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Urban Climate xxx (2015) xxxxxx

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Urban Climate
journal homepage: www.elsevier.com/locate/uclim

Passive measurement of NO2 and application


of GIS to generate spatially-distributed air
monitoring network in urban environment
Sailesh N. Behera a,, Mukesh Sharma b, P.K. Mishra c, Pranati Nayak b,
Bruno Damez-Fontaine d, Renaud Tahon e
a

Department of Civil and Environmental Engineering, National University of Singapore, Singapore 117576, Singapore
Department of Civil Engineering, Indian Institute of Technology Kanpur, Kanpur 208016, India
c
Central Pollution Control Board, Lucknow 226010, India
d
INPG BURGEAP, Paris, France
e
Inter-American Development Bank, 1300 New York Avenue, N.W. Washington, DC 20577, USA
b

a r t i c l e

i n f o

Article history:
Received 26 February 2014
Revised 24 October 2014
Accepted 14 December 2014
Available online xxxx
Keywords:
GIS
Nitrogen oxides
Passive sampling
Vehicular pollution
Monitoring network
Kriging method

a b s t r a c t
Nitrogen dioxide (NO2) plays an important role in atmospheric chemistry through formation of secondary particulate nitrate that contributes a major portion to the mass of particulate matter (PM) that has
several impacts on the environment in the scales of local, regional
and global. NO2 is regulated in most of the countries, because it acts
as a precursor for nitrate formation and it shows signicant negative
effects on human health. The present study was conducted for measurement of NO2 concentration at 204 and 101 sampling locations
in two Indian large cities (population more than 4 million), Delhi
and Kanpur, respectively by using passive samplers. From the
experimental results, an average concentration of 68.6 20.1 lg/m3
was observed in Delhi and it was 36.9 12.1 lg/m3 in Kanpur. The
observed data from all sampling sites were utilized on the platform
of Geographic Information System (GIS) to generate spatially distributed pollution maps (using Kriging interpolation method) and maps
of probability of exceedences of air quality standards. Based on the
survey results on emission activities, meteorology and pollution
maps, this study proposed locations of air quality sampling sites for
a long-term monitoring network in Delhi and Kanpur.
2014 Elsevier B.V. All rights reserved.

Corresponding author.
E-mail address: saileshnb@gmail.com (S.N. Behera).
http://dx.doi.org/10.1016/j.uclim.2014.12.003
2212-0955/ 2014 Elsevier B.V. All rights reserved.

