Chemical characterization and source identification of particulate matter at Ballari (15.15°N, 76.93°E), Karnataka over Southern Indian region

Chemical characterization and source identification of particulate matter at Ballari (15.15°N, 76.93°E), Karnataka over Southern Indian region

Journal Pre-proof Chemical characterization and source identification of particulate matter at Ballari (15.15°N, 76.93°E), Karnataka over Southern Ind...

3MB Sizes 0 Downloads 33 Views

Journal Pre-proof Chemical characterization and source identification of particulate matter at Ballari (15.15°N, 76.93°E), Karnataka over Southern Indian region V. Shalini, K. Narasimhulu, K. Raja Obul Reddy, G. Balakrishnaiah, K. Rama Gopal, T. Lokeswara Reddy, T. Chakradhar Rao, B. Elijabetthamma, C. Manjunatha, R.R. Reddy PII:

S1364-6826(20)30012-2

DOI:

https://doi.org/10.1016/j.jastp.2020.105192

Reference:

ATP 105192

To appear in:

Journal of Atmospheric and Solar-Terrestrial Physics

Received Date: 12 September 2019 Revised Date:

6 January 2020

Accepted Date: 16 January 2020

Please cite this article as: Shalini, V., Narasimhulu, K., Raja Obul Reddy, K., Balakrishnaiah, G., Rama Gopal, K., Reddy, T.L., Chakradhar Rao, T., Elijabetthamma, B., Manjunatha, C., Reddy, R.R., Chemical characterization and source identification of particulate matter at Ballari (15.15°N, 76.93°E), Karnataka over Southern Indian region, Journal of Atmospheric and Solar-Terrestrial Physics (2020), doi: https:// doi.org/10.1016/j.jastp.2020.105192. This is a PDF file of an article that has undergone enhancements after acceptance, such as the addition of a cover page and metadata, and formatting for readability, but it is not yet the definitive version of record. This version will undergo additional copyediting, typesetting and review before it is published in its final form, but we are providing this version to give early visibility of the article. Please note that, during the production process, errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain. © 2020 Published by Elsevier Ltd.

1

Chemical characterization and source identification of particulate

2

matter at Ballari (15.15N, 76.93E), Karnataka over Southern Indian

3

region

4

V. Shalinia, K. Narasimhulub, K. Raja Obul Reddya, G. Balakrishnaiaha, K. Rama Gopal

5

a*

, T. Lokeswara Reddya, T. Chakradhar Raoa, B. Elijabetthammaa, C. Manjunathaa, R.R. Reddya

6 7

a

Aerosol & Atmospheric Research Laboratory, Department of Physics, Sri Krishnadevaraya University, Anantapur – 515003, A.P. India.

8 b

9

SSA Govt. First Grade College (Autonomous), Ballari, Karnataka, India

10 11

* Corresponding author:

12

Dr. Rama Gopal Kotalo

13

Assistant Professor

14

Aerosols and Atmospheric Research Laboratory

15

Department of Physics

16

Sri Krishnadevaraya University

17

Anantapur – 515 003.

18

A.P., India

19

Email: [email protected]

20 21

1

22 23

ABSTRACT

24

the total suspended particulate matter in the sub-urban environment, Ballari. There were

25

28 particulate matter aerosol sampled between February 2017-July 2018. The surface

26

mass concentration ranged from 103 µg m-3 to 367 µg m-3 with an average value of ~

27

225±65 µg m-3 during the study period. The morphology and elemental composition of

28

aerosol particles were analyzed by using a scanning electron microscope (SEM) coupled

29

with an energy dispersive X-ray system (EDX). From the EDX results aluminosilicate

30

group (Al, Si, K, Fe, Na, Mg, Ti and Ca) contains about ~31 % of the total particles,

31

which mainly due to mineral particulate aerosol originate from crustal origin through

32

windblown dust. Further, we also investigated the morphology and chemical composition

33

of total mass concentration during haze (27-03-2018) and clear days (23-02-2018). The

34

SEM pictures show the most notable deposition of spherical particles with smooth

35

surfaces on a hazy day suggesting that the carbon aerosols on haze day were favourable

36

to coagulation of Aitken mode particles, which is consistent with their respective aerosol

37

subtypes captured from Cloud-Aerosol Lidar with Orthogonal Polarization (CALIPSO)

38

satellite over the study region. Inductively coupled plasma optical emission spectrometer

39

(ICP-OES) analysis showed the relative contribution of inorganic ions ( SO 24 , NO 3 , Na+,

40

Ca2+, Cl-, NH 4 , K+) is higher than others on 1-05-2017 and 01-01-2018 days over the

41

observational site. The relative contribution of non-sea salt SO 24 was abundance (~35%)

42

on both days, indicating the significant anthropogenic influence at this location. The

43

concentration weighted trajectory (CWTs) analysis showed the major sources of

44

particulate matter were soil particles, vehicular emissions, and mining activities

45

surroundings the vicinity of the sampling site.

