Pollution characteristics and ecological risks of trace elements in PM2.5 over three COALESCE network sites - Bhopal, Mesra, and Mysuru, India.

Time-synchronized, 24 h integrated PM2.5 trace element (TE) measurements made as a part of the COALESCE project (Venkataraman et al., 2020) at Bhopal, Mesra, and Mysore during all of 2019 were analyzed in this study. The concentrations of 15 key elements ranged between 0.05 ng m-3 and 50 µg m-3 across the study sites. Pronounced seasonal variation of elements from multiple source classes showed that the crustal origin elements (Al, Si, Fe, Ti, and Ca) peaked during the pre-monsoon season, while the anthropogenic activities driven element (P, S, K, V, Mn, Cu, Zn, and Pb) concentrations increased during the winter and post-monsoon seasons. Spearman correlation coupled with hierarchical clustering separated the matrix of elements into three common clusters at all sites, corresponding to crustal sources, combustion and biomass burning emissions, and industrial/non-exhaust vehicular emissions, respectively. Furthermore, episodes of metal pollution throughout the year were examined using characteristic radar charts of TEs to identify the association between TE sources and poor air quality. For example, maximum metal pollution in Bhopal occurred during the post-monsoon season, attributable to biomass burning, dust storms, industrial and non-exhaust vehicular emissions. Finally, an ecological risk assessment revealed that the risk index was higher than the threshold value of 600 for all heavy metals at all sites. Pb, Cu, and Zn were the top contributors to 'extremely high risk' amongst all heavy metals. Overall, the results show that although TE concentrations at all three locations were much lower than in other urban locations in India, the risk from heavy metals to the ecosystem (and likely to human health) cannot be ignored. The findings warrant a full source apportionment of fine PM to better identify TE-rich source contributions and future studies to examine the atmospheric processing and eco-system uptake of TEs.

Tracing the predominant sources of carbon in PM2.5 using δ13C values together with OC/EC and select inorganic ions over two COALESCE locations.

As part of the COALESCE (Carbonaceous Aerosol Emissions, Source apportionment and Climate Impacts) campaign, ambient PM2.5 was collected at two regional sites (Bhopal and Mysuru) in India during 2019. We utilized organic carbon (OC), elemental carbon (EC) and water-soluble inorganic ions together with δ13C values, to better understand total carbon (TC) sources at these locations. The annual average δ13C values (-26.2 ± 0.6‰) at Mysuru and Bhopal (-26.6 ± 0.6‰) were comparable. However, at Mysuru, except during winter, day-to-day variability was much lower (narrow range of -26.8 to -26.0‰) than that at Bhopal (range: -28.1 to -24.7‰), suggesting that TC was contributed by few sources, likely dominated by vehicular emissions. Seasonal average δ13C values at Bhopal increased slightly (-25.8 ± 0.5‰) during the winter (Jan-Feb) and decreased (-27.0 ± 0.3‰) during the monsoon (Jun-Sep) season compared to the annual average. The decrease in δ13C values during the monsoon season was likely driven by enhanced secondary organic aerosol formation. Further, based on MODIS derived fire spots and back trajectories, we infered that the δ13C values (-27.5 to -26.0‰) in Bhopal during the post-monsoon season (Oct-Dec) were indicative of dominant biomass burning contributions. The inorganic ions/TC ratio during this season suggested that biomass burning aerosol was aged and may have been transported from crop residue burning in the Indo-Gangetic plains. At Mysuru, like the trend at Bhopal, the δ13C values during the monsoon season were lower than those during the winter season. Finally, δ13C values were input to a Bayesian model-MixSIAR to demonstrate the usefulness of such models in apportioning TC. In its simplest implementation, the model separated TC sources into fossil fuel emissions and non-fossil fuel sources . Fossil fuel combustion emissions accounted for 47 ± 19% and 62 ± 22% of the TC at Bhopal and Mysuru, respectively.