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1. Introduction
A fast growing population coupled with industrialization, urbanization and high levels of energy
consumptions is worsening the ambient air quality of urban areas, particularly in developing countries (Bhati, 2000; Lawrence et al., 2007; Sharma et al., 2013). Out of several air pollutants, nitrogen
dioxide (NO2) (representative of nitrogen oxides, (NOx) = nitric oxide (NO + NO2), is originated from
both primary sources and secondary transformation in the atmosphere. NO2 is regulated in most of
the countries and is used as an indicator to assess the status of ambient air quality in the urban
environments (Baldasano et al., 2003; Ravindra et al., 2008). NOx is predominantly present as NO2
in the ambient air, whereas NO dominates at the emitting sources followed by its oxidation to
NO2 in the ambient air. The important attribute of NO2 is to act as a precursor in the atmospheric
chemistry leading to formation of secondary particulate nitrate, which in turn has major impacts on
local, regional and global scales in the environment (Millstein and Harley, 2010; Stock et al., 2013).
In the atmospheric system, various NO-2related complex reactions take place which produce several
secondary pollutants that are sometimes more harmful than NO2 (Vione et al., 2006; Stock et al.,
2013). In addition, NO2 causes several adverse effects on human health, causing pulmonary edema
and damages to the central nervous system, tissues etc. (Lal and Patil, 2001; Kampa and Castanas,
2008).
The major sources of NO/NO2 in urban environments are fuel combustion in motor vehicles, thermal power plants and industrial furnaces (Garg et al., 2006; Klimont et al., 2009; Bootdee et al., 2012).
The motor transport system is increasing at an alarming rate in large cities of the world due to rapid
growth in urbanization and modernization. For example, from 1981 to 2002, the total number of
motorized two-wheelers raised from fewer than 3 million to 42 million in India, with a 14-fold
increase (Pucher et al., 2007; Behera et al., 2014). The fast growing transportation system causes rapid
increase in levels of ambient NO2 and other criteria pollutants in the large cities (Cohen et al., 2004;
Gokhale and Raokhande, 2008). Therefore, it is pertinent to monitor ambient NO2 levels on regular
basis in the large cities, as a surrogate of other pollutants and to control NO2 emissions (Janssen
et al., 2001; Maruo et al., 2003; Jackson, 2005).
The measurement of NO2 is normally conducted either through bubbling air in a chemical medium
or using real-time online analysers through chemiluminescence technique (Allegrini and Costabile,
2002; Hadad et al., 2005). Both these methods require nancial and human resources, however, passive samplers require almost insignicant resources and can be installed at multiple locations simultaneously (Krochmal and Kalina, 1997; Ferm and Svanberg, 1998; Briggs et al., 2000; Varshney and
Singh, 2003). Several studies in the past measured NO2 levels using passive sampling diffusion tubes
in different urban environments (e.g., Hansen et al., 2001; Lewne et al., 2004; Lozano et al., 2009;
Salem et al., 2009; Ahmad et al., 2011). Most of these studies focused on presentation of results of
NO2 concentrations and their interpretation with respect to spatial distribution and meteorology.
The site selection for air quality monitoring depends largely on data availability on intensity of pollutant concentrations, distribution of emitting sources, meteorology and possible extent of human
exposure (Noll et al., 1977; Allegrini and Costabile, 2002). To develop a control strategy for effective
reduction of NO2 pollution, information on spatial distribution of NO2 levels is necessary. Spatial distribution of NO2 concentration can be prepared from the measurements taken at several monitoring
sites more than 50. The measurements at more sites can conveniently be done through installation of
a large number of inexpensive passive samplers (Hadad et al., 2005; Allegrini and Costabile, 2002).
Preparation of pollution maps through the techniques of Geographic Information System (GIS)
requires a spatial interpolation method that includes statistical or other methods to model the pollution surface. Among relevant interpolation methods (e.g. trend surface analysis, moving window
methods, Kriging method, spline interpolation), Kriging method is a linear interpolation procedure
which is reliable and provides linear unbiased estimation for quantities at unsampled sites that vary
in space (e.g., Oliver and Webster, 1990; Myers, 1994; Briggs et al., 1997). Several studies reported the
applications of Kriging method with various applications; e.g., Haas (1992) on design of continentalscale monitoring networks; Schaug et al. (1993) on acid precipitation; Campbell et al. (1994) on
national patterns of NO2 concentrations; Liu et al., 1995 on ozone concentrations. However, it is
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necessary to combine the results of passive air sampling with Kriging method to achieve some significant applications, such as optimization of air quality networks.
The present study demonstrates a systematic approach on application of GIS through Kriging
interpolation method from the experimental outcomes of passive sampling to generate spatiallyresolved maps of NO2 followed by identication of monitoring sites required for continuous
measurement in two large cities (population more than 4 million) in the Ganga basin, India; i.e.
Delhi (latitude 28360 N and longitude 77130 E) and Kanpur (latitude 26280 N and longitude
80240 E) (Fig. 1). The Ganga basin is the largest river basin in India, located between latitudes
22300 N and 31300 N and longitudes 73300 E to 8900 E (Fig. 1), supporting more than 40% of Indias
population and accounting for 26% of Indian landmass (Behera and Sharma, 2010; Behera et al.,
2011). The ndings of this study can also be implemented in other large cities of developing countries (e.g., Mumbai, Kolkata, Dhaka, Lahore) and the methodology demonstrated in this study can
also be followed for other pollutants.

2. Materials and methods


2.1. Characteristics of the study areas
Fig. 1 shows the study areas; Delhi and Kanpur. These cities represent typical urban agglomeration
and pollution patterns of the large cities in developing countries. The dotted marks in the maps of
Delhi and Kanpur show the sampling sites in both these cities, where passive sampling of NO2 was
undertaken.

Fig. 1. Map of India, Ganga basin, study areas (Delhi and Kanpur): dots in maps of Delhi and Kanpur show locations of sampling
sites.

Please cite this article in press as: Behera, S.N., et al. Passive measurement of NO2 and application of GIS to generate spatially-distributed air monitoring network in urban environment. Urban Climate (2015), http://
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2.1.1. Delhi
Delhi, the capital city of India, situated on the banks of River Yamuna has an area of about 1500 km2
and population of 13,782,976 (2001 Census of India) and is the largest city in the Ganga basin. The
sources of air pollution in Delhi include vehicles, industries, power production, biomass burning, landlls, sewage treatment plants etc. (Singh et al., 2011; Sharma et al., 2013). A signicant rise in levels of
ambient NO2 concentration during 1999 to 2004 can be attributed to rapid incremental trends in various types of vehicles in Delhi (Fig. 2). It can be inferred from the ndings of previous studies that the
cause of increase in levels of ambient NO2 concentrations in urban areas is mainly due to rise in vehicle population (Jackson, 2005; Agarwal et al., 2006; Mallik and Lal, 2014).
2.1.2. Kanpur
Kanpur, a large industrial city in the state of Uttar Pradesh, has a population of over 4.0 million
(2001 Census of India) and an area of about 500 km2. The sources of air pollution in Kanpur include
motor vehicles, industries, coal-based power plants, domestic cooking and biomass burning (Behera
and Sharma, 2010; Behera et al., 2011). The number of vehicles in Kanpur increased from 0.37 to
0.47 million during 2001 to 2004, adding to increased air pollution (RTO, 2006; Behera et al., 2014).
2.2. Sampling site classication and site selection criteria
The United States Environmental Protection Agency (USEPA) has adopted a classication of micro,
middle, neighborhood, urban, regional, national/global air quality stations, depending on the scale of
representativeness of measurements (USEPA, 1994). Similar to USEPA, the EuroAirNet classies monitoring stations based on three criteria including trafc, industrial and background (EEA, 1999). In this
study, a modied station typology was adopted based on convention of the prevailing European classication that included (i) suburban, (ii) urban, and (iii) trafc.
Maps of Delhi and Kanpur were obtained from respective municipal authorities for preliminary
surveys and identication of the sampling sites. Initially, the whole study area was divided into several zones and the basis for generation of zones was population density. Hence, sizes of the zones in
highly populated areas were smaller compared to less populated areas. In the process of site selection,
grids were constructed on the maps and sampling sites were identied considering emission sources,
trafc ow and number of inhabitants in that particular locality. Overall, total area of Delhi was
divided into twenty zones based on the grid sizes of 2 km  2 km and passive samplers were installed
at 204 locations. Kanpur was divided into seven zones based on the grid sizes of 1.5 km  1.5 km and
passive samplers were installed at 101 locations. The purpose for selection of two different grid sizes
of the study areas was on the hypothesis to accommodate equal number of grids surrounding each
sampling location. In other words, the distribution of sampling locations per grid would be uniform
in both the cities. In that way, by adopting 2 km  2 km grid size for Delhi and 1.5 km  1.5 km grid