46

Keywords: Particulate matter, SEM, ICP-OES, aerosol types, Ballari

47

1. Introduction

The present study reports the chemical composition and source identification of

48

Aerosols are known to have a major impact on both the climate and human health,

49

and they exhibit highly spatial-temporal distribution, and it is known to be originating

50

from various sources, both natural and anthropogenic (Boiyo et al., 2018; Reddy et al.,

51

2016a; Babu et al., 2013; Gopal et al., 2015; Wang et al., 2011). Fossil fuel combustion, 2

52

biomass burning, and desert dust are the main sources of air pollutants around the globe.

53

Absorption of solar radiation due to aerosol particles is mainly caused by carbonaceous

54

particles (elemental carbon, EC, and organic carbon, OC) and mineral dust. The primary

55

parameters that determine the environmental and health effects of aerosol particles are

56

their concentration, size, structure, and chemical composition (Pöschl, 2005; Reddy et al.,

57

2016b; Partanen et al, 2018). Aerosols with sizes less than one micron can be categorized

58

as fine mode particles, such as sulphate particles, organic carbon and soot. Aerosol

59

particles with a size greater than one micron are called coarse mode particles, i.e. dust,

60

vegetation debris and sea salt. The categorization can also be carried out by an assortment

61

of aerosols based on their generation source (Casimiro et al., 2013). Health studies

62

indicate that long-term exposure to particulate matter has both climate and health

63

effects. Several studies (Timonen et al., 2018; Campos Ramos et al., 2009; Srivastava

64

and Jain, 2007; Wang et al., 2006) have made the major chemical components in ambient

65

aerosol particles and their elemental concentration levels in urban areas and they

66

concluded that the chemical composition of aerosol particles depends mainly on

67

geographical location, season, local meteorological conditions and long range transport.

68

Ballari is situated from southwest to northeast of Karnataka state and it is known

69

as one of fastest growing city in the Karnataka state as well as endowed with rich mineral

70

resources. Apart from being a major source region for aerosols, is centered by densely

71

industrialized areas where different aerosol species such as mineral dust, soot, nitrate,

72

sulfate particles and organics are produced. Therefore, monitoring of particulate matter

73

and their chemical composition of aerosol particles in Ballari is needful for identification

74

of emissions sources, determination of compliance for air quality standards, and

75

establishment of effective pollution control programs.

76

The goal of the present work is to report on the chemical characterization and

77

source identification of near-surface total particulate matter in an urban environment

78

(Ballari) in the Southern part of India. Samples were collected for 28 days in between

79

February 2017 to July 2018 over Ballari. However, we also analyzed elemental

80

composition and morphology of particulate matter on hazy and clear days and these are

81

compared with their respective lidar-based (CALIPSO) aerosol types over the 3

82

measurement location. Further, Concentration weighted trajectory (CWT) is concurrently

83

discussed using back trajectories to realize the regional transport of aerosols. Our analysis

84

is for the first time the chemical characterization of particulate matter and their sources

85

relating to the study area.

86

1.1 Description of Study Area

87

Ballari is a major city in the state of Karnataka, India. It is 311 km from the state

88

capital of Bengaluru and 358 km from Hyderabad. Ballari is located at 15.15°N 76.93°E

89

(Fig.1a). It has an average elevation of 495 metres (1,624 ft). Historical sites, farmland

90

and rich minerals characterize in Ballari district. Also, cotton processing and garment

91

manufacture are one of the major industries around Ballari. Daily mean variation of the

92

temperature and Relative Humidity (RH) over the sampling location is shown in Fig.1b.

93

The ambient temperature (RH) shows a higher value in summer days and lower in winter

94

days. The average temperature and RH during the observational period is ~ 29 C ±4(~55

95

± 16 %).

96

2.0 Instrumentation

97

2.1 High Volume Sampler

98

The ambient air sample with diameters greater than 100 µm were collected using

99

the high volume sampler (HVS model: PEM-HVS-4 NL), which operate at a flow rate of

100

140 LPM (Litre Per Minute). It has 2% offset value of flow control accuracy. It collects

101

air samples through a pre-weighed filter paper for 24 hours of continuous exposure. After

102

sampling, the filter is re-weighed and the difference in filter weight is the collected

103

particulate matter mass. Dividing the mass by the volume of air sampled gives the

104

concentration of TSP. Quartz fibre filters with a diameter of 47mm are used for the

105

present study. Sampling was conducted at Ballari and each sample had a sampling

106

duration of 24 h (6:00 am to 6:00 am) during 2017-18 at Ballari.

107 108

2.2. Methodology

109

investigations of environmental aerosols, including particle composition identification,

110

size and shape classifications (Roberto et al., 2014; Matthew et al., 2017). In the present

111

study, the quartz filter tape was casually cut in size of about 1 mm 2 out of the main filter.

