Abstract
Carbonaceous aerosols play an important role in affecting human health, radiative forcing, hydrological cycle, and climate change. As our current understanding about the carbonaceous aerosols, the source(s) and process(es) associated with them in the ecologically sensitive North-Western Himalayas are limited; this systematic study was planned to understand inherent dynamics in the mass concentration and source contribution of carbonaceous aerosols in the Dhauladhar region. During four winter months (January 2015–April 2015), 24-h PM10 samples were collected every week simultaneously at the rural site of Pohara (32.19° N, 76.20° E; 750 m amsl) and the urban location of Dharamshala (32.20° N, 76.32° E; 1350 m amsl). These samples were analyzed by using thermal/optical carbon analyzer for different carbon forms. Organic carbon (OC) dominated over elemental carbon (EC) and was found to be 59.3 and 64.1% in total carbon (TC) at Pohara and Dharamshala, respectively. The respective mass concentrations of OC and EC were higher at Pohara (6.8 ± 2.3 and 4.8 ± 2.0 μg.m−3) in comparison to that observed in Dharamshala (5.0 ± 3.1 and 2.5 ± 0.6 μg.m−3). The OC/EC ratio at Pohara (1.51 ± 0.41) indicates the dominance of fossil fuel combustion (coal and vehicular exhaust), while at Dharamshala, an OC/EC of 2.01 ± 1.07 signified additional contribution from secondary organic carbon (SOC). Diagnostic ratios (OC/EC and char-EC/soot-EC) suggested dominance of emissions from fossil fuel combustion sources over biomass burning sources in the region. Estimated non-sea salt (nss)K+/OC and nssK+/EC ratios indicated heterogeneity within the biomass burning sources over low and high altitude locations. A strong correlation between nssK+ and SOC over a high altitude urban location further suggested possible conversion of gaseous precursors to carbonaceous particles during coniferous wood burning.
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References
Andreae MO, Merlet P (2001) Emission of trace gases and aerosols from biomass burning. Glob Biogeochem Cycles 15(4):955–966. https://doi.org/10.1029/2000GB001382
Begam GR, Vachaspati CV, Ahammed YN, Kumar KR, Reddy RR, Sharma SK, Saxena M, Mandal TK (2017) Seasonal characteristics of water-soluble inorganic ions and carbonaceous aerosols in total suspended particulate matter at a rural semi-arid site, Kadapa (India). Environ Sci Pollut Res 24(2):1719–1734. https://doi.org/10.1007/s11356-016-7917-1
Bhattu D, Tripathi SN, Chakraborty A (2016) Deriving aerosol hygroscopic mixing state from size-resolved CCN activity and HR-ToF-AMS measurements. Atmos Environ 142:57–70. https://doi.org/10.1016/j.atmosenv.2016.07.032
Bhuyan P, Barman N, Bora J, Daimari R, Deka P, Hoque RR (2016) Attributes of aerosol bound water soluble ions and carbon, and their relationships with AOD over the Brahmaputra Valley. Atmos Environ 142:194–209. https://doi.org/10.1016/j.atmosenv.2016.07.045
Bisht DS, Dumka UC, Kaskaoutis DG, Pipal AS, Srivastava AK, Soni VK, Attri SD, Sateesh M, Tiwari S (2015) Carbonaceous aerosols and pollutants over Delhi urban environment: temporal evolution, source apportionment and radiative forcing. Sci Total Environ 521-522:431–445. https://doi.org/10.1016/j.scitotenv.2015.03.083
Cao J (2003) Characteristics of carbonaceous aerosol in Pearl River Delta Region, China during 2001 winter period. Atmos Environ 37(11):1451–1460. https://doi.org/10.1016/S1352-2310(02)01002-6
Cao J, Wu F, Chow J, Lee S, Li Y, Chen S, An Z, Fung K, Watson J, Zhu C (2005) Characterization and source apportionment of atmospheric organic and elemental carbon during fall and winter of 2003 in Xi’an, China. Atmos Chem Phys 5(11):3127–3137. https://doi.org/10.5194/acp-5-3127-2005
