Atmospheric Pollution Research xxx (2017) 1e9

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Atmospheric Pollution Research

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Wet deposition fluxes of atmospheric inorganic reactive nitrogen at an

urban and rural site in the Indo-Gangetic Plain
Saumya Singh, Anshu Sharma, Bablu Kumar, U.C. Kulshrestha*
School of Environmental Sciences, Jawaharlal Nehru University, New Delhi, 110067, India

a r t i c l e i n f o a b s t r a c t

Article history: Excess nitrogen deposition is a matter of concern for sensitive ecosystems. However, understanding the
Received 11 June 2016 sources and transport of Nr species has been a challenge due to limited observations of atmospheric
Received in revised form deposition of the key Nr species across India. In this study, wet deposition of atmospheric inorganic Nr
22 December 2016
species was investigated during the year 2013 at two regionally representative sites: Delhi (an urban site)
Accepted 25 December 2016
and Jaunpur (a rural site). These sites are located in the Indo-Gangetic Plain (IGP) region, which is one of
Available online xxx
the most populated and fertile regions of India. The average NHþ 4 concentrations in rain water were found
to be 25.4 meql1 and 98.5 meql1 at the rural and urban sites, respectively, whereas average NO 3 con-
Keywords:
Wet deposition flux
centrations were 12.4 meql1 and 28.7 meql1 at the rural and urban sites (respectively). The annual
Nitrogen average wet deposition fluxes of NHþ 
4 and NO3 at Delhi were calculated as 10.45 and 3.05 kgN ha
1
yr1
Indo-Gangetic Plain respectively, whereas at Jaunpur the fluxes were 3.19 and 1.56 kgN ha1 yr1 respectively. In order to
Delhi assess the Nr deposition, our estimates showed 486% increase in NO 3 (from 0.52 to 3.05 kgN ha
1
yr1)
LULC while 283% NHþ 4 (2.72e10.44 kgN ha
1
yr1) between 1994 and 2013 at Delhi, clearly indicating the
Agriculture effect of urbanization and Land Use Land Cover (LULC) change. Reduced versus oxidized N deposition
contribution was also estimated. This study provides key quantitative information to support regional
nitrogen budget estimates in south Asia.
© 2017 Turkish National Committee for Air Pollution Research and Control. Production and hosting by
Elsevier B.V. All rights reserved.

1. Introduction activities have drastically accelerated the nitrogen (N) cycle,

Nitrogen oxides (NOx) and ammonia are the key reactive ni-
trogen (Nr) species in atmospheric chemistry and ecosystem
productivity. Although the major source of ammonia in the at-
mosphere is agriculture, other sources can include industry,
landfills, household products, biomass burning, motor vehicles,
and even wild animals (Ianniello et al., 2010). Before 1995, the
contribution of vehicles to non-agricultural NH3 emissions was
negligible, but in recent times NH3 concentrations in urban en-
vironments have also increased due to the over-reduction of ni-
trogen oxide compounds in catalytic converters of automobile
exhaust and industrial power stations (Sutton et al., 1995; Sutton
et al., 2000). Fossil fuel emissions and intensive agricultural
* Corresponding author.
E-mail address: umeshkulshrestha@gmail.com (U.C. Kulshrestha).
Peer review under responsibility of Turkish National Committee for Air Pollu-
tion Research and Control.
resulting in increasing deposition rates of N species (Galloway
et al., 2008; Penuelas et al., 2012; Canfield et al., 2010).
Increasing Nr deposition has many adverse effects on human
health, vegetation health, air quality, soil acidification, eutrophi-
cation, and most importantly global climate change (Sutton et al.,
1994; Sun et al., 2004; Ianniello et al., 2011). Further, it affects the
global carbon cycle (Goulding et al., 1998; Galloway et al., 2004).
Once the reactive nitrogen species are released into the atmo-
sphere, their fate is decided by several processes such as trans-
formation, transport, and deposition. Nr species are deposited
either through dry deposition or wet removal processes. Despite a
long history of precipitation composition measurements (almost
150 years), the spatial and temporal variations of atmospheric Nr
deposition remain unclear due to the complexity of reactions
during transport and deposition (Park and Lee, 2002). Neverthe-
less, the wet deposition of Nr species has been studied by a
number of groups as part of acid deposition studies. Available
research indicated N deposition reached 70 Tg yr1 N and