Scanning electron microscope (SEM) has been successfully applied in

4

112

A very thin film of carbon was deposited on the surface of the quartz filters to make

113

electrically conductive by using a vacuum coating unit. These samples were mounted on

114

electron microprobe stubs. The SEM - EDX analysis was conceded with the help of a

115

computer-controlled field emission equipped with an EVEX- EDX detection system. In

116

the present investigation, the SEM was used in the emission mode. The SEM was a

117

‘Merlin’ type manufacturer and SEM EDX facilities JEOL JSM-5600 available at Yogi

118

Vemana University, Kadapa (A.P).

119

For the identification of trace metals we have used the optima 2100 DV Perkin

120

Elmer, Inductively coupled plasma optical emission spectrometer (ICP-OES) In this

121

technique the sample is aspirated through the nebulizer which primarily charges the

122

liquid and transports it into the plasma flame (Malgorzata et al., 2016). The ICP-torch

123

consists of three concentric quartz glass tubes, a radio frequency (RF) and a Tesla coil.

124

Argon gas generates the plasma flame with a flow rate of 0.80 L/min. Nitrogen gas and

125

compressed air passed through the system with flow rates of 0.5 L/min and 2.0 L/min

126

respectively. The analyzed elements included the major (crustal) elements (Zn, Ba, Ca,

127

Al, Fe, Mg), sub-major and the ionic elements ( SO 24 , NH 4 , F−, NO 3 , Cl−).

128

2.3. CALIPSO

129

The Cloud-Aerosol Lidar with Orthogonal Polarization, onboard the CALIPSO platform,

130

is a dual-wavelength polarization lidar measuring attenuated backscatter radiation at 532

131

and 1064 nm since June 2006 (Winker et al., 2009). We used Version 4.1 of the Level 2

132

images was obtained to identify the aerosol types. CALIPSO infers an aerosol subtype

133

classification based on aerosol geographic location, the underlying surface type (land vs.

134

water), layer integrated attenuated backscatter, depolarization ratio at 0.532 μm, and

135

observed aerosol altitude (Omar et al., 2009). The CALIPSO 5-km aerosol layer product

136

reports the spatial and optical properties of aerosol layers that were detected at horizontal

137

averaging resolutions of 5, 20, and80 km, and vertical resolutions of up to 30m (Vaughan

138

et al., 2009; Omar et al., 2009; Kittaka et al., 2011; Young and Vaughan, 2018).

139

2.4. Concentration weighted trajectory (CWT) Analysis

140

To identify the relative contribution of potential source regions of aerosol getting

141

transported at the measurement location, CWT analysis was performed. In CWT 5

142

technique, the trajectories reaching over the measurement location were weighted based

143

on the mean concentration measured at the location during the arrival of the trajectory. In

144

this technique, each grid cell is assigned a concentration obtained by averaging associated

145

concentrations that had crossed the grid cell

146

C ij 

147

where Cij is the average weighted concentration in the ijth cell, l is the index of the

148

trajectory, M is the total number of trajectories, Cl is the concentration observed in the

149

trajectory endpoint and τijl is the time spent in the ijth cell by the trajectory l (Seibert et

150

al.,1994).

151

3.0 Results and discussion

152

3.1. Daily variation of total mass concentration and morphology, elemental

153

identification

154

The 24 hours near-surface total suspended mass concentration levels varied from 103 µg

155

m-3 to 367 µg m-3 with an average value of 225±65 µg m-3 over Ballari (Fig. 2). The high

156

concentration (334 µg m-3) was noticed on 24-01-2018, whereas low concentration was

157

(137 µg m-3) observed on 31-05-2017 during the study period. The significant variability

158

of total mass concentration was mainly due to the seasonal variability of aerosol sources

159

and local meteorological conditions. We also investigated the morphology and elemental

160

composition by using SEM coupled with EDX for six days samples. Particle morphology

161

and composition were classified based on the method widely applied by other researchers

162

(Sharma and Srinivas, 2009; Cong et al., 2010; Pipal et al., 2011; Pachauri et al., 2013;

163

Satsangi et al., 2014). Figure 3(a-f) shows the SEM images of total mass concentration on

164

different days collected at Ballari. The SEM pictures show the most notable deposition of

165

oval/spherical shapes with smooth surfaces, irregular, and amorphous shaped aggregates.

