A year-long study on PM2.5 and its carbonaceous components over eastern Himalaya in India: Contributions of local and transported fossil fuel and biomass burning during premonsoon.

A year-long (March 2019-February 2020) study on the characterization of fine mode carbonaceous aerosols has been conducted over a high altitude urban atmosphere, Darjeeling (27.01°N, 88.15°E, 2200 m asl) in eastern Himalaya. The fine mode aerosol (PM2.5; 41.7 ± 23.7 µgm-3), total carbonaceous aerosols (TCA; 19.8 ± 7.7 µgm-3), organic carbon (OC; 8.0 ± 3.9 µgm-3) and elemental carbon (EC; 2.0 ± 0.9 µgm-3) exhibited similar seasonal variability with the highest abundance during winter followed by premonsoon, postmonsoon and minimum in monsoon. The OC:EC varied over a range of 2.8-19.4 whereas the secondary organic carbon ranged between 1.9 and 17.1 µgm-3 respectively. Higher PM2.5 associated with higher winds and elevated mixing layer depth suggest a strong influence of regional and long-range transport. In addition to the usual morning and evening rush-hour peaks, the impact of low land plain regions driven by up-slope valley winds was observed for the carbonaceous components. A novel approach has been taken to find out the individual contributions from the local and transported fossil fuel, biomass burning, and biogenic sources to OC and EC during premonsoon. We observed that the local fossil fuel (43%) contributions dominated over the biomass burning (39%) for EC whereas the contributions of local biomass burning and the local fossil fuel were same (46%) for OC. EC exhibited a higher contribution (18%) from the regional/long-range transport compared to OC (8%). IGP and Nepal were found to be the maximum contributing long distant source regions for the carbonaceous aerosol loading over eastern Himalaya. Such individual source apportionment of carbonaceous aerosols over eastern Himalaya makes the study unique and first-ever of its kind and immensely helpful for building robust mitigation action plans.

High rise in carbonaceous aerosols under very low anthropogenic emissions over eastern Himalaya, India: Impact of lockdown for COVID-19 outbreak.

The present study has been conducted to investigate the relative changes of carbonaceous aerosols (CA) over a high altitude Himalayan atmosphere with and without (very low) anthropogenic emissions. Measurements of atmospheric organic (OC) and elemental carbon (EC) were conducted during the lockdown period (April 2020) due to global COVID 19 outbreak and compared with the normal period (April 2019). The interesting, unexpected and surprising observation is that OC, EC and the total CA (TCA) during the lockdown (OC: 12.1 ± 5.5 µg m-3; EC: 2.2 ± 1.1 µg m-3; TCA: 21.5 ± 10 µg m-3) were higher than the normal period (OC: 7.04 ± 2.2 µg m-3; EC: 1.9 ± 0.7 µg m-3; TCA: 13.2 ± 4.1 µg m-3). The higher values for OC/EC ratio too was observed during the lockdown (5.7 ± 0.9) compared to the normal period (4.2 ± 1.1). Much higher surface O3 during the lockdown (due to very low NO) could better promote the formation of secondary OC (SOC) through the photochemical oxidation of biogenic volatile organic compounds (BVOCs) emitted from Himalayan coniferous forest cover. SOC during the lockdown (7.6 ± 3.5 µg m-3) was double of that in normal period (3.8 ± 1.4 µg m-3). Regression analysis between SOC and O3 showed that with the same amount of increase in O3, the SOC formation increased to a larger extent when anthropogenic emissions were very low and biogenic emissions dominate (lockdown) compared to when anthropogenic emissions were high (normal). Concentration weighted trajectory (CWT) analysis showed that the anthropogenic activities over Nepal and forest fire over north-east India were the major long-distant sources of the CA over Darjeeling during the normal period. On the other hand, during lockdown, the major source regions of CA over Darjeeling were regional/local. The findings of the study indicate the immense importance of Himalayan biosphere as a major source of organic carbon.

Acidity and oxidative potential of atmospheric aerosols over a remote mangrove ecosystem during the advection of anthropogenic plumes.