http://dx.doi.org/10.1016/j.apr.2016.12.021
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Please cite this article in press as: Singh, S., et al., Wet deposition fluxes of atmospheric inorganic reactive nitrogen at an urban and rural site in
the Indo-Gangetic Plain, Atmospheric Pollution Research (2017), http://dx.doi.org/10.1016/j.apr.2016.12.021
2 S. Singh et al. / Atmospheric Pollution Research xxx (2017) 1e9
averaged 5 kg ha1 yr1 N at the global scale (Holland et al., 1999;
Galloway et al., 2004). Asia including India has the third highest N
deposition rates, following North America and Europe (Holland
et al., 1999; Galloway and Cowling, 2002).
The reported studies suggest that the Indo-Gangetic Plain (IGP)
is a major hotspot of Nr deposition in India (Galloway et al., 2004;
Kulshrestha et al., 2005; Van et al., 2011; Vet et al., 2014). The IGP
is one of the most densely populated and polluted regions in the
world, consequently having increasing emissions. Use of tradi-
tional biofuels for cooking and heating purposes in rural areas in
the IGP leads to significant air pollution (Singh et al., 2014). One of
the most powerful causes of high pollution load in the IGP is rapid
urbanization, which results in high emissions of N-containing
pollutants and affects levels of atmospheric N deposition (Lovett
et al., 2000; Liu et al., 2008). In Europe and the United States,
urban areas tend to receive higher rates of N deposition than rural
areas (Lovett et al., 2000; Power and Collins, 2010). Similar to
many Indian cities, Delhi (the urban site of the present study) is
experiencing a high growth rate. During the last two decades
(from 1991 to 2011), the population of Delhi is increased by
approximately 169% (Table 1).
In order to sustain the increasing population, humans are
drastically changing land use land cover (LULC) as well. LULC
change has been linked to high dust fall fluxes in Delhi, ultimately
affecting the air quality (Kumar et al., 2014). Urbanization and land
use changes have resulted in temperature increases in the USA
during the last several decades, ultimately affecting the climate
(Kalnay and Cai, 2003). In China, diurnal temperature differences
have decreased due to land cover change leading to change in
regional climate (Zhou et al., 2004). These land use practices also
affect air quality by altering emissions and changing the atmo-
spheric conditions that affect reaction rates, transport, and depo-
sition of pollutants (Sillman, 1999).
Delhi is facing an issue of increased traffic emissions due to a
tremendous increase in the number of vehicles on the road (Goyal
et al., 2013). Being capital, Delhi city has been a location of common
concern but unfortunately, the city is not covered by any systematic
and long term measurement network of wet deposition of reactive
nitrogen species. This is also true for rural areas. Along with highly
populated cities, rural sites in the IGP are important contributors to
Nr emissions due to extensive agricultural practices and use of
synthetic fertilizers. Hence, the present study is an attempt to
measure the wet N deposition levels in one of the world's most
polluted cities (Delhi) along with the measurements at a rural site
in Jaunpur district of Uttar Pradesh state. This study reports the
measurements of wet deposition of inorganic Nr species at an ur-
ban and a rural site in Indo-Gangetic plain, providing Nr estimates
from a rather large area through these regionally representative
sites. In addition, in order to observe the influence of two decades
of land use change and urbanization on Nr fluxes, this study com-
pares the present deposition fluxes of Nr species at Delhi with
observations reported for 1994.
Table 1
Descriptive statistics of demographic change of Delhi between 1991 and 2011.
Area type Census year
1991 2011
Population 6,220,406 1,67,53,235
Rural 452,206 4,19,319
Urban 5,768,200 1,63,33,916
Population density (person km2) 6352 11,297
Category 1994 2013e14
Motor vehicle No.* 24,32,295 82,93,167
Source*: Transport department, Govt. of NCT of Delhi.
Please cite this article in press as: Singh, S., et al., Wet deposition fluxes of atmospheric inorganic reactive nitrogen at an urban and rural site in
the Indo-Gangetic Plain, Atmospheric Pollution Research (2017), http://dx.doi.org/10.1016/j.apr.2016.12.021
2. Methodology
2.1. Site description
Two sites having different land use, land cover, sources and
population density located in Indo-Gangetic plains in India were
selected for this study. The Delhi site is representative of urban
areas whereas the Jaunpur site, in the adjacent Uttar Pradesh state,
represents rural areas (see Fig. 1). Basic information regarding both
the sites is given below.
2.1.1. Delhi (urban site)
In Delhi, Jawaharlal Nehru University (latitude
0 00 0 00 0 00 0 00
28 31 30 e28 33 30 and longitude 77 9 0 7711 0 ) was
selected as the urban representative site. According to several re-
ports, Delhi is the most polluted city in the world (Gargava et al.,
2014; Pant et al., 2015). The main sources of pollution in Delhi are
thermal power plants, on-road transport, small-scale industries,
and domestic cooking/heating activities (Khillare et al., 2004;
Chowdhury et al., 2007; Lelieveld et al., 2001; Chelani et al.,
2010; CPCB, 2010). The air quality of Delhi is most affected by
vehicular exhaust (Verma and Kulshrestha, 2015; Bisht et al., 2013;
Dholakia et al., 2013). The sampling site was located at the School of
Environmental Science (SES) building, Jawaharlal Nehru University,
New Delhi. The JNU campus lies in the southernmost section of
Delhi, and is surrounded by a very small forested area.
2.1.2. Juanpur (rural site)
0 00 0 00
Mai village (25 37 23.5 N, 82 51 10.1 E), in Jaunpur, was selected
for the study, which is 885 km from Delhi. The total area of the
village is 617 ha, out of which 385 ha land (approximately 62%) is
used for agricultural purpose. The area around the site is dominated
by agricultural activities, thus it is an excellent representative
location for the study of reactive nitrogen emissions from urea and
DAP fertilizer applied in agricultural fields. A few industrial estab-
lishments are located at a distance of 13 km from the village
including one vegetation oil production factory to the southeast
(Singh and Kulshrestha, 2014).
2.2. Sample collection
Sampling was conducted at the terrace of the School of Envi-
ronmental Science building (~23 m height) at the university
campus in Delhi, and on a house roof (~20 m) at the rural site,
Jaunpur. An assembly of polythene funnel of 20 cm diameter fitted
onto 2 L capacity polythene bottle was used for rain water collec-
tion at both the locations. The sampling occurred during the
southwest monsoon (SW monsoon) of 2013. The SW monsoon
occurs from July through September. Monsoon rainfall accounts for
about 80% of the total annual precipitation in India and is a major
factor controlling water resources, agriculture, and ecosystems
(Gadgil and Kumar, 2006). It is characterized by huge spatial vari-
ability, which is largely a function of topography. The samples were
collected manually during rainfall events using pre-washed plastic
bottles and funnels (Kulshrestha et al., 2003a). The collection as-
semblies were placed at about 1.5 m above the roof and were
deployed as soon as the rain began, and were retrieved immedi-
ately after the rain stopped. After each sample, the bottle and
funnel were cleaned with deionized water to avoid any residual
contamination.
Collected samples were stored in prewashed small polythene
bottles of 60 ml volume. A small amount of thymol was added to
each sample to prevent biological degradation (Gillet and Ayers,
1991; Granat et al., 1992; Koshy et al., 1993; Kulshrestha et al.,
2005). For each event, two samples of 30 ml volume were kept
 S. Singh et al. / Atmospheric Pollution Research xxx (2017) 1e9 3