166

Numerous studies (Giere et al., 2006; Brown et al., 2011; Li and Shao, 2009) reported

167

that fly ash particles contain Si and Al with minor Ca, Ti, and those are in the amorphous

168

phase. Tripti et al., (2018) mentioned that biological related particles contain major C and

169

O with minor elements (Na, K, Cl, Al, Fe, Ca, Mg and Si) and those are in variable

M

1

lM1

 ijl

 Cl ijl

l 1

6

170

morphology. The percentage distribution of various elements presented in the total mass

171

concentration based on EDX spectra, as shown in Fig 4. Quartz fibre filters consist of

172

high amounts of Si and O (≈ 50% by weight) (Pachauri et al., 2013). Therefore, those two

173

elements were subtracted from the loaded filters. As shown in Fig. 4, Twenty-four

174

chemical parameters (C, O, Na, Mg, Al, Si, S, CI, Mo, K, Ca, Ba, Ti, Fe, Zn, Co, Hf and

175

Br) were determined and elemental levels of carbon (C) and aluminosilicates (containing

176

Al, Si, K, Fe, Na, Mg, Ti and Ca) were commonly noticed in all days. Major elements

177

detected in aluminosilicate particles (besides Al and Si, of course) include K, Ca, and Fe;

178

minor elements include Na, Mg, Ti, Zn, Mn, and Ni. This aluminosilicate group contains

179

about ~31 % of the total particles, which indicating the abundance of soil sediments and

180

road dust. Silicon (Si) is one of the largest constituents of soil-derived mineral particles,

181

resuspended road dust and aluminosilicates with significant levels of Al, Si and K can

182

also release from crustal sources, agricultural activities, and biomass burning. Further,

183

elemental levels of carbon particles (C) were significantly varied than other elements and

184

their percentage contribution was varied from 4-23% during the study period. The carbon

185

(C) species percentages were higher, except monsoon day (31-08-2017), which might be

186

associated with anthropogenic aerosols produced by agriculture activities. Van Malderen

187

et al., 1996; Cong et al., 2009 concluded that a major type of chemical compound in the

188

earth’s crest is an aluminosilicate group, which accounts for ~72% of the total particles.

189

Trace elements are important components of aerosols, and industrial, residential, and

190

traffic related activities have resulted in a substantial increase in trace metals (e.g., Cu,

191

Pb, Zn, Cd, Ni etc.) in the atmosphere (Watson et al., 2001; Gugamsetty et al., 2012).

192

Several studies show that ambient particulate pollution is associated with certain health

193

and environmental effects (Choosong et al., 2010; Ning et al., 2010; Wang et al., 2012).

194

3.2. CALIPSO vertical feature mask and morphology, elemental identification of

195

particulate matter on the clear and hazy event.

196

The CALIPSO vertical feature mask and aerosol subtypes observed on 23-02-

197

2018 (clear day) and 27-03-2018 (hazy day) are shown in Fig. 5(a ‒ d). On Clear day, the

198

aerosol vertical profile was relatively low (1‒ 3 km) due to the dominance of dust,

199

polluted dust (dust mixed with smoke) (Fig. 5a,b), whereas for hazy day, aerosol vertical 7

200

profile was found greater height (surface to 4km) due to the polluted continental, polluted

201

dust and smoke (Fig.5c,d). we also investigated the morphology and elemental

202

composition of aerosol particles by using SEM coupled with EDX for both clear and hazy

203

day samples. The clear (23-02-2018) and haze day (27-03-2018) images were captured

204

by the NASA both and Terra Aqua Moderate Resolution Imaging Spectroradiometer

205

(MODIS) satellite, as shown in the Fig. 6(a-d).The total mass concentration on the clear

206

and hazy days was found to be 227 and 327 µg m-3 at Ballari (Fig.2). The SEM pictures

207

confirm the most notable deposition of spherical particles with smooth surfaces on a hazy

208

day, which indicates that the smoke aerosols on haze day were favourable to the

209

coagulation of Aitken mode particles (Fig. 6f). Morphologically, soot particles can be

210

generally classified into three categories: oval/spherical, rod-like, and flocculent

211

amorphous bodies (Wu et al., 2015). Soot particles produced from combustion processes

212

were predominantly spherical and rounded with smooth surfaces. Soot particles emitted

213

from combustion processes were predominantly spherical and rounded with smooth

214

surfaces. However, we also analyzed the different elements presented in the total mass

215

concentration on typical clear, Hazy days in the region. As shown in Fig.6g, the

216

percentage of carbon particles is abundant (13.1%) on a hazy day compare to clear days

217

and it played a significant role in the formation of hazy over this region, which is

218

consistent with the respective CALIPSO aerosol subtypes observed over the study region.

219

3.3. Total Suspended Particulate and Major Ion Concentrations of Aerosol Samples

220

Figure 7 illustrates both elemental and ionic mass concentrations of particulate

221

matter on 01-01-2018 and 11-05-2017 over measurement location. The most abundant

222

elements in the particulate were Zn (10.79 µg m-3) Ba (9.75 µg m-3), Ca (15.36 µg m-3),

223

Al (5.19 µg m-3), Fe (7.38 µg m-3), Mg (1.46 µg m-3) followed by Mn, Sr, Ti, Cr, Pb, Cu,

224

As, Ni, Co, V and Sb was found were below 1 µg m-3 on 11-05-2017 (7a). Similarly, Ca

225

was the abundant element noted on 01-01-2018, whereas remaining elements

226

concentrations are nearly similar to the concentration observed on 11-05-2017. The mass

227

concentration of the inorganic ions on 11-05-2017 and 01-01-2018 days were SO 24 (>7.5

228

µg m-3) followed by NO 3 (>7 µg m-3), Na+ (>2 µg m-3), and Ca2+, Cl-, NH 4 , K+, F-, Br-

229

were (<2µg m-3) (Fig. 7b). 8

230

The estimated percentage contribution of both ion and ionic mass followed by an

231

order of SO 24 > NO 3 > Cl- > F- > Br- for anions and Na+ > Ca2+ > NH 4 > K+ for cations.