To investigate the acidity and the water-soluble oxidative potential of PM10, during the continental biomass-burning plume transport, a three-year (2018-2020) winter-time campaign was conducted over a pristine island (21.35°N, 88.32°E) of Sundarban mangrove ecosystem situated at the shore of Bay of Bengal. The average PM10 concentration over Sundarban was found to be 98.3 ± 22.2 µg m-3 for the entire study period with a high fraction of non-sea-salt- SO42- and water-soluble organic carbons (WSOC) that originated from the regional solid fuel burning. The thermodynamic E-AIM(IV) model had estimated that the winter-time aerosols over Sundarban were acidic (pH:2.4 ± 0.6) and mainly governed by non-sea-salt-SO42-. The volume and mass normalized oxidative potential of PM10 was found to be 1.81 ± 0.40 nmol DTT min-1 m-3 and 18.4 ± 6.1 pmol DTT min-1 µg-1 respectively which are surprisingly higher than several urban atmospheres across the world including IGP. The acid-digested water-soluble transition metals (Cu, Mn) show higher influences in the oxidative potential (under high aerosol acidity) compared to the WSOC. The study revealed that the advection of regional solid fuel burning plume and associated non-sea-salt-SO42- is enhancing aerosol acidity and oxidative stress that in turn alters the intrinsic properties of aerosols over such marine ecosystems rich in ecology and bio-geochemistry.

A district-level emission inventory of anthropogenic PM2.5 from the primary sources over the Indian Indo Gangetic Plain: Identification of the emission hotspots.

A district-wise emission inventory was made for the states and union territories (UTs) of the Indian Indo-Gangetic Plain for the base year of 2018 to estimate the emissions of PM2.5 from various sectors. In addition to conventional sectors, emissions from road dust, fossil-fuelled irrigation pumps, and construction dust were also taken into account. Total primary anthropogenic PM2.5 emission was estimated to be 3157.3 Gg (or kilo-tones) for the year 2018 of which 32 % originated from the industrial sector, 27 % from domestic fuel consumption, 23 % from open burning, 14 % from road dust, 2 % from vehicular and 2 % from various unorganized sectors. The highest emissions were observed during the premonsoon (1013 Gg/year) followed by postmonsoon (802Gg/year), winter (788 Gg/year), and lowest during the monsoon (554Gg/year). Among the states and UTs, Uttar Pradesh contributes the most in total emissions (39 %), followed by Punjab (19 %), Bihar (17 %), West Bengal (13 %), Haryana (11 %), Delhi (0.9 %) and Chandigarh (0.1 %). Emission for per capita and for billion-rupee of state gross domestic product (GDP) were the highest for Punjab and Haryana. Results have identified the districts of Punjab (Firozpur, Ludhiana, Jalandhar), scattered pockets of Uttar Pradesh (Sonbhadra, Agra, Varanasi, Kanpur, Lucknow, Prayagraj) and lower Gangetic delta (Gaya, Muzaffarpur, Burdwan, both 24-parganas and Murshidabad) as potent hotspots of cumulative PM2.5 emissions. On the other hand, the districts of Punjab (Faridkot, Mansa, Muktsar, Fatehgarh) were found to be the hotspots for per capita emissions. High emissions were observed from the domestic sector, brick kilns, and micro and small-scale industries, and regulating norms should be more stringent for these sectors. Such a study will be a value add for the policymakers and health experts to assess emission hot spots, pollution simulation, and associated mortality analysis of the region.

Identification of sources of coarse mode aerosol particles (PM10) using ATR-FTIR and SEM-EDX spectroscopy over the Himalayan Region of India.

This study attempts to examine the morphological, elemental and physical characteristics of PM10 over the Indian Himalayan Region (IHR) using FTIR and scanning electron microscopy-energy dispersive X-ray (SEM-EDX) analysis. The study aimed at source identification of PM10 by exploring the inorganic ions, organic functional groups, morphology and elemental characteristics. The pollution load of PM10 was estimated as 63 ± 22 µg m-3; 53 ± 16 µg m-3; 67 ± 26 µg m-3 and 55 ± 11 µg m-3 over Mohal-Kullu, Almora, Nainital and Darjeeling, respectively. ATR-FTIR spectrum analysis revealed the existence of inorganic ions (SiO44-, TiO2, SO42-, SO3-, NO3-, NO2-, CO32-, HCO3-, NH4+) and organic functional groups (C-C, C-H, C=C, C≡C, C=O, N-H, C≡N, C=N, O-H, cyclic rings, aromatic compounds and some heterogeneous groups) in PM10 which may arise from geogenic, biogenic and anthropogenic sources. The morphological and elemental characterization was performed by SEM-EDX, inferring for geogenic origin (Al, Na, K, Ca, Mg and Fe) due to the presence of different morphologies (irregular, spherical, cluster, sheet-like solid deposition and columnar). In contrast, particles having biogenic and anthropogenic origins (K, S and Ba) have primarily spherical with few irregular particles at all the study sites. Also, the statistical analysis ANOVA depicts that among all the detected elements, Na, Al, Si, S and K are site-specific in nature as their mean of aw% significantly varied for all the sites. The trajectory analysis revealed that the Uttarakhand, Jammu and Kashmir, the Thar Desert, Himachal Pradesh, Pakistan, Afghanistan, Nepal, Sikkim, the Indo-Gangetic Plain (IGP) and the Bay of Bengal (BoB) contribute to the increased loading of atmospheric pollutants in various locations within the IHR.