for replicate measurements and to improve the quality of data. A
“blank” to characterize data artifacts from washing the collection
device was collected after thoroughly washing the funnel. A dry
deposition blank of 60 ml deionized water was collected by
washing the funnel after 6 h to check interference to dry deposition
measurements. A small amount of thymol was added to these
blanks. Both blanks were analyzed for major anions and cations. In
the analysis, all major ions were found below detection limits in
both the blanks. A total of 47 samples (21 from urban and 26 from
the rural site) were selected for chemical analysis and were
refrigerated at 4  C in the laboratory before analysis. The pH of the
samples was measured immediately after the collection. The pH
was measured by using a Eutech PC 510 pH meter. Standard cali-
bration solutions/buffers were used for the calibration of pH. Un-
certainty in pH measurements of rural site samples is expected due
to occasional delay of the pH measurement.
2.3. Chemical analysis
The major cations (Naþ, NHþ þ 2þ 2þ
4 K , Ca and Mg ) and major
  2
anions (Cl , NO3 and SO4 ) were analyzed by ion chromatography
(Metrohm). The anions were determined by using Metrosep A SUPP
4, 250/4.0 column and an eluent of 1.8 mmol L1 Na2CO3 and
1.7 mmol L1 NaHCO3 at a flow rate of 1.0 ml/min with Metrohm
limits, thereby indicating that no significant contamination of the
rain samples occurred during the sampling, handling, filtration, or
measurement steps. Prior to the injections, all the samples were
filtered through syringe filters of pore size 0.2 mm.
2.4. Data quality and analysis
Ion balance is an important parameter for data quality assess-
ment. It gives an indication of the quality of analysis as well as the
possibility of any missing parameters. The acceptable USEPA range
of ion difference in rainwater samples is 15e30% for samples having
ion sum >100 meqL1 (Ayers, 1995; Kulshrestha et al., 2005). In this
study, the average percentage of ion difference was observed to be
16.57% for rural samples and 23.75% for urban samples, indicating
good quality of data. Also, the precision values were observed to be
0.23% for Naþ, 1.23% for NHþ þ 2þ
4 , 0.17% for K , 0.37% for Ca , 0.7% for
 
