spain 18 80 n. a. (Jensen et al., 2014)
Selective reversal Israel 1690 84–89 n. a. (Jensen et al., 2014)
Biological denitrification Rialto (California) 10,901 17–19 n. a.
Riverside (California) 9102 44–89 n. a.
Obersiebenbrunn (Austria) 4320 n. a.
Chateau Landon (France) 1248 n. a.
Champfleur (France) 1680 n. a.
Issoudun (France) 14,000 n. a.
Bourg les valences (France) 10,800 n. a.
Nord Sarthe (France) 7200 n. a.
Dreux-Vernouillet (France) 16,800 n. a.
Niort (France) 48,000 n. a.
Thouard (France) 20,400 n. a. (Jensen et al., 2014)
Vernoy (France) 4800 n. a.
Hanau (Germany) 1200 n. a.
Neuss (Germany) 3600 n. a.
Frankfurt Airport (Germany) 7680 n. a.
Aschaffenburg (Germany) 38,400 n. a.
Föhr Island (Germany) 2160 n. a.
Albanacci (Italy) 9120 n. a.
Czestochowa (Poland) 12,000 n. a.
Rancho Cucamonga (California) 3600 n. a.
Coyle (Oklahoma) 300 n. a.
Falset (Spain) 120 2018 (Alvarez and Murría, 2020)
Republic (Washington) 272 2006
Republic (Washington) 32,7 2005
Cajamarca (Perú) 1199 2003 (Reinsel, 2014)
Lead (Dakota del Sur) 2180 1997
Nye (Montana) 13,082 1995
Langenfeld and Monheim (Germany) n. a.
Monchengladback (Germany) n. a.
Vsetaty (Czech Republic) n. a.
(Shams, 2010)
Drosing (Austria) n. a.
Montferland (the Netherlands) n. a.
Blankaart (Belgium) n. a.
Electrocatalytic reduction Borrassà (Spain) 100 2017 (“Breakthrough in Nitrate-polluted Water
Treatment”, 2021)
CRediT authorship contribution statement I. Ortiz: Writing - Review & Editing, Supervision, Funding
acquisition
E. Abascal: Formal Analysis, Investigation, Writing - Original Draft A. Ortiz: Conceptualization, Investigation, Writing - Review & Editing,
L. Gómez-Coma: Methodology, Investigation, Writing - Original Draft Supervision, Project administration, Funding acquisition
19
Declaration of competing interest Anim-Gyampo, M., Anornu, G.K., Appiah-Adjei, E.K., Agodzo, S.K., 2018. Hydrogeochemical
evolution and quality assessment of groundwater within the atankwidi basin: the case of
northeastern Ghana. Arab. J. Geosci. 11. https://doi.org/10.1007/s12517-018-3753-6.
The authors declare that they have no known competing financial Archna, Sharma, S.K., Sobti, R.C., 2012. Nitrate removal from ground water: a review.
interests or personal relationships that could have appeared to influence E-J. Chem. 9, 1667–1675. https://doi.org/10.1155/2012/154616.
Arsénio, A.M., Salim, I.C., Hu, M., Matsinhe, N.P., Scheidegger, R., Rietveld, L., 2018. Mitiga-
the work reported in this paper. tion potential of sanitation infrastructure on groundwater contamination by nitrate in
Maputo. Sustainability (Switzerland) 10, 1–18. https://doi.org/10.3390/su10030858.
Acknowledgments Ashun, E., Bansah, K.J., 2017. Groundwater quality index of upper Athi river basin in Kenya.
Int. J. Glob. Environ. Issues 16, 217–230. https://doi.org/10.1504/IJGENVI.2017.
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This work has been conducted with financial support from the Spanish Asmael, N.M., Huneau, F., Garel, E., Celle-Jeanton, H., le Coustumer, P., Dupuy, A., Hamid, S.,
Ministry of Economy and Competitiveness (project RTI2018-093310-B- 2015. Origin and recharge mechanisms of groundwater in the upper part of the Awaj
River (Syria) based on hydrochemistry and environmental isotope techniques. Arab.
100). This research is also being supported by the Project “HYLANTIC”-
J. Geosci. 8, 10521–10542. https://doi.org/10.1007/s12517-015-1953-x.
EAPA_204/2016, which is co-financed by the European Regional Develop- Atikul Islam, M., Zahid, A., Rahman, M.M., Rahman, M.S., Islam, M.J., Akter, Y.,
ment Fund in the framework of the Interreg Atlantic program. E. Abascal is Shammi, M., Bodrud-Doza, M., Roy, B., 2017. Investigation of groundwater quality
supported by the Spanish Ministry of Science, Innovation and Universities and its suitability for drinking and agricultural use in the south central part of the
coastal region in Bangladesh. Expo. Health 9, 27–41. https://doi.org/10.1007/
through the grant PEJ2018-003323-A. s12403-016-0220-z.
Awomeso, J.A., Ahmad, S.M., Taiwo, A.M., 2020. Multivariate assessment of groundwater
Appendix A. Supplementary data quality in the basement rocks of Osun State, Southwest, Nigeria. Environ. Earth Sci. 79,
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Science of the Total Environment 810 (2022) 152233

Contents lists available at ScienceDirect

Science of the Total Environment

Global diagnosis of nitrate pollution in groundwater and review of

• 272 regions worldwide are analyzed to a

1. Introduction In contrast, the inordinate use of fertilizers and pesticides in agriculture

Fig. 1. Nitrogen cycle.

Groundwater polluon Nitrates in groundwater

Number of regions with [NO−3 ] average > 50 ppm 20 1 9 30 60

Fig. 6. Risk of nitrate pollution in groundwater aquifers in USA.

Reverse osmosis Bakersﬁeld (California) 654 75–84 n. a. (Jensen et al., 2014)

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