Fig. 2. Trends of increase in vehicular population and NO2 concentration in Delhi (Source:Motor Transport Statistics of India,
2005 and Central Pollution Control Board (CPCB), 2006).

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size for Kanpur, Delhi and Kanpur were divided into 408 and 202 grids, respectively. Thus, the number
of grids presenting each sampling location was two grids in both cities.
While deciding the sampling locations, the following precaution measures were considered: (i)
security of the samplers, (ii) the location of sampling site was at least 100 m away from heavy trafc
roads and 40 m away from the minor trafc lanes, (iii) no instantaneous sources of air pollution (especially responsible for NO2 pollution) were present close to the sampling location, and (iv) height of the
sampler was maintained between 310 m above ground level with unrestricted air movement. The
measurement campaign was conducted at Delhi and Kanpur during FebruaryMarch, 2004 and the
exposure time for passive sampling at each sampling site was two weeks.
2.3. Passive sampling and analysis of NO2
The principle of passive sampler is based on Ficks diffusion law; as a pollutant from the ambient air
gets accumulated in the sampling medium via gaseous diffusion (Shoeib and Harner, 2002; Bartkow
et al., 2005). The driving force is the concentration gradient between the surrounding air and the
absorbing surface, where the pollutant concentration is initially zero. The air pollutant remains in
the absorbing medium after being absorbed by the medium. The advantages of using passive samplers
can be summarized as follows: it needs no eld calibration and power supply or technical people at
the sampling sites for operation, and it can also be reused with 100% time coverage (Cruz et al.,
2004; Harner et al., 2004; Hadad et al., 2005).
In this study, plastic Passam diffusion tubes (Passam Ag, Switzerland) of approximately 1 cm in diameter and 6 cm in length were used for NO2 sample collection. The principle of sampling and analysis were
based on Palmes et al. (1976). Molecules of NO2 diffused along the tube were trapped within the absorbent (triethanolamine (TEA) impregnated mesh) by forming TEANO2 complex. After exposure of tubes
for the time period of two weeks, NO2 was quantied by chemically extracting nitrite (NO
2 ), and analyzing it by colorimetric method. Due to limitation of resources, one tube was installed at each sampling site
in both the study areas except for duplicates and site repetitions. For quality assurance and quality control (QAQC) of the laboratory method for analysis, duplicate tubes were installed simultaneously at 10%
locations of the total sampling sites in Delhi and Kanpur. These duplicates were blank samples and kept
sealed during sampling. The break-up of number of sites in each category was: suburban 31, urban 85
and trafc 88 in Delhi; and suburban 18, urban 41 and trafc 42 in Kanpur. As the sampling lasted
for two months, repetitions of sampling at few sites were done to collect samples. In other words, the
sampling was continued during two months at these sampling sites. Hence, four sets of samples were
collected at each of those sites to assess the variations of NO2 concentrations with respect to time at a
particular site. For this purpose, the selected numbers of sites were: suburban 1, urban 4 and trafc
4 in Delhi; and suburban 1, urban 2 and trafc 2 in Kanpur.
The boxes (10 cm diameter and 17 cm length) closed at the top and open at the bottom were used
to protect the sampling tubes from direct sunlight and excessive aeration. The caps of tubes were
removed and mounted vertically with the absorbent at the uppermost part of the tube with the opening pointing downwards to prevent the entry of rain water and dust particles. The time at the start and
end of each exposure period (two weeks) was recorded accurately. At end of the exposure period, the
samples and blanks were collected, and were placed in air tight containers. These sealed samples were
then refrigerated at 4 C and protected from sunlight until sent out for further analysis by colorimetric
method. After sampling were done at all locations, sampled tubes, duplicate tubes and blank samples
were shipped with air tight package containing dry ice to Passam Ag Laboratory, Switzerland for further analysis.
In this study, all chemicals used were of analytical grades from SigmaAldrich (USA) or Merck
(Germany) and deionized water was used throughout the analysis. During sample preparation, a premixed color reagent was prepared by adding sulphanilamide (20 g sulphanilamide reagent +50 ml
concentrated orthophosphoric acid diluted to 1000 ml with distilled water) and N-1-naphthylethylenediamine- dihydrochloride (NEDA; 0.5 g NEDA in 500 ml distilled water) in 1:1 proportion. After
sampling and prior to analysis, 3 ml of the pre-mixed color reagent was added to each sample tube.
The tube was then closed and was stirred with a vortex mixer for 1015 seconds and left for 30 min.
After formation of purple red azodye, absorbance was measured with an UV spectrophotometer at
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540 nm. The intensity of the azodye was proportional to the amount of NO2 absorbed over the sampling
period. The mass of NO
2 present in the analyte was derived from the reference calibration curve prepared from the standard solutions of sodium nitrite.
From the mass of NO
2 , the average ambient concentration of NO2 was estimated using Eq. (1):