Mg2þ, 2.18% for SO2 4 , 2.13% for NO3 , 1.6% for Cl and 0.79% for F-,
indicating good data quality.
In order to calculate the wet deposition flux of nitrogen species,
the measured concentration (mg/l) of each nitrogen species was
multiplied by the volume (l) of collected water and the resultant
was divided by the opening area (0.0314 m2) of the funnel
(Kulshrestha et al., 2003b). This can be expressed as the follows:

  Concentration of speciesðmg=lÞ  Precipitation volumeðlÞ  104

Flux kg ha1 y1 ¼
0:0314m2  106

suppressor technique. The cation separation was achieved with the Annual precipitation for Delhi and Jaunpur was taken as
Metrosep C4-100/4.0 column and an eluent of 1.7 mmol l1 Nitric 758 mm and 897 mm, respectively, from IMD report for the year
acid and 0.7 mmol l1 dipicolinic acid at a flow rate of 0.9 ml min1 2013. We collected 228 mm rain in Delhi and 211 mm rain at the
without a suppressor. The concentrations of ions were calculated rural site in Jaunpur. However, in order to estimate the average
based upon the peak area of standards that were prepared regularly annual wet deposition flux of Nr species, we applied a scaling factor
from the stock solutions. Calibration of the method andquantifi- of 3.32 (758/228) for Delhi and 4.24 (897/211) for Jaunpur. Then the
cation of components were carried out using MERCK reference average wet N deposition fluxes of each nitrogen species were
standards (CertiPUR). Typical standard concentrations were estimated in kg N ha1 yr1.
noticed in the range of 0.5e10 ppm. The calibration was checked by
analyzing standard solution frequently. The detection limits (DL) of
3. Results and discussion
F, Cl SO2  þ þ þ
4 , NO3 , Na , NH4 , K ,Ca
2þ
and Mg2þ for our instrument
were calculated as 0.03, 0.75, 0.24, 1.13, 0.35, 0.29, 0.63, 0.85 and
3.1. Variation of NHþ 
4 and NO3
0.33 mg/ml, respectively. Field blanks were handled and analyzed in
the same way as other samples. The levels of all ions in the field
Nitrogen in precipitation is present mainly as ammonium (NHþ 4)
blanks and in rinses of the collection devices were below detection
and nitrate (NO
3 ) out of the total inorganic nitrogen (TIN) (Xie et al.,

Table 2
Concentrations (meqL1) of major ions in rain water at a rural (Jaunpur) and urban (Delhi) monitoring site.

NHþ
4 NO
3 SO2
4 Cl Naþ Kþ Ca2þ Mg2þ

Rural Mean 25.4 12.4 16.0 12.4 10.6 3.7 15.7 4.1
Max 72.7 37.4 40.6 23.9 39.6 9.0 42.2 14.7
Min 3.7 1.1 1.9 4.4 2.7 1.1 5.1 0.3
Median 23.7 11.3 13.4 12.4 8.5 2.9 13.3 3.6
1st quartile 12.9 6.2 24.1 8.9 5.1 2.2 7.9 2.2
3rd quartile 32.6 14.5 49.1 15.8 14.1 4.9 19.0 4.8
Size 26 26 26 26 26 26 26 26
Urban Mean 98.5 28.7 63.3 19.6 17.1 13.9 35.2 3.9
Max 179.4 68.8 162.4 63.2 40.4 101.0 112.1 14.6
Min 24.6 9.6 4.8 3.9 3.7 1.1 10.9 1.1
Median 92.0 23.2 84.4 13.9 17.4 5.9 28.9 3.7
1st quartile 75.0 12.3 50.3 9.7 11.2 3.9 22.0 2.1
3rd quartile 118.7 42.1 184.5 22.7 21.1 8.9 46.8 4.6
Size 21 21 21 21 21 21 21 21

Please cite this article in press as: Singh, S., et al., Wet deposition fluxes of atmospheric inorganic reactive nitrogen at an urban and rural site in
the Indo-Gangetic Plain, Atmospheric Pollution Research (2017), http://dx.doi.org/10.1016/j.apr.2016.12.021
4 S. Singh et al. / Atmospheric Pollution Research xxx (2017) 1e9

Fig. 1. Map showing locations of sampling sites.