232

The higher portion was occupied by SO 24 (37.71%) to the mass followed by NO3-

233

(30.47%), Na+ (11.14 %), Ca2+ (10.5%) and Cl- (4.47%) (Fig.8b). The contribution of

234

anions share was high (~73.89%), and cations contribution was low (~26.10%) over the

235

observational site on 11-05-2017.

236

The percentage contribution on 01-01-2018 was followed by an order SO 24 >

237

NO 3 > Cl > Br > F for anions and Na > Ca

238

portion was occupied by SO 24 (34.81%) to the mass followed by NO 3 (31.11%), Na+

239

(11.78 %), Ca2+ (9.19%) and Cl- (7.46%). The contribution of anions share was high

240

(~74.39%), and cations contribution was low (~25.60%) over the study region (Fig. 8d).

241

Since the measurement location is too far away from the coast, hence, the contribution of

242

sea-salt sulphate will be insignificant. This was further confirmed by a high SO 24 /Na+

243

ratio was 1.11 and 1.23 on 11-05-2017 and 01-01-2018, respectively. Begum et al. (2017)

244

noticed high SO42− (11.7 μg m−3) at a suburban location over Kadapa and they concluded

245

that sulphate might be soil-derived components or formed by the reactions of gas-phase

246

sulphur dioxide. The relatively low ratio of NO 3 / SO 24 (< 1.0) indicated that industrial

247

emissions played a key role compared to mobile sources (Lai et al. 2007), like vehicular

248

emissions over the study region. The average concentration of K+ was only 0.19 μg m−3

249

and 0.22 μg m−3 (0.75 % and 1.01%) was observed on 11-05-2017 and 01-01-2018,

250

respectively. The mining activity is the main source for the occurrence of K+, Ca2+ and

251

Na+ over the study area. The observed average concentration of NH4+ was 0.71 μg m−3

252

and 0.91 μg m−3 (3.19 % and 4.11%) on 11-05-2017 and 01-01-2018, respectively,

253

produced from the agricultural farmlands and anthropogenic activities.

254

4. Source apportionment

-

-

-

+

2+

> NH 4 > K+ for cations. The higher

255

The CWTs were calculated for total suspended particulate mass concentration and

256

are shown in Fig. 9. This indicates that the sampling site is getting affected mostly due to

257

the local contribution and far moderate from the southeast continental region of India.

258

The sampling site surrounded by the eight iron ore mining’s, 6 coal-based power plants 9

259

and 2 steel plants, which are major emission sources for PM concentration levels. The

260

results reveal that the local emissions are representing the most important potential

261

sources for PM concentrations. Air masses originating from the Arabian Peninsula and

262

Bay of Bengal Persian Gulf traversing the northern AS can also contribute to medium BC

263

mass concentrations, while the air masses from southern AS seem to be cleaner.

264

5 Conclusions

265

Monitoring and analysis of the chemical composition of air pollutants were

266

conducted for 28 sampling days between February 2017-July 2018 in the sub-urban area of

267

Ballari. The main findings can be summarized as follows:

268



value of ~ 225±65 µg m-3 during the study period.

269 270

The total mass concentration varied from 103 µg m-3 to 367 µg m-3 with an average



The SEM pictures show the most notable deposition of oval/spherical shapes with

271

smooth surfaces and EDX results confirmed aluminosilicate group (Al, Si, K, Fe, Na,

272

Mg,Ti and Ca) accounted for ~31 % of the total suspended particulate matter over the

273

measurement location.

274



The carbon particles displayed a higher percentage (13.1%) of the total mass

275

concentration on hazy day than that (9.3%) on clear day, which consistent with

276

respective calipso aerosol subtypes observed over the measured location.

277



278 279

ICP-OES results showed the relative contribution of anions was higher (~74.39%) than cations (~25.60%) over the observational site.



The CWTs analysis revealed that numerous sources were contributing over pollution

280

in Ballari such as carbon aerosols from vehicles, mining activities local and

281

transported dust particles.

282

Acknowledgment

283

The authors wish to thank the Indian Space Research Organization Bangalore, for

284

their financial support under the project ISRO-GBP (ARFI & AT-CTM). We

285

acknowledge the NOAA Air Resources Laboratory for the provision of the HYSPLIT

286

transport and dispersion model. We are also grateful to NASA for providing CALIPSO

287

data.