Cao J, Lee S, Ho K, Fung K, Chow JC, Watson JG (2006): Characterization of roadside fine particulate carbon and its eight fractions in Hong Kong. Aerosol Air Qual. Res 6
Cao JJ, Lee SC, Chow JC, Watson JG, Ho KF, Zhang RJ, Jin ZD, Shen ZX, Chen GC, Kang YM, Zou SC, Zhang LZ, Qi SH, Dai MH, Cheng Y, Hu K (2007): Spatial and seasonal distributions of carbonaceous aerosols over China. Journal of Geophysical Research Atmospheres 112 (22), D22S11
Cao J, Shen Z, Chow JC, Qi G, Watson JG (2009) Seasonal variations and sources of mass and chemical composition for PM10 aerosol in Hangzhou, China. Particuology 7(3):161–168. https://doi.org/10.1016/j.partic.2009.01.009
Census (2011) Census of India - 2011. Available at http://www.censusindia.gov.in
Chakraborty A, Rajeev P, Rajput P, Gupta T (2017) Water soluble organic aerosols in indo gangetic plain (IGP): insights from aerosol mass spectrometry. Sci Total Environ 599-600:1573–1582. https://doi.org/10.1016/j.scitotenv.2017.05.142
Chatterjee A, Dutta C, Jana T, Sen S (2012) Fine mode aerosol chemistry over a tropical urban atmosphere: characterization of ionic and carbonaceous species. J Atmos Chem 69(2):83–100. https://doi.org/10.1007/s10874-012-9231-8
Chow JC, Watson JG, Chen LWA, Chang MCO, Robinson NF, Trimble D, Kohl S (2007) The IMPROVE_a Temperature protocol for thermal/optical carbon analysis: maintaining consistency with a long-term database. J Air Waste Manage Assoc 57(9):1014–1023. https://doi.org/10.3155/1047-3289.57.9.1014
Duan FK, He KB, Ma YL, Yang FM, XC Y, Cadle SH, Chan T, Mulawa PA (2006) Concentration and chemical characteristics of PM2.5 in Beijing, China: 2001–2002. Sci Total Environ 355(1-3):264–275. https://doi.org/10.1016/j.scitotenv.2005.03.001
Gelencsér A (2004) Carbonaceous aerosol, atmospheric and oceanographic sciences library, 30. Springer, The Netherlands, p 350
Gustafsson Ö, Kruså M, Zencak Z, Sheesley RJ, Granat L, Engström E, Praveen P, Rao P, Leck C, Rodhe H (2009) Brown clouds over South Asia: biomass or fossil fuel combustion? Science 323(5913):495–498. https://doi.org/10.1126/science.1164857
Han Y, Cao J, Chow JC, Watson JG, An Z, Jin Z, Fung K, Liu S (2007) Evaluation of the thermal/optical reflectance method for discrimination between char- and soot-EC. Chemosphere 69(4):569–574. https://doi.org/10.1016/j.chemosphere.2007.03.024
Han YM, Han ZW, Cao JJ, Chow JC, Watson JG, An ZS, Liu SX, Zhang RJ (2008) Distribution and origin of carbonaceous aerosol over a rural high-mountain lake area, Northern China and its transport significance. Atmos Environ 42(10):2405–2414. https://doi.org/10.1016/j.atmosenv.2007.12.020
Han YM, Lee SC, Cao JJ, Ho KF, An ZS (2009) Spatial distribution and seasonal variation of char-EC and soot-EC in the atmosphere over China. Atmos Environ 43(38):6066–6073. https://doi.org/10.1016/j.atmosenv.2009.08.018
Han Y, Cao J, Lee S, Ho K, An Z (2010) Different characteristics of char and soot in the atmosphere and their ratio as an indicator for source identification in Xi’an, China. Atmos Chem Phys 10(2):595–607. https://doi.org/10.5194/acp-10-595-2010
He K, Yang F, Ma Y, Zhang Q, Yao X, Chan CK, Cadle S, Chan T, Mulawa P (2001) The characteristics of PM 2.5 in Beijing, China. Atmos Environ 35(29):4959–4970. https://doi.org/10.1016/S1352-2310(01)00301-6
Huma B, Yadav S, Attri AK (2016) Profile of particulate-bound organic compounds in ambient environment of Srinagar: a high-altitude urban location in the North-Western Himalayas. Environ Sci Pollut Res 23(8):7660–7675. https://doi.org/10.1007/s11356-015-5994-1
Jacobson MZ (2006) Effects of externally-through-internally-mixed soot inclusions within clouds and precipitation on global climate. J Phys Chem A 110(21):6860–6873. https://doi.org/10.1021/jp056391r
Kaul DS, Gupta T, Tripathi SN, Tare V, Collett JL (2011) Secondary organic aerosol: a comparison between foggy and nonfoggy days. Environ Sci Technol 45(17):7307–7313. https://doi.org/10.1021/es201081d