2007). Table 2 gives the statistical description of major ions at the 2015). Although NO 3 concentration was noticeably higher at the
rural and urban sites. The concentration of NHþ 4 varied from 3.7 to urban site, the value of NO 3 at the rural site was also significantly
72.7 meql1 with an average of 25.4 meql1at the rural site, and high. At the rural site, NO
3 concentrations are high due to biomass
NO 1
3 concentrations varied from 1.1 to 37.4 meql with an average of burning, local and regional transport, and nearby factory activity
1 þ
12.4 meql . At the urban site, NH4 concentrations varied from 24.6 (Singh and Kulshrestha, 2014).
to 179.4 with an average of 98.5 meql1and NO 3 varied from 9.6 to
68.8 with an average of 28.7 meql1. Among all the ions, NHþ 4 had
3.2. Relationship between major anthropogenic ionic species
the highest concentration at both sites. This indicated that
increasing traffic and biomass burning with rapid urbanization
Linear regression analysis for major anthropogenic ions NHþ 4,
have significant influence at the urban site. On the other hand, at
NO 2
3 and SO4 exhibits characteristic trends at the rural and ur-
the rural site, agricultural activity and fertilizer application in the
ban sites (Fig. 2a and b). A Pearson correlation test was positive
fields are the major causes of high NHþ 4 values. The high density of
and significant (p < 0.01) for these ions at both the urban and
human population and agricultural activities are among the key
rural sites, with the exception of the correlation between NHþ 4
players for higher NHþ 4 values in the Indo-Gangetic region.
and SO24 which was not found to be significant (p value > 0.01).
Kulshrestha et al. (2005) have also reported higher concentrations
This difference is due to the difference in the crustal aerosol
of NHþ 4 in this region (the Northern Indian region) as compared to
loadings in the atmosphere. At most of Indian sites, the natural
other areas. Their results were supported by model output as well,
abundance of Ca2þ in the atmosphere is higher due to greater
in which higher deposition has been linked to regions with higher
presence of soil dust which plays an important role in scavenging
population density.
of SO2 having higher preference for calcium sulphate formation
According to Galloway (1995), agricultural activities in Asian
(Kulshrestha et al., 2003a). Due to this reason, the correlation of
regions are major contributors of NH3, similarly to North America
NHþ 2
4 vs SO4 is noticed weaker. However, after removal of dust
and Europe. Delhi and its surrounding areas such as Punjab, Har-
particulates through continuous rains, such co-variation of NHþ 4
yana, and Uttar Pradesh have dairy and grain production as major
with SO24 is reported stronger in India (Kulshrestha et al.,
activities which can be significant sources of atmospheric NH3.
2003a,c, 2009).
Hence, the higher concentrations of reactive nitrogen in Delhi can
In the reactions of gas phase NH3 with sulphuric acid (H2SO4)
be attributed to rapid urbanization and the transboundary effect.
and nitric acid (HNO3), gaseous NH3 reacts with H2SO4 forming
The NO 3 concentration was found to be higher by a factor >2 in the
(NH4)2SO4 or NH4HSO4 while its reaction with HNO3 gives rise to
urban site rain water as compared to the rural site. A possible
NH4NO3 formation (eqs. (1)e(3)). H2SO4 is formed when SO2 reacts
reason for this difference is higher emissions of NOx in Delhi city.
with H2O2 or O3 (depending upon the pH of the cloud droplet) and
Vehicular emissions are the major NOx contributors (Chelani and
NH3 can increase the reaction rate due to its influence on pH
Devotta, 2007; Goyal et al., 2006; Pant et al., 2015; Tiwari et al.,
(Apsimon et al., 1994; Junge and Ryan, 1958). Generally, the reaction

Please cite this article in press as: Singh, S., et al., Wet deposition fluxes of atmospheric inorganic reactive nitrogen at an urban and rural site in
the Indo-Gangetic Plain, Atmospheric Pollution Research (2017), http://dx.doi.org/10.1016/j.apr.2016.12.021
 S. Singh et al. / Atmospheric Pollution Research xxx (2017) 1e9 5

Fig. 2. Correlation and regression plots of NHþ  2

4 , NO3 and SO4 (a) at rural (Juanpur) and (b) urban (Delhi) sites.

between NH3 and H2SO4 is irreversible whereas the reaction with

other gaseous acids is reversible.

NH3 þ H2 SO4 /NH4 HSO4 (1)

NH3 þ NH4 HSO4 /ðNH4 Þ2 SO4 (2)

NH3 þ HNO3 4NH4 NO3 (3)

3.3. Wet deposition fluxes of Nr

Table 3 gives the annual wet deposition fluxes at Delhi and

Jaunpur sites. The fluxes of NHþ 
4 and NO3 at Delhi were observed to
be 10.45 and 3.05 kg N ha1 respectively whereas at Jaunpur the

Table 3
Wet deposition fluxes of NH4þ and NO3 for different categories of sites in India.