C NO2

M a  M b  l
DAt

where C NO2 was the ambient concentration of NO2, Ma was the mass of NO
2 absorbed in lg, Mb was
NO
2 of blank in lg, l was the diffusion path or length of the tube in cm, A was the surface area of the
tube in cm2, D was the diffusion co-efcient of NO2 through air in cm2/s, t was time of exposure in s. A
suitable conversion factor was multiplied with the value of C NO2 in Eq. (1) (i.e. lg/cm3) to get the concentration of NO2 in lg/m3.
Before commencement of this measurement campaign, some passive sampling tubes were calibrated against the active air sampler with calibration factor as 0.9939 with R2 value as 0.9604. The
detection limit of NO2 measurement (i.e., 0.3 lg/m3) was determined by 3 times the standard deviation of the concentration of blank samples. The uncertainty and repeatability of laboratory analysis
were <20% and <10%, respectively.
2.4. Pollution mapping with geostatistics tool
In general, an air quality management plan (AQMP) describes the current state of air quality in an
area, the ways for its change over time and steps to be followed for better air quality in that region.
The process of developing AQMP and implementing it effectively involves several steps that include
goal setting, baseline air quality assessment, air quality management system (AQMS), development
and evaluation of policies for strategic reduction of air pollution, initiative for implementation of
action plans, time to time evaluation of action plans and follow up. Among these steps, AQMS is
the central theme of the AQMP. AQMS involves several steps that include air pollution monitoring,
development of emission inventory and air quality modeling. In this study, we focused on monitoring
of NO2 at several places, acquiring of activity data from on-site surveying. These data were put on the
GIS modeling system to generate spatially distributed pollution maps that helped in identication of
hotspots in Delhi and Kanpur.
For mapping the pollution levels of NO2, we used the ArcGIS geostatistical analysis tool due to its
ability to manage a wide range of data formats that are represented by layers of digital maps of various
observations within the framework of spatio-temporal analysis (Briggs et al., 1997; Behera et al., 2011).
Ordinary Kriging method was adopted for interpolation to create a continuous surface from the database of measured concentration (at various locations) due to its capability of quick interpolation that
can be extracted or smoothed depending on the measurement error model (Oliver and Webster,
1990; Myers, 1994; Briggs et al., 1997). The generated surface was then used to predict the NO2 levels
at unmeasured locations. In addition to above facts, ordinary Kriging method predicted standard error
of indicators and probability of exceedance of certain pollution level.
In this study, the topographical maps of Delhi and Kanpur, issued by the Survey of India (prepared
in 1977) having scale of 1:50,000 were geo-coded as the base map in the form of polygons for geo-referencing other maps. The base map of each city was then transformed to Universal Transverse Mercator projection with Everest 1956 as the datum. The other two maps, (i) road network and
intersections (from CPCB, Delhi), and (ii) ward (smallest political unit in a city) boundary (from Delhi
and Kanpur Municipal Corporations) were geo-referenced with respect to the base map.
3. Results and discussion
3.1. Passive sampling of NO2
The statistics of observed results of NO2 concentration after 2 weeks of exposure through passive
samplers at 204 sampling sites in Delhi were as follows: mean 68.6 lg/m3; standard deviation of
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20.1 lg/m3; minimum 27.9 lg/m3 and maximum 126.3 lg/m3 (Table 1). From Table 1, it was conrmed that the concentrations at trafc sites were higher than urban sites, and the suburban sites
had least concentrations. The concentrations at urban sites located in the industrial areas were as high
as the trafc sites (see Fig. 1 for land-use patterns of the study area). From the trends in levels of NO2
at various types of sites, it can be inferred that vehicles could be the predominant sources responsible
for ambient NO2 concentration. Fig. 3a shows the frequency distribution of NO2 concentration in
10 lg/m3 unit intervals which ranged from 0 to 130 lg/m3 in Delhi. The values of NO2 concentration
appeared most frequently in a range from 60 to 70 lg/m3 with a frequency of 23%, followed by a range
from 80 to 90 lg/m3 with a frequency of 18% and by a range from 50 to 60 lg/m3 with a frequency of
16% (Fig. 3a). Overall, the existing levels of NO2 exceeded the 24-h Indian Standard of 80 lg/m3 at 24%
of observed data. In other words, 24% monitoring sites in the city had levels of NO2 that exceeded the
24-hr Indian standard.
Varshney and Singh (2002) measured ambient levels of NO2 along the north-west and south-east
transact of Delhi using passive samplers from November 1998 to June 1999 with two weeks of exposure at 9 trafc sites. They observed NO2 levels varied from 13 lg/m3 to 200 lg/m3, and NO2 levels
exceeded the Indian standard of 80 lg/m3 at 45% of the sites. The reason for difference in percentage
of exceedence compared to our study could be due to the site characteristics. Looking into the percentage of exceedence of only trafc sites in our study, it was found that 51% sites could not meet the
Indian standard. The average NO2 concentration at trafc sites (85 lg/m3) was higher than
Varshney and Singh (2002) (i.e. 70 lg/m3) and that could be attributed to increase in vehicle population along with time. Our study has the advantage of observations at 204 sampling sites which gave
the overall pollution picture of the entire city, and these results were utilized in developing the pollution map through GIS techniques.
The statistics of NO2 concentration in Kanpur at 101 sampling sites can be summarized as follows:
mean 36.9 lg/m3; standard deviation of 12.1 lg/m3; minimum 16.5 lg/m3 and maximum 68.8 lg/m3
(Table 1). Similar to Delhi, higher levels of NO2 were observed at trafc sites in Kanpur. In contrary to
NO2 levels in Delhi, NO2 concentrations in Kanpur were less than the 24-h Indian standard (80 lg/m3)
at all sites. Fig. 3b shows the frequency distributions of NO2 concentration in 10 lg/m3 unit intervals
which ranged from 0 to 60 lg/m3. The values of NO2 concentration appeared most frequently in a
range from 20 to 30 lg/m3 with a frequency of 29%, followed by a range from 30 to 40 lg/m3 with
a frequency of 27% and by a range from 40 to 50 lg/m3 with a frequency of 22% (Fig. 3b).
As described in a previous section that the repetition of sampling was performed at few sites for the
duration of two months to assess the variations in concentrations of NO2 with respect to time at a particular site. From the results at those sites, it was observed that the standard deviation of the results at