Kirillova EN, Andersson A, Sheesley RJ, Kruså M, Praveen PS, Budhavant K, Safai PD, Rao PSP, Gustafsson Ö (2013) 13C- and 14C-based study of sources and atmospheric processing of water-soluble organic carbon (WSOC) in South Asian aerosols. J Geophys Res Atmos 118(2):614–626. https://doi.org/10.1002/jgrd.50130
Kumar A, Attri AK (2016) Biomass combustion a dominant source of carbonaceous aerosols in the ambient environment of Western Himalayas. Aerosol Air Qual Res 16(3):519–529. https://doi.org/10.4209/aaqr.2015.05.0284
Kumar A, Ram K, Ojha N (2016) Variations in carbonaceous species at a high-altitude site in Western India: role of synoptic scale transport. Atmos Environ 125:371–382. https://doi.org/10.1016/j.atmosenv.2015.07.039
Kumar P, Yadav S (2016) Seasonal variations in water soluble inorganic ions, OC and EC in PM10 and PM>10 aerosols over Delhi: influence of sources and meteorological factors. Aerosol Air Qual Res 16(5):1165–1178. https://doi.org/10.4209/aaqr.2015.07.0472
Lambe AT, Chhabra PS, Onasch TB, Brune WH, Hunter JF, Kroll JH, Cummings MJ, Brogan JF, Parmar Y, Worsnop DR, Kolb CE, Davidovits P (2015) Effect of oxidant concentration, exposure time, and seed particles on secondary organic aerosol chemical composition and yield. Atmos Chem Phys 15(6):3063–3075. https://doi.org/10.5194/acp-15-3063-2015
Lim H-J, Turpin BJ (2002) Origins of primary and secondary organic aerosol in Atlanta: results of time-resolved measurements during the Atlanta supersite experiment. Environ Sci Technol 36(21):4489–4496. https://doi.org/10.1021/es0206487
Mkoma SL, Kawamura K, Fu PQ (2013) Contributions of biomass/biofuel burning to organic aerosols and particulate matter in Tanzania, East Africa, based on analyses of ionic species, organic and elemental carbon, levoglucosan and mannosan. Atmos Chem Phys 13(20):10325–10338. https://doi.org/10.5194/acp-13-10325-2013
Moorthy KK, Satheesh SK, Sarin MM, Panday AK (2016) South Asian aerosols in perspective: preface to the special issue. Atmos Environ 125:307–311. https://doi.org/10.1016/j.atmosenv.2015.10.073
Novakov T, Andreae M, Gabriel R, Kirchstetter T, Mayol-Bracero O, Ramanathan V (2000) Origin of carbonaceous aerosols over the tropical Indian Ocean: biomass burning or fossil fuels. Geophys Res Lett 27(24):4061–4064. https://doi.org/10.1029/2000GL011759
Pachauri T, Singla V, Satsangi A, Lakhani A, Kumari KM (2013) Characterization of carbonaceous aerosols with special reference to episodic events at Agra, India. Atmos Res 128:98–110. https://doi.org/10.1016/j.atmosres.2013.03.010
Pant P, Baker SJ, Shukla A, Maikawa C, Godri Pollitt KJ, Harrison RM (2015) The PM10 fraction of road dust in the UK and India: characterization, source profiles and oxidative potential. Sci Total Environ 530-531:445–452. https://doi.org/10.1016/j.scitotenv.2015.05.084
Pipal AS, Tiwari S, Satsangi PG, Taneja A, Bisht DS, Srivastava AK, Srivastava MK (2014) Sources and characteristics of carbonaceous aerosols at Agra “world heritage site” and Delhi “capital city of India”. Environ Sci Pollut Res 21(14):8678–8691. https://doi.org/10.1007/s11356-014-2768-0
Panicker AS, Ali K, Beig G, Yadav S (2015) Characterization of particulate matter and carbonaceous aerosol over two urban environments in Northern India. Aerosol Air Qual Res 15(7). https://doi.org/10.4209/aaqr.2015.04.0253
Pavuluri CM, Kawamura K, Aggarwal SG, Swaminathan T (2011) Characteristics, seasonality and sources of carbonaceous and ionic components in the tropical aerosols from Indian region. Atmos Chem Phys 11(15):8215–8230. https://doi.org/10.5194/acp-11-8215-2011
Pio C, Cerqueira M, Harrison RM, Nunes T, Mirante F, Alves C, Oliveira C, de la Campa AS, Artíñano B, Matos M (2011) OC/EC ratio observations in Europe: re-thinking the approach for apportionment between primary and secondary organic carbon. Atmos Environ 45(34):6121–6132. https://doi.org/10.1016/j.atmosenv.2011.08.045