Site category NHþ

4 (kgN/ha/yr) NO
3 (kgN/ha/yr)

Rural 2.3 4.06

Suburban 2.3 2.03
Rural & suburban 2.3 3.39
Urban 2.3 4.52
Industrial 4.7 3.84
Delhi (present urban study) 10.45 3.05
Jaunpur (present rural study) 3.19 1.56
Fig. 3. Total wet N deposition fluxes of (reduced N þ Oxidized N) at Delhi and Jaunpur.

Please cite this article in press as: Singh, S., et al., Wet deposition fluxes of atmospheric inorganic reactive nitrogen at an urban and rural site in
the Indo-Gangetic Plain, Atmospheric Pollution Research (2017), http://dx.doi.org/10.1016/j.apr.2016.12.021
6 S. Singh et al. / Atmospheric Pollution Research xxx (2017) 1e9

Table 4
Details of used satellite data for LULC study in Delhi.

Image Path/row Acquisition date Spatial resolution

Landsat 5 146/40 05/09/1994 30 m

Landsat 7 146/40 08/11/2013 30 m

fluxes were 3.19 and 1.56 kgN ha1 for NHþ 

4 and NO3 respectively.
At Delhi, the total wet deposition flux was 13.5 kg N ha1 with
almost 77.5% contributed by reduced N and 22.5% by oxidized N
(Fig. 3). In the case of Jaunpur, total N deposition was 4.75 kg N ha1
with 67.15% contributed by reduced N and 32.85% by oxidized N. In
this study, the wet deposition fluxes of N were found to be higher at
Fig. 5. Comparison of N-NHþ 
4 , N-NO3 and total N flux of the present study with that
the urban site as compared to the rural site. The levels of Nr reported by Kulshrestha et al. (1996) for Delhi.
deposition have been reported higher in cities worldwide (Huang
et al., 2012, 2015; Fang et al., 2011). Comparison of these flux
values with the values given by Kulshrestha et al. (2003b) for urban resulting in very high NO þ
3 and NH4 concentrations. The reason for
sites reveals that the urban site of the present study has a very high such increasing trend can be explained with the rapid industriali-
value of wet deposition flux of Nr. Table 3 gives the fluxes of zation, urbanization and traffic growth in India (Akimoto, 2003;
NHþ 
4 and NO3 of this study along with the values reported by Ghude et al., 2008). Though there is a decrease in agriculture in
Kulshrestha et al. (2003b) for different categories in India. Delhi, NH3 emissions are going to increase due to increase in
population and waste water generation etc. too. As mentioned
earlier, the Delhi city is growing in size so the number of people is
3.4. Effect of Land use and land cover (LULC) changes during past
also increasing. The population of Delhi is grown from 6,220,406 in
two decades
1991e16,753,235 in 2011, and to 18,686,902 in 2016. Similarly, the
waste water generation of the city is increased drastically from
We compared two decadal observations from Landsat in 1994
1812 million liters per day (MLD) in 2004e4144 MLD in 2011 which
and 2013 (see Table 4 for details) to observe changes in land use
can contribute NH3 in air.
cover and implications for wet depositions of Nr species over Delhi.
The reason of higher NHþ 4 concentration could be the additional
The LULC map (Fig. 4) clearly shows that there has been a signifi-
agricultural source from NW states like Punjab and Haryana.
cant decrease in the vegetation-agricultural land cover in Delhi
The two decadal comparison shows one very interesting fact
from 1994 to 2013. A strong agricultural source of NHþ 4 does not
that in Delhi, reduced N has always dominated (always more than
seem to play a major role in this region: despite the decreasing
50%) in total N deposition, but its contribution to total N has
trend of agriculture and associated vegetation, NHþ 4 increased
declined from 84% to 74% from 1994 to 2013. Conversely, oxidized N
remarkably during this decade. Results show that there is a drastic
has increased from 16% to 22.5% which is unlike US study as re-
increase in the wet deposition of Nr species in spite of several
ported by Li et al. (2016) where a shift from oxidized N dominance
measures taken to reduce the emissions from the vehicles and in-
to reduced N dominance has been recorded in recent years. How-
dustries. Fig. 5 gives the value of wet deposition of NO 3 and NH4
þ
ever, Pan et al. (2012) have reported similar results for China, where
during 1994 and 2013. The 1994 values are from Kulshrestha et al.
the nitrogen wet deposition is dominated by reduced N (63%e78%).
(1996), who reported rain water chemistry measurements at a site
As shown in Fig. 5, N-NOe 3 (i.e. oxidized N) increased by 486%
in Delhi which is approximately 10 km NW from our urban site in
while N-NHþ 4 (i.e. reduced nitrogen) increased by 283% from 1994
Delhi. The increase in NO 3 levels in Delhi can be attributed mainly
to 2013. These changes can be linked to the changes that have
to non-agricultural sources such as motor vehicles and fossil fuel
occurred over the last two decades in Delhi, such as a significant
burning (Table 1). The comparison reveals that during past two
increase in the number of motor vehicles (Table 1). The urbanized
decades, NOx and NH3 emissions are increased significantly