Table 1
Statistical summary of the measurement results in Delhi and Kanpur (NO2 concentration is in lg/m3).
Study area

Statistical parameter

Type of sampling sites

Overall

SU

Delhi

N*
Mean
SD
Min
Max

31
46.7
14.9
27.9
64.3

85
74.5
22.6
39.4
114.6

88
84.6
22.9
52.3
126.3

204
68.6
20.1
27.9
126.3

Kanpur

N*
Mean
SD
Min
Max

18
24.9
7.5
16.5
33.7

41
34.9
15.2
18.2
53.4

42
50.7
13.4
33.2
68.8

101
36.9
12.1
16.5
68.8

SU: suburban site; U: urban site; T: trafc site.


SD: standard deviation.
Min: minium; Max: maximum.
*
N: number of observations and the results are presented from the observations of single samples collected at each of the sites
(i.e., number of sampling sites is equal to number of observations).

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Fig. 3. Frequency distributions of NO2 concentrations observed from passive sampling in: (a) Delhi, and (b) Kanpur.

all categories of sites were less than 8% of the mean value at the respective sites. Therefore, it could be
inferred that the distinctions in NO2 concentrations presented in Table 1 at all categories of sites were
more dependent on spatial variations.
Table 2 presents NO2 levels measured at various parts of the world through passive sampling techniques. It appears that Delhi is more polluted than other cities of the world and it is expected that
there would be more pollution in future, unless any mitigation measure has been undertaken. During
the sampling campaign, meteorological parameters, such as temperature, relative humidity and wind
speed were measured at sampling sites in both cities. Locally available potable wet and dry bulb thermometers were used for measurement of temperature and relative humidity, respectively. Wind
speed was measured by potable anemometer. To assess the inuence of meteorology on ambient levels of NO2 concentration, the results of correlation analysis of NO2 in relation to independent meteorological parameters including temperature, relative humidity and wind speed are presented in Tables
3 and 4. Correlation analyses of meteorological parameters with NO2 levels indicated that NO2 was
signicantly associated with temperature, relative humidity and wind speed in Delhi and Kanpur.
3.2. Spatial variable analysis and pollution maps
In this study, the pollution mapping for the entire study area was done at two stages in the Kriging
interpolation method. In the rst stage, spatial structure of the data was quantied to produce a variogram that represented a spatial dependence model of the data. For prediction of concentrations at
unknown locations, Kriging used the tted model from the variogram, the spatial data conguration
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Table 2
Comparison of the measurement results with other reported studies.
Study area