Pipal AS, Gursumeeran Satsangi P (2015) Study of carbonaceous species, morphology and sources of fine (PM2.5) and coarse (PM10) particles along with their climatic nature in India. Atmos Res 154:103–115. https://doi.org/10.1016/j.atmosres.2014.11.007
Popovicheva OB, Kozlov VS, Engling G, Diapouli E, Persiantseva NM, Timofeev M, Fan T-S, Saraga D, Eleftheriadis K (2015) Small-scale study of Siberian biomass burning: I. Smoke microstructure. Aerosol Air Qual Res 15:117–128
Poschl U (2005) Atmospheric aerosols: composition, transformation, climate and health effects. Angew Chem 44(46):7520–7540. https://doi.org/10.1002/anie.200501122
Rajput P, Sarin M, Sharma D, Singh D (2014): Characteristics and emission budget of carbonaceous species from post-harvest agricultural-waste burning in source region of the Indo-Gangetic Plain. Tellus, Series B: Chemical and Physical Meteorology 66 (1), 21026
Ram K, Sarin MM, Hegde P (2008) Atmospheric abundances of primary and secondary carbonaceous species at two high-altitude sites in India: Sources and temporal variability. Atmos Environ 42(28):6785–6796
Ram K, Sarin MM, Tripathi SN (2012) Temporal trends in atmospheric PM(2).(5), PM(1)(0), elemental carbon, organic carbon, water-soluble organic carbon, and optical properties: impact of biomass burning emissions in the Indo-Gangetic Plain. Environ Sci Technol 46(2):686–695. https://doi.org/10.1021/es202857w
Ram K, Tripathi SN, Sarin MM, Bhattu D (2014) Primary and secondary aerosols from an urban site (Kanpur) in the Indo-Gangetic Plain: impact on CCN, CN concentrations and optical properties. Atmos Environ 89:655–663. https://doi.org/10.1016/j.atmosenv.2014.02.009
Rastogi N, Singh A, Singh D, Sarin MM (2014) Chemical characteristics of PM2.5 at a source region of biomass burning emissions: evidence for secondary aerosol formation. Environ Pollut 184:563–569. https://doi.org/10.1016/j.envpol.2013.09.037
Rastogi N, Singh A, Sarin MM, Singh D (2016) Temporal variability of primary and secondary aerosols over northern India: impact of biomass burning emissions. Atmos Environ 125:396–403. https://doi.org/10.1016/j.atmosenv.2015.06.010
Rengarajan R, Sarin MM, Sudheer AK (2007) Carbonaceous and inorganic species in atmospheric aerosols during wintertime over urban and high-altitude sites in North India. J Geophys Res Atmos 112(21):D21307. https://doi.org/10.1029/2006JD008150
Rollins AW, Browne EC, Min KE, Pusede SE, Wooldridge PJ, Gentner DR, Goldstein AH, Liu S, Day DA, Russell LM, Cohen RC (2012) Evidence for NO(x) control over nighttime SOA formation. Science 337(6099):1210–1212. https://doi.org/10.1126/science.1221520
Safai PD, Raju MP, Rao PSP, Pandithurai G (2014) Characterization of carbonaceous aerosols over the urban tropical location and a new approach to evaluate their climatic importance. Atmos Environ 92:493–500. https://doi.org/10.1016/j.atmosenv.2014.04.055
Schauer JJ, Kleeman MJ, Cass GR, Simoneit BR (2001) Measurement of emissions from air pollution sources. 3. C1− C29 organic compounds from fireplace combustion of wood. Environ Sci Technol 35(9):1716–1728. https://doi.org/10.1021/es001331e
Schwarz JP, Gao RS, Spackman JR, Watts LA, Thomson DS, Fahey DW, Ryerson TB, Peischl J, Holloway JS, Trainer M, Frost GJ, Baynard T, Lack DA, de Gouw JA, Warneke C, Del Negro LA (2008) Measurement of the mixing state, mass, and optical size of individual black carbon particles in urban and biomass burning emissions. Geophys Res Lett 35(13):L13810. https://doi.org/10.1029/2008GL033968
Sharma SK, Mandal TK, Sharma C, Kuniyal JC, Joshi R, Dhyani PP, Rohtash SA, Ghayas H, Gupta NC, Sharma P, Saxena M, Sharma A, Arya BC, Kumar A (2014) Measurements of particulate (PM2.5), BC and trace gases over the Northwestern Himalayan region of India. Mapan 29(4):243–253. https://doi.org/10.1007/s12647-014-0104-2