Fig. 4. LULC map of Delhi.

Please cite this article in press as: Singh, S., et al., Wet deposition fluxes of atmospheric inorganic reactive nitrogen at an urban and rural site in
the Indo-Gangetic Plain, Atmospheric Pollution Research (2017), http://dx.doi.org/10.1016/j.apr.2016.12.021
 S. Singh et al. / Atmospheric Pollution Research xxx (2017) 1e9 7

Table 5
NHþ 
4 -N, NO3 -N and Total Inorganic N (TIN) at various sites. Unit: kg N ha
1 1.
yr

Sites Category N-NHþ

4 N-NO
3 TIN NHþ 
4 -N/NO3 -N References

Delhi,India Urban 2.7 0.52 3.22 5.19 Kulshrestha et al. (1996)

Hudegadde,India Rural 6.22 0.90 7.12 6.91 Kulshrestha et al. (2014)
Hyderabad, India Urban 11.66 14.22 25.88 0.82 Kulshrestha et al. (2014)
Agra, India Suburban 23.33 0.90 24.23 25.92 Saxena et al. (1991)
Pune,India Urban 1.33 2.69 4.02 0.49 Rao et al. (2014)
Bhosari, India Industrial 2.99 9.70 12.69 0.30 Rao et al. (2014)
USA Miscellaneous 1.37 1.63 3.0 0.84 Holland et al. (2005)
USA Miscellaneous 2.0 1.5 3.5 1.46 Du et al. (2014)
Europe Miscellaneous 4.22 2.58 6.8 1.64 Holland et al. (2005)
China Miscellaneous 6.82 2.63 9.45 2.59 Lu and Tian, 2007
China Miscellaneous 8.08 5.16 13.24 1.56 Huang et al. (2014)
China Urban 14.18 8.91 23.04 1.96 Du and Liu (2014)
China Rural 11.22 7.14 18.95 1.73 Du and Liu (2014)
Dry Savannas, Africa Grassland 1.7 1 2.7 1.7 Galy-Lacaux and Delon, 2014
Wet Savannas, Africa Grassland 3 1.4 4.4 2.14 Galy-Lacaux and Delon, 2014
Delhi, India Urban 10.45 3.05 13.5 3.42 Present study
Jaunpur, India Rural 3.19 1.56 4.75 2.04 Present study