Year of measurement

NO2 (lg/m3)

Reference

Urban area, Sweden


Delhi, India
Germany
Netherland
Sweden
Shiraz, Iran
Rawalpindi, Pakistan
Malaga, Spain
Al-Ain, UAE
Delhi, India
Kanpur, India

1989
1998-99
1999-2000
1999-2000
1999-2000
2003
2008
2000-2001
2005-2006
2004
2004

24.4
70.0
28.8
28.9
18.5
>100.0
55.74
22.8
59.3
68.6
36.9

Ferm and Svanberg (1998)


Varshney and Singh (2002)
Lewne et al. (2004)
Lewne et al. (2004)
Lewne et al. (2004)
Hadad et al. (2005)
Ahmad et al. (2011)
Lozano et al. (2009)
Salem et al. (2009)
This study
This study

Table 3
Pearson correlation coefcients (r) between NO2 and meteorological parameters in Delhi.

NO2 concentration
Temperature
Relative humidity
Wind speed

NO2 concentration

Temperature

Relative humidity

Wind speed

1.00
0.86
0.91
0.97

1.00
0.94
0.73

1.00
0.87

1.00

Bold marked are statistically signicant with p value <0.01.

Table 4
Pearson correlation coefcients (r) between NO2 and meteorological parameters in Kanpur.

NO2 concentration
Temperature
Relative humidity
Wind speed

NO2 concentration

Temperature

Relative humidity

Wind speed

1.00
0.91
0.89
0.93

1.00
0.92
0.82

1.00
0.91

1.00

Bold marked are statistically signicant with p value <0.01.

and the values of the measured sample points around the location of interest. We deduced the experimental variogram by averaging the variograms over all intervals that were required for the denition
of a lag value of 1 km. Then a theoretical variogram was tted to the experimental variogram. The theoretical variogram acted as a key tool for weighting the inuence of different sampling points for evaluating concentration at a node of the target grid.
For spatially-resolved pollution maps, all grids in the digitized maps of Delhi and Kanpur were
assigned conventional codes to locate respective sampling sites. The cells in grids falling over the areas
of Delhi and Kanpur were digitized to convert each cell into an individual polygon. The continuous
surfaces created by interpolation technique were in greyscale. For creating color gures, the images
were processed using the unsupervised classication method available in Geomatica to assign colors
to each pixel based on its data/emission value. To generate the spatial map showing probability of
passing a concentration level, we preferred a reference mark of 40 lg/m3, as this value represented
the annual Indian National Standard of NO2. As a result, an overall view of the entire study area with
strategic point of view in long turn aspect could be assessed.
The probability Kriging method was used to create a probability map that exceeds a critical threshold value (40 lg/m3). Probability Kriging method assumes the model as follows:

Is IZs > ct l1 e1 s

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Zs l2 e2 s

where l1 and l2 are unknown constants and I(s) is a binary variable created by using a threshold indicator, I(Z(s) > ct). It can be noticed about two types of random errors, e1(s) and e2(s), so there is autocorrelation for each of them and cross-correlation between them.
Probability Kriging method strives to do the same thing as indicator Kriging method, but it uses
cokriging in an attempt to do a better job (http://resources.arcgis.com/en/home/). For more information about the steps to follow, please refer the tutorials explained in the weblink (http://resources.arcgis.com/en/home/) and the tutorial documented by Johnston et al. (2001).
Fig. 4a shows the spatial distribution map of NO2 in Delhi and it can be clearly seen that the concentrations were at the highest levels near roadsides indicating that vehicles were largely responsible
for NO2 emission. Next to roadside levels, industrial areas showed high levels of NO2 concentrations
also. For checking the consistency of our results, we compared our spatial map with concentrations
at specic location measured at a few locations through active sampling by our team members at
CPCB (Central Pollution Control Board, Delhi) for the study on national ambient air quality status
(CPCB, 2004). From the comparison, it appeared that the trends in spatial variations of NO2 levels were
quite similar in both the observations with the highest levels were observed in heavy trafc areas of
ITO trafc intersection and Town Hall due to more trafc volumes and trafc congestion in these
areas. Fig. 4b shows the spatial distribution of NO2 which represents the probability of exceeding
40 lg/m3. It could be inferred that most of the areas in Delhi were having higher chances with probability of 0.9 to exceed the annual Indian standard.
The spatial distribution of NO2 concentration in Kanpur is shown in Fig. 5a. In comparison to Delhi,
Kanpur experienced less pronounced levels of pollution. Similar to Delhi, Kanpur had higher pollution
levels near roadsides and industrial areas. Due to large commercial activities and more trafc congestions taking place in the city central area, this area could be considered as one of the hotspots of NO2
concentrations. The trends of spatial distributions of NO2 levels in this study were quite similar to the
levels, measured at a few locations through active sampling by our team members at CPCB (CPCB,
2004). Fig. 5b shows the spatial distribution of NO2 that represented the probability to exceed
40 lg/m3 concentrations in a locality. From Fig. 5b, it could be inferred that 50% area in Kanpur had
higher chance with probability of 0.9 to exceed the annual Indian standard.