288

References 10

289

Babu, S., Manoj, M. R., Moorthy, K. K., Gogoi, M. M., Nair, V. S., Kompalli, S.K.,

290

Satheesh, S. K., Niranjan, K., Ramagopal, K., Bhuyan, P. K., Singh, D., 2013.

291

Trends in aerosol optical depth over Indian region: Potential causes and impact

292

indicators. J. Geophys. Res. Atmos. 11, 11794–11806.

293

Begam, G.R., Vachaspati, C.V., Ahammed, Y.N., Kumar, K.R., Reddy, R.R., Sharma,

294

S.K., Saxena, M., Mandal, T.K., 2017. Seasonal characteristics of water-soluble

295

inorganic ions and carbonaceous aerosols in total suspended particulate matter at a

296

rural semi-arid site, Kadapa (India). Environ. Sci. Pollut. Res. 24, 1719–1734.

297

Boiyo, R., Kumar, K.R., Zhao, T., 2018. Spatial variations and trends in AOD

298

climatology over East Africa during 2002–2016: a comparative study using three

299

satellite data sets. Int. J. Climat. 38, 1221–1240.

300

Brown, P., Jones, T., BéruBé, K., 2011. The internal microstructure and fibrous

301

mineralogy of fly ash from coal-burning power stations. Environ. Pollut. 159,

302

3324–3333.

303

Campos‐ Ramos, A., Aragon‐ Pina, A., Galindo‐ Estrada, I., Querol, X., Alastuey, A.,

304

2009. Characterization of atmospheric aerosols by SEM in a rural area in the

305

western part of Mexico and its relation with different pollution sources. Atmos.

306

Environ., 43, 6159–6167.

307

Casimiro P., Mirante, F., Oliveira, C., Matos, M., Caseiro, A., Oliveira, C., Xavier, Q.,

308

Célia, A., Natércia, M., Mário, C., Filomena, C., Hugo, S., Feliciano, P., 2013.

309

Size-segregated chemical composition of aerosol emissions in an urban road tunnel

310

in Portugal. Atmos. Environ. 71, 15–25.

311

Choosong, T., Chomanee, J., Tekasakul, P., Tekasakul, S., Otani, Y., Hata, M., Furuuchi,

312

M., 2010. Workplace Environment and Personal Exposure of PM and PAHs to

313

Workers in Natural Rubber Sheet Factories Contaminated by Wood Burning Smoke.

314

Aerosol Air Qual. Res. 10, 8–21.

315

Cong, Z., Kang, S., Dong, S. and Zhang, Y., 2009. Individual Particle Analysis of

316

Atmospheric Aerosols at Nam Co, Tibetan Plateau. Aerosol Air Qual. Res. 9, 323–

317

331.

11

318

Cong, Z., Kang, S., Dong, S., Liu, X., Qin, D., 2010. Elemental and individual particle

319

analysis of atmospheric aerosols from high Himalayas. Environ. Mon. Asses. 160,

320

323–335.

321

Giere, R., Blackford, M., Smith, K., 2006. TEM study of PM2.5 emitted from coal and tire

322

combustion in a thermal power station. Environ. Sci. Technol. 40, 6235–6240.

323

Gugamsetty, B., Wei, H., Liu, C.N., Awasthi, A., Hsu, S.C., Tsai, C.J., Roam, G.D., Wu,

324

Y.C., Chen, C.F., (2012). Source characterization and apportionment of PM10,

325

PM2.5 and PM0.1 by using positive matrix factorization. Aerosol Air Qual. Res. 12,

326

476–491.

327

Huang, X.F., Yu, J.Z., He, L.Y., Yuan, Z., 2006. Water-soluble organic carbon and

328

oxalate in aerosols at a coastal urban site in China: Size distribution characteristics,

329

sources, and formation mechanisms. J. Geophys. Res. 111, D22212.

330

Kittaka, C., Winker, D.M., Vaughan, M.A., Omar, A., Remer, L.A., 2011. Inter-

331

comparison of column aerosol optical depths from CALIPSO and MODIS-Aqua

332

Atmos. Meas. Tech.. 4, 131–141.

333 334

Li, W.J., Shao, L.Y., 2009. Transmission electron microscopy study of aerosol particles from the brown hazes in northern China. J. Geophys. Res. 114, D09302.

335

Malgorzata H., Magdalena, G., Piekoszewski, W., Walas, S., Napierala, M.,

336

Wyganowska-Swiatkowska, M., Kurhanska-Flisykowska, A., Wozniak, A., Florek

337

E., (2016). Essential and Toxic Metals in Oral Fluid– a Potential Role in the

338

Diagnosis of Periodontal Diseases. Biol. Tra. Elem. Res. 173, 275–282.