area of Delhi is increased by 17.66 percent during this period
(Fig. 5). Sindhwani and Goyal, 2014 also observed an appreciable
increase in NOX emissions after 2005, which might be due to the
use of CNG fuel. Diesel burning has been a major contributor of NOx
in Delhi (Goyal et al., 2013). Table 1 gives important statistics about
demographic changes in Delhi during the past two decades.
3.5. NHþ 
4 -N and NO3 -N and total inorganic nitrogen at various sites
The majority of total inorganic nitrogen in rain water is present
in the form of NHþ 
4 -N and NO3 -N (Xie et al., 2007). It is calculated by
þ 
the sum of NH4 -N and NO3 -N in precipitation. Table 5 gives the
total wet N deposition fluxes of various sites in India and other sites
worldwide.
From Table 5 we can see that among the major hotspots of
reactive nitrogen over the globe, India and China have high wet
deposition of N, especially in the form of NHþ 4 -N. The ratios of NH4 -
þ
N/NO 3 -N show the dominance of NH þ
4 -N in wet deposition of total
inorganic nitrogen, indicating substantial agricultural source con-
tributions to the atmospheric N deposition (Du and Liu, 2014;
Holland et al., 2005; Kulshrestha et al., 1996; Galy-Lacaux and
Delon, 2014). Pan et al., 2012 have also suggested that NH3 from
agriculture and animal excreta have a major contribution to wet N
deposition, resulting in a higher molar ratio of NHþ 
4 /NO3 in the
North China Plain. The present study also indicated a similar
pattern. However, some studies have reported NO 3 -N as the
dominant part of total inorganic N deposition to the atmosphere
(Holland et al., 2005; Rao et al., 2014; Kulshrestha et al., 2014). On
comparing the previous study in Delhi (Kulshrestha et al., 1996)
with the present study, we can see that the pattern of deposition is
similar in terms of NHþ 4 deposition dominance. However, the ratio
of NHþ 
4 /NO3 has decreased over the time indicating the increase in
dominant N species in wet deposition. Effective regulations on
reactive nitrogen emissions, especially on NOx emissions from
industrialization, should have useful implications for countries like
India and China that are experiencing a rapid increase of NH3 and
NOx emissions (Ghude et al., 2009; Garg et al., 2006; Singh and
Kulshrestha, 2014).
Table 5 also indicates that among the sites from India mentioned
here, urban sites like Delhi and Hyderabad have higher wet N
deposition in terms of TIN, or both NHþ 
4 and NO3 (Kulshrestha et al.,
1996, 2014). But in Hyderabad, wet deposition of oxidizing N is
higher than reducing species which can be attributed to the un-
regulated heavy traffic and industrial development in the city
(Kulshrestha et al., 2014). The rural site included in Table 5
(Hudegade) has shown relatively low deposition as compared to
the sites of present study. The difference of the values in rural and
urban sites in India is probably due to varying methods of collec-
tion, sample storage and delay in chemical analysis (Kulshrestha
et al., 2005).
4. Conclusion
Estimation of atmospheric deposition of inorganic nitrogen
species has high significance due to the impact of Nr deposition
over the ecosystem. This study provides a comparison of Nr
deposition between an urban and a rural site. The reduced nitrogen
fraction was more than 50% of the total inorganic N deposition at
both sites, indicating the influence of possible sources such as
emissions from the agricultural areas of surrounding states,
biomass burning, rapid urbanization, and increasing traffic density
at the urban site; and agriculture activity and fertilizer application
in the fields at the rural site. Annual wet N deposition fluxes of
NHþ 
4 and NO3 at Delhi were observed to be 10.45 and 3.05 kgN ha
1

NO 3 -N in precipitation, whereas total TIN deposition has increased
in Delhi. China's wet N deposition trend is similar to our present
study. Although we do not have an exhaustive data set to see the
whole Indian scenario at present, but from the comparison of the
present study, it is clear that in China also, wet TIN deposition
increased at higher rate, with increases in both NHþ 
4 and NO3 in the
past several decades (increasing NHþ 4 /NO 
3 ratio). But this is not the
case in the USA (Table 5), according to a wet deposition trend study
by Du et al., 2014. In the USA, TIN has not changed significantly
since 1985 to 2012, while a consistent increase has been observed
in NHþ 
4 /NO3 . Nitrate dominated wet deposition across the USA in
1985 (mean NHþ  þ
4 eN: NO3 eN ratio ¼ 0.72) and the NH4 eN:NO3 eN

ratio had increased to 1.49 in 2012, indicating a transition of the
respectively whereas at Jaunpur the fluxes were 3.19 and 1.56 kgN
ha1 for NHþ 
4 and NO3 respectively. The results of this study
showed significantly higher Nr deposition over Delhi than that
reported two decades ago, raising concerns regarding ecological
impacts. NO þ
3 in rain water increased by 486% while NH4 increased
by 283% from 1994 to 2013 due to increased vehicular and other
anthropogenic activities along with LULC of the city. Though
reduced N is the dominant part of total inorganic wet N deposition
at the Delhi site, its fraction declined from 84% to 74% in the past
two decades, which is an interesting trend. On the basis of this
study, we conclude that India's (Delhi) nitrogen deposition rate
shows a higher mean value than those in the China, the United
States, and Europe. Comparing to changes in the past, India's

Please cite this article in press as: Singh, S., et al., Wet deposition fluxes of atmospheric inorganic reactive nitrogen at an urban and rural site in
the Indo-Gangetic Plain, Atmospheric Pollution Research (2017), http://dx.doi.org/10.1016/j.apr.2016.12.021
8 S. Singh et al. / Atmospheric Pollution Research xxx (2017) 1e9
nitrogen deposition has increased at a higher rate than other Nr
hotspots in terms of NH4 þ, NO3 and TIN. The results of this study
are highly important not only to strengthen our understanding
about Nr deposition but also for necessary abatement measures.
Acknowledgement
We are sincerely grateful for the financial support received from
DST-PURSE grants, which helped us to carry out this work. Author
Saumya Singh acknowledges the award of the Senior Research
Fellowship from CSIR. India.
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