3.3. Proposing monitoring network for sampling sites


To examine the fact that control of NO2 can lead to reduce levels of other pollutants, we performed
a linear correlation analysis between particulate matter with aerodynamic diameter 610 lm (PM10)
and NO2 for 15 days average data during 2004 at national air quality sites that were maintained by
our team members at CPCB in Delhi and Kanpur. As our passive sampling measurement was undertaken during February-March, 2004, we considered the observational data during these two months
from national air quality sites for correlation analysis. The PM sampling was carried out using high
volume respirable dust sampler (APM-460 RDS, Envirotech, Delhi), which was equipped with a
cyclone to provide separation of PM10 particles with sharper cutoff (D50 at 10 lm) from the coarser
particles by centrifugal forces. When the suspended particles in air were drawn through the sampler,
non-respirable particles (NRP) in air fell into the cyclones conical hopper and got collected in the
cyclonic dust cup. The ne dust comprising the respirable fraction (PM10) passed through the cyclone
and gets collected on the 20  25 cm Glass Microbre Filter (GFF; Whatman grade). The sampling ow
rate was maintained between 0.8 and 1.2 m3/min. The GFF lters and dust cups were pre-conditioned
and post-conditioned at temperature 22 C and RH 40% with controlled desiccators in the room
meant for conditioning for 24-hr. PM10 mass concentration (lg/m3) was determined gravimetrically
by the difference in mass of GFF after and before sampling (lg) divided by the volume of sampled
air (m3). In a similar way to gravimetric method of PM10, the concentration of NRP was determined
from mass difference of respective dust cup after and before sampling and the volume of sampled
air. The total suspended particle (TSP) concentration was calculated as the sum of PM10 collected
on the lter and NRP collected in the dust cup. In this study, we used the measurement data of
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Fig. 4. Spatial distribution NO2 in Delhi: (a) map showing NO2 concentration in lg/m3, and (b) map showing possibility to pass
40 lg/m3.

PM10 for interpretation. NO2 was measured by sampling through an absorbing solution in midget impinger system (connected in APM-460 RDS) followed by colorimetric method in the laboratory.
The number of national air quality sites being nine and six in Delhi and Kanpur, the pairs for linear
correlation analysis were: n = 9  4 = 36 in Delhi and n = 6  4 = 24 in Kanpur. Fig. 6a and b shows the
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Fig. 5. Spatial distribution NO2 in Kanpur: (a) map showing NO2 concentration in lg/m3, and (b) map showing possibility to
pass 40 lg/m3.

scatter plots between PM10 and NO2 in Delhi and Kanpur, respectively. The squared correlation coefcients (R2) were determined from the linear best t line. The correlation coefcients were signicant
in Delhi and Kanpur; i.e. R2 = 0.87 and p < 0.01 for Delhi and R2 = 0.82 and p < 0.01 for Kanpur. Interestingly, lower correlation in Kanpur compared to Delhi could be attributed to PM coming from noncombustion sources (e.g., road and soil dust). In other words, the contribution of road and soil dust to
PM mass was higher in Kanpur than Delhi and these trends of observations were similar to our previous studies (Behera and Sharma, 2010; Behera et al., 2011). Overall, signicant correlation between
NO2 and PM10 in both the cities suggested that the spatial pollution mapping of NO2 was a better way
to describe the patterns and trends of other pollutants prevailing in the study areas. Moreover, studies
in the past (Boogaard et al., 2011; Minguilln et al., 2012; Wang et al., 2013) also reported strong correlations between concentrations of NOx and PM at urban sites, suggesting that NOx can be used as a
proxy for PM exposure to emitting sources.
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Fig. 6. Scatter plots between NO2 and PM and linear correlation from the best-t line: (a) in Delhi, and (b) in Kanpur.

In the decision making process to propose the locations and numbers of sampling sites in these two
large cities, maps showing spatial distributions of NO2 were examined to assess the most vulnerable
areas through identication of hot spots. As described in a previous section, the current situation of
trafc volume, congestion and commercial activities were considered in addition to identifying the
hotspots. In other words, the hotspots having higher probability of exceedance of critical threshold
value of 40 lg/m3 on NO2 concentration and with more trafc congestion were highly sensitive to
human health risk due to more exposure of pollution. This should be noted that the sequence of plans
for making a proposal on location of monitoring sites was within the guidelines of EEA (1999). Hence,
after identifying the critical areas, survey results on long-term meteorology, demographic patterns,
and distribution of emitting sources were taken into account during the exercise in locating the sampling sites. It was observed that most populated districts in Delhi were (in decreasing order) as follows: Northeast, Central, East, North and West. The site classications were based on the
convention of three types; i.e. trafc, urban and suburban. The purpose for choosing suburban site
was to get the background concentration and assess the effects of city pollution on the surrounding
areas under downwind conditions.
Fig. 7a shows the locations of existing monitoring sites of national ambient air quality study maintained by CPCB team during 200304. During decision making process, the existing sites of CPCB were
examined for their suitability on the aspect whether to retain or reject. From this map, it was clear that
the areas labelled with red color were extremely polluted and termed as hotspots for NO2 pollution.
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Based on source characteristics and population density, it was assessed that locating two trafc and
three urban monitoring sites would be more appropriate to present the data at such a highly polluted
area of the city. The use of prevailing meteorology became paramount during nalization of sampling
location of suburban sites. From the meteorological data during 200304, it was observed that the
directions of prevailing wind in Delhi were North to Northwest and East to Southeast. Therefore, allocating suburban sites at SE and NW would full the purpose to represent the sites of background and