PM2.5 pollution exceeding Indian standard over a semi-urban region at eastern IGP: Chemistry, meteorological impact, and long-range transport.

A year-long study (January-December 2019) on the chemical characterization and meteorological impact on PM2.5 was conducted over a semi-urban station, Shyamnagar, in the easternmost part of the Indo-Gangetic Plains (IGP). PM2.5 concentrations (Mean = 81.69 ± 66.27 µgm-3; 7.10-272.74 µgm-3), the total carbonaceous aerosols (TCA) (Mean = 22.85 ± 24.95 µgm-3; 0.77-102.97 µgm-3) along with differential carbonaceous components like organic carbon (OC) (Mean = 11.28 ± 12.48 µgm-3; 0.48-53.01 µgm-3) and elemental carbon (EC) (Mean = 4.83 ± 5.28 µgm-3; 0.1-22.13 µgm-3) exhibited prominent seasonal variability with the highest concentrations during winter, followed by post-monsoon, pre-monsoon and lowest during monsoon. A similar seasonal variation was observed for the total water-soluble ionic species (Mean = 31.91 ± 20.12 µgm-3; 0.1-126.73 µgm-3). We observed that under the least favorable conditions (low ventilation coefficient), high PM2.5 pollution (exceeding Indian standard) was associated with a high increase in secondary components of PM2.5. Eastern, central and western parts of IGP, as well as Nepal, were the major long-distant source regions whereas the northern part of West Bengal and parts of Bangladesh were the major regional source region for high PM2.5 pollution over Shyamnagar. The ratios like char-EC/soot-EC, non-sea-K+/EC and non-sea-SO42-/EC strongly indicated the dominance of fossil fuel burning over biomass burning. Compared with other studies, we observed that the PM2.5 pollution over this semi-urban region was comparable (and even higher in some cases) with other parts of IGP. The high exceedance of PM2.5 over the Indian standard in Shyamnagar strongly demands an immediate initiation of systematic and regular based air pollution monitoring over semi-urban/non-urban regions in India, especially IGP, in addition to the polluted cities.

Relative role of black carbon and sea-salt aerosols as cloud condensation nuclei over a high altitude urban atmosphere in eastern Himalaya.

The present study is an attempt to investigate the relative role of black carbon (BC) and sea-salt aerosols on the CCN activation over a high altitude station, Darjeeling (27.1° N and 88.15° E, 2200 m asl) at eastern Himalaya. Aerosols (CN, CCN, BC and PM2.5) were measured during premonsoon and monsoon in 2017 and 2018. A unique sampling strategy and a novel methodology were adopted that enabled us to quantitatively and separately determine the contributions of local emissions (LE), valley wind transport (VWT) and long-range transport (LRT) to BC aerosols and their role in CCN activation. On the other hand, the contributions of transported sea-salt (NaCl) aerosols to CCN activation were also determined when they interact with the local anthropogenic soluble species and when they do not. CCN (0.5% super-saturation) concentrations were found to be increased when BC aerosols were more aged (~ 80 cm-3 and 218 cm-3 increase in CCN for 1 µg m-3 increase in BCLE and BCLRT with activation ratios of 0.17 and 0.55 respectively). Local anthropogenic acidic species (SO42-/H2SO4 (g) and NO3-/HNO3 (g)) interact with NaCl resulting to Cl- depletion. Cl- depletion was increased with the increase in NO3- + SO42-(45% for1 µg m-3increase in NO3- + SO42-) that in turn sharply decreased the AR of NaCl (0.04 for 1% increase in Cl- depletion). On the other hand, higher the NO3- + SO42-, higher were the CCN activation of transported BC which could be due to the soluble coating on BC. The important and interesting fact is that when transported and interacted with anthropogenic soluble species, BC aerosols (though hydrophobic) act as much better CCN than NaCl (though hydrophilic).