Singh A, Rastogi N, Patel A, Satish RV, Singh D (2016) Size-segregated characteristics of carbonaceous aerosols over the northwestern Indo-Gangetic plain: year round temporal behavior. Aerosol Air Qual Res 16(7):1615–1624. https://doi.org/10.4209/aaqr.2016.01.0023
Srivastava AK, Bisht DS, Ram K, Tiwari S, Srivastava MK (2014) Characterization of carbonaceous aerosols over Delhi in Ganga basin: seasonal variability and possible sources. Environ Sci Pollut Res Int 21(14):8610–8619. https://doi.org/10.1007/s11356-014-2660-y
Sudheer AK, Aslam MY, Upadhyay M, Rengarajan R, Bhushan R, Rathore JS, Singh SK, Kumar S (2016) Carbonaceous aerosol over semi-arid region of western India: heterogeneity in sources and characteristics. Atmos Res 178-179:268–278. https://doi.org/10.1016/j.atmosres.2016.03.026
Tandon A, Yadav S, Attri AK (2013) Non-linear analysis of short term variations in ambient visibility. Atmos Pollut Res 4(2):199–207. https://doi.org/10.5094/APR.2013.020
Turpin BJ, Huntzicker JJ (1991): Secondary formation of organic aerosol in the Los Angeles Basin: a descriptive analysis of organic and elemental carbon concentrations. Atmospheric Environment. Part . General Topics 25, 207–215, 2, DOI: https://doi.org/10.1016/0960-1686(91)90291-E
Turpin BJ, Huntzicker JJ (1995) Identification of secondary organic aerosol episodes and quantitation of primary and secondary organic aerosol concentrations during SCAQS. Atmos Environ 29(23):3527–3544. https://doi.org/10.1016/1352-2310(94)00276-Q
Villalobos AM, Amonov MO, Shafer MM, Devi JJ, Gupta T, Tripathi SN, Rana KS, Mckenzie M, Bergin MH, Schauer JJ (2015) Source apportionment of carbonaceous fine particulate matter (PM 2.5) in two contrasting cities across the Indo–Gangetic Plain. Atmos Pollut Res 6(3):398–405. https://doi.org/10.5094/APR.2015.044
Wang H, Kawamura K, Shooter D (2005) Carbonaceous and ionic components in wintertime atmospheric aerosols from two New Zealand cities: implications for solid fuel combustion. Atmos Environ 39(32):5865–5875. https://doi.org/10.1016/j.atmosenv.2005.06.031
Yadav S, Tandon A, Attri AK (2013) Characterization of aerosol associated non-polar organic compounds using TD-GC-MS: a four year study from Delhi, India. J Hazard Mater 252-253:29–44. https://doi.org/10.1016/j.jhazmat.2013.02.024
Yadav S, Tandon A, Attri AK (2014) Timeline trend profile and seasonal variations in nicotine present in ambient PM 10 samples: a four year investigation from Delhi region, India. Atmos Environ 98:89–97. https://doi.org/10.1016/j.atmosenv.2014.08.058
Acknowledgements
Authors extend their sincere acknowledgements to National Oceanic and Atmospheric Administration and Indian Meteorological Department for providing meteorological datasets. Kind support of Managing Director, Kangra Cooperative Bank, Dharamshala, is duly appreciated for providing logistic support for sampling at Dharamshala. Deepika Kaushal is grateful to University Grants Commission (UGC), India, for providing Non-NET fellowship to PhD students. Shweta Yadav acknowledges UGC, India, for financial support provided by UGC, in the form of major research project no. MRP-MAJOR-ENVI-2013-30069 vide file no. 43-332/2014. Acknowledgements to all the anonymous reviewers for their critical comments that improved the quality of this manuscript.
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Kaushal, D., Kumar, A., Yadav, S. et al. Wintertime carbonaceous aerosols over Dhauladhar region of North-Western Himalayas. Environ Sci Pollut Res 25, 8044–8056 (2018). https://doi.org/10.1007/s11356-017-1060-5
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DOI: https://doi.org/10.1007/s11356-017-1060-5