Fig. 7. Sampling network in spatial distribution map of Delhi: (a) existing NAMP sites, and (b) proposed monitoring sites.

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effects on city pollution ux on suburban region. For example under NW wind, NW suburban site
would give background level characteristic of air in Delhi and SE suburban site would give levels of
pollution coming from city centre after photochemical transformation, where ozone (O3) levels are
expected to be the highest. This should be noted that during allocation of sampling sites, the trends
in levels of ambient O3 must be considered as the role of ambient O3 is very important in the atmospheric chemistry. From the observations of previous studies (Mavroidis and Ilia, 2012; Banan et al.,
2013), it was believed that higher levels of O3 prevailing in the suburban regions could undergo transportation to reach the city area and would play signicant role in atmospheric chemistry the city area.
Therefore, as a future scope of work, it could be recommended that levels of tropospheric O3 at suburban regions should be monitored regularly. Fig. 7b shows the possible locations of automated sites
to be included in our proposed monitoring network in Delhi. In the decision making process for proposal of sampling sites, we considered to retain six sampling sites of national ambient air quality sites
and proposed nine more sites (total fteen). Overall, these sites would present a complete pollution
scenario and the potential for population exposure to pollution over the city.
The prevailing wind direction in Kanpur was northwest to southeast. Approaches similar to Delhi
were adopted for decision making process on proposal of sampling sites (trafc, urban and suburban)
in Kanpur for a monitoring network. Fig. 8 shows the proposed locations of the sampling sites. Two
suburban sites were proposed to represent both upwind and downwind characteristics of pollution
in the city. One sampling site was identied to account for industrial emissions (marked as industrial
site in Fig. 8 and it was urban type in nature). Based on the locations of hotspots, source characteristics
and population density, it was decided to allocate one trafc and two urban sampling sites in the city
central area. Other possible locations were considered for trafc and urban set up at moderate pollution levels. In addition, one urban sampling site was proposed to account for the second critical area in
the east side of Kanpur. Retaining location of the industrial site, trafc and urban sites in the city central area of the national ambient air quality study, we proposed ve additional sampling sites. Hence,
it appeared that by allocating eight sampling sites in Kanpur, overall pollution scenario of the city
could be represented.
The future scope of the research on proposal of monitoring network for measurement of air
pollutants in urban environment could be extended through parallel measurement of O3, SO2 and
NH3 along with NO2 using passive samplers. With the measurement results of these precursor gases,
the trends of atmospheric chemistry could be studied in distinctions with time and space. The ndings
from the role of atmospheric chemistry of these precursor gases on formation of secondary components of PM would improve the decision making process on allocation of sampling sites.

Fig. 8. Sampling network in spatial distribution map of Kanpur: proposed monitoring sites.

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4. Conclusions
The present study demonstrates a systematic approach that describes the application of GIS
through Kriging interpolation method with the experimental outcomes of passive sampling to generate spatially-resolved maps of NO2 levels. These results were used in identication of monitoring sites
required for continuous long-term measurement in two megacities of India (Delhi and Kanpur). Passive sampling of NO2 was conducted at 204 and 101 sampling locations in Delhi and Kanpur, respectively. It was observed that Delhi and Kanpur experienced an average NO2 concentration of
68.6 20.1 lg/m3and 36.9 12.1 lg/m3, respectively. A signicant correlation between NO2 and
PM10 in both cities suggests that the spatial pollution mapping of NO2 is good enough to describe
the patterns and trends that are also valid for other pollutants. On the basis of survey results on emission activities, meteorology and guidelines for site selection criteria with its characteristics (urban,
trafc and suburban types), this study proposes that Delhi and Kanpur need fteen and eight number
of sampling sites to represent the complete pollution scenario. The study emphasizes on location of
suburban or background sampling sites for overall assessment on the pollution levels and their exposure to the existing population.
Acknowledgements
This research study was part of the project Air Quality Monitoring in India, conducted in collaborative efforts among Central Pollution Control Board, Delhi, ETI group, BURGEAP, France, and Indian
Institute of Technology, Kanpur. We also thank two anonymous reviewers for their valuable comments that helped for substantial improvement of this article.
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