339

Ning, Z., Sioutas, C., 2010. Atmospheric Processes Influencing Aerosols Generated by

340

Combustion and the Inference of their Impact on Public Exposure: A Review.

341

Aerosol Air Qual. Res. 10, 43–58.

342

Omar, A.H., Winker, D.M., Kittaka, C., Vaughan, M.A., Liu, Z., Hu, Y., Trepte, C.R.,

343

Rogers, R.R., Ferrare, R.A., Lee, K.P., Kuehn, R.E., Hostetler, C.A., 2009. The

344

CALIPSO automated aerosol classification and lidar ratio selection algorithm. J.

345

Atmos. Ocean Techn. 26, 1994–2014.

12

346

Pachauri, T., Singla, V., Satsangi, A., Lakhani, A. and Kumari, K.M., 2013. SEM-EDX

347

characterization of individual coarse particles in Agra. India Aerosol Air Qual. Res.

348

13, 523–536.

349 350

Partanen A., Sébastien, J.L., Matthews, H. D., 2018. Climate and health implications of future aerosol emission scenarios. Environ. Res. Lett. 13(2), 024028.

351

Pipal, A.S., Kulshrestha, A., Taneja, A., 2011. Characterization and morphological

352

analysis of airborne PM2.5 and PM10 in Agra located in north central India. Atmos.

353

Environ. 45, 3621–3630.

354 355

Pöschl, U., 2005. Atmospheric Aerosols: Composition, Transformation, Climate and Health Effects. Angewandte Chemie International Edition, 44, 7520–7540.

356

Rama Gopal, K., Arafath, S., Balakrishnaiah, G., Raja Obul Reddy, K., Siva Kumar

357

Reddy, N., Lingaswamy, A.P., PavanKumari, S., Uma Devi, K., Reddy, R.R., Babu,

358

S.S., 2015. Columnar-integrated aerosol optical properties and classification of

359

different aerosol types over the semi-arid region Anantapur. Sci. Total Environ.

360

(527–528), 507–519.

361

Reddy, K.R.O., Balakrishnaiah, G., Gopal, K., Reddy, N.S.K., Chakradhar Rao, T.,

362

Reddy, L.T., Reddy, Reddy R.R., Babu, S., 2016a. Direct radiative forcing

363

properties of atmospheric aerosols over semi–arid region, Anantapur in India. Sci.

364

Total Environ. (566–567), 1002–1013.

365

Reddy, K.R.O., Balakrishnaiah, G., Gopal, K., Reddy, N.S.K., Chakradhar Rao, T.,

366

Reddy, L.T., Reddy, Hussain N.S., Reddy, M.V., Reddy, R. R., Boreddy, S.K.R.,

367

Babu, S., 2016b. Long term (2007 – 2013) observations of columnar aerosol optical

368

properties and retrieved size distributions over Anantapur, India using Multi

369

Wavelength solar Radiometer. Atmos. Environ.142, 238–250.

370

Satsangi, P.G., Yadav, S., 2014. Characterization of PM2.5 by X-ray diffraction and

371

scanning electron microscopy-energy dispersive spectrometer: Its relation with

372

different pollution sources. Int. J. Environ. Sci. Technol. 11, 217–232.

373

Sharma, S., Srinivas, M., 2009. Study of chemical composition and morphology of

374

airborne particles in Chandigarh, India using EDXRF and SEM techniques.

375

Environ. Moni. Assess. 150, 417–425. 13

376

Srivastava, A., Jain, V.K., 2007. Size distribution and source identification of total

377

suspended particulate matter and associated heavy metals in the urban atmosphere

378

of Delhi. Chemosp., 68(3), 579–589.

379

Timonen, H., Saarikoski, S., Tolonen-Kivimäki, O., Aurela, M., Saarnio, K., Petäjä,

380

T., Aalto, P.P., Kulmala, M., Pakkanen, T., Hillamo, R., 2018. Size distributions,

381

sources and source areas of water-soluble organic carbon in urban background air.

382

Atmos. Chem. Phys. 8, 5635–5647.

383

Tripti, P., Singla, V., Satsangi, A., Lakhani, A., Kumari, M.K., 2013. SEM-EDX

384

characterization of Individual Coarse Particles in Agra, India. Aerosol Air Qual.

385

Res. 13, 523–536.

386

Van Malderen, H., Van Grieken, R., Bufetov, N.V., Koutzenogii, K.P., (1996). Chemical

387

Characterization of Individual Aerosol Particles in Central Siberia. Environ. Sci.

388

Tech. 30, 312–321.

389

Vaughan, M.A., Powell, K.A., Kuehn, R.E., Young, S.A., Winker, D.M., Hostetler, C.A.,

390

Hunt, W.H., Liu, Z.Y., McGill, M.J., Getzewich, B.J., 2009. Fully automated

391

detection of cloud and aerosol layers in the CALIPSO lidar measurements. J.

392

Atmos. Ocean Tech. 26, 2034–2050.

393

Wang, Y., Xin, Y., Li, Z., Wang, S., Wang, P., Hao, M.W., Nordgren, L.B., Chen, H.,

394

Wang, L., Sun. Y., 2011. Seasonal variations in aerosol optical properties over

395

China. J. Geophys. Res. 116, D18209.

396

Wang, Y., Zhuang, G., Sun, Y., Zhisheng, A., 2006. The Variation of Characteristics and

397

Formation Mechanisms of Aerosols in Dust, Haze, and Clear Days in Beijing.

398

Atmos. Environ. 40, 6579–6591.

399

Wang Z.S., Wu, Ting., Shi, G.L., Fu, X., Tian, Y., Feng, Y.C., Wu, X.F., Wu, G., Bai,

400

X.P., Zhang, W.J., 2012. Potential Source Analysis for PM10 and PM2.5 in

401

Autumn in a Northern City in China. Aerosol Air Qual. Res. 12, 39–48.

402

Watson, J.G., Chow, J.C., 2001. PM2.5 chemical source profiles for vehicle exhaust,

403

vegetative burning, geological material, and coal burning in northwestern Colorado

404

during 1995. Chemos. 43, 1141–1151.

14

405

Winker, D.M., Vaughan, M.A., Omar, A., Hu, Y., Powell, K.A., Liu, Z., Hunt, W.H.,

406

Young, S.A., 2009. Overview of the CALIPSO Mission and CALIOP data

407

processing Algorithms. J. Atmos. Ocean. Technol. 26(11), 2310–2323.

408

Young, A.S., Vaughan, A.M., Garnier, A., Tackett, L.J., Lambeth, D.J., Powell, A.K.,

409

2018. Extinction and optical depth retrievals for CALIPSO’s Version 4 data release.

410

Atmos. Meas. Tech. 11, 5701–5727.

411

Yu, G., Zhang, Y., Cho, S.Y., Park, S., 2017. Influence of haze pollution on water-

412

soluble chemical species in PM2.5 and size-resolved particles at an urban site during

413

fall. J. Environ. Sci. 57, 370-382.

15

Fig.1(a-b). Schematic site map of the sampling site and prevailing meteorological features (Temperature & Relative Humidity) over sampling site during the study period Fig.2. Daily variation of the total mass concentration measured at Ballari. Fig.3. Scanning electron images and energy dispersive X-ray spectra of aerosols. Fig.4. The percentage contribution of each elemental composition obtained from EDX spectra of aerosols at Ballari. Fig.5. CALIPSO-retrieved vertical feature mask and aerosol subtype images on clear day (23-02-2018) and hazy day (27-03-2018). The marked with red colour oval shape around the measurement location. Fig.6. MODIS both Terra and AQUA satellite images (a) MODIS Terra image on clear day (23-02-2018) (b) MODIS Aqua image on clear day (23-02-2018) (c) MODIS Terra image on Hazy day (27-03-2018) (d) MODIS Aqua image on hazy day (27-03-2018) over sampling location. The circle in each map indicates the sampling location. Typical examples of different scanning electron micrographs of aerosols and their percentage contribution of each elemental composition obtained from EDX spectra of aerosol on both clear and hazy days at Ballari (e-g). Fig.7. Mass concentration of various elements and ions in the total mass concentration on 1105-2017 and 01-01-2018 at Ballari. Fig.8. Percentage contribution of various elements and ions in the total mass concentration on 11-05-2017 and 01-01-2018 at Ballari. Fig.9. Concentration Weighted Trajectories map for total suspended particulate mass concentration with 1° resolution for the 28 collected samples using HVS. The highly concentrated area is enlarged which clearly shows the possible source areas (Cyan circles indicates Iron Ore mining areas, Orange coloured triangle indicates coal based power plants, black coloured rhombus indicates steel and cement plants and black coloured star indicates the sampling site).

Fig. 1(a).

Fig. 2(b).

Fig. 2.

(a) 31-08-2017

(b) 08-11-2017

(c) 24-01-2018

(d) 07-02-2018

(e) 14-03-2018

(f) 11-04-2018

Fig. 3.

Fig. 4.

(a)

(b)

(c)

(d)

Fig. 5.

(b) 23-02-2018 MODIS Aqua Aqua

(a) 23-02-2018 MODIS Terra

(c) 27-03-2018 MODIS Terra Terra

(d) 27-03-2018 MODIS Aqua Aqua

(e) 23-02-2018

(f) 27-03-2018

Fig. 6.

Fig. 7.

Fig. 8.

Fig. 9.

 The total mass concentration varied from 103 µg m-3 to 367 µg m-3 over Bellary.  EDX results showed aluminosilicate group contains about ~31 % during study period.  ICP-OES analysis confirmed the inorganic ions dominant over study region.  CWT results showed the major sources were mining and anthropogenic sources over location.