Comprehensive source identification of heavy metals in atmospheric particulate matter in a megacity: A case study of Hangzhou.

Megacities face significant pollution challenges, particularly the elevated levels of heavy metals (HMs) in particulate matter (PM). Despite the advent of interdisciplinary and advanced methods for HM source analysis, integrating and applying these approaches to identify HM sources in PM remains a hurdle. This study employs a year-long daily sampling dataset for PM1 and PM1-10 to examine the patterns of HM concentrations under hazy, clean, and rainy conditions in Hangzhou City, aiming to pinpoint the primary sources of HMs in PM. Contrary to other HMs that remained within acceptable limits, the annual average concentrations of Cd and Ni were found to be 20.6 ± 13.6 and 46.9 ± 34.8 ng/m³, respectively, surpassing the World Health Organization's limits by 4.1 and 1.9 times. Remarkably, Cd levels decreased on hazy days, whereas Ni levels were observed to rise on rainy days. Using principal component analysis (PCA), enrichment factor (EF), and backward trajectory analysis, Fe, Mn, Cu, and Zn were determined to be primarily derived from traffic emissions, and there was an interaction between remote migration and local emissions in haze weather. Isotope analysis reveals that Pb concentrations in the Hangzhou region were primarily influenced by emissions from unleaded gasoline, coal combustion, and municipal solid waste incineration, with additional impact from long-range transport; it also highlights nuanced differences between PM1 and PM1-10. Pb isotope and PCA analyses indicate that Ni primarily stemmed from waste incineration emissions. This explanation accounts for the observed higher Ni concentrations on rainy days. Backward trajectory cluster analysis revealed that southern airflows were the primary source of high Cd concentrations on clean days in Hangzhou City. This study employs a multifaceted approach and cross-validation to successfully delineate the sources of HMs in Hangzhou's PM. It offers a methodology for the precise and reliable analysis of complex HM sources in megacity PM.

Compounds of wastewater origin in remote upland lakes in Ireland.

It is well established that persistent organic pollutants are transported long distances in the atmosphere and deposited into aquatic and terrestrial ecosystems in remote areas, including high altitude lakes. The objective of this research was to evaluate whether compounds of wastewater origin were present in four remote upland headwater lakes in Ireland that primarily receive loadings from atmospheric deposition. Using Polar Organic Chemical Integrative Samplers (POCIS) deployed in the lakes for 60 to 68 days, seven compounds were detected at levels that could be quantified but 25 of the target compounds were not detected. The detected compounds included the cannabinoid metabolite, tetrahydrocannabinol carboxylate (THC-COOH), codeine, acetaminophen (paracetamol), ibuprofen, and the artificial sweeteners, sucralose, and saccharin, which were all present at concentrations estimated to be < 125 ng/L. Caffeine was also present in the lakes at estimated concentrations between 213 and 1320 ng/L. Cocaine and tramadol were detected in POCIS deployed in some of the lakes, but at levels below the limits of quantitation. The highest concentrations of the target analytes were detected in two lakes located in the eastern part of Ireland. These data are consistent with regional atmospheric transport of these compounds originating from wastewater treatment plants in Ireland. However, contaminants from wastewater treatment plants in the United Kingdom may also be a source in these upland lakes that are located far from emissions of urban pollution.

Seven-year study of monsoonal rainwater chemistry over the mid-Brahmaputra plain, India: assessment of trends and source regions of soluble ions.

This work is a 7-year study of monsoonal rainwater chemistry (n = 302), over mid-Brahmaputra plain during 2012 to 2018. The samples were analyzed for major chemical parameters viz. pH, electrical conductivity (EC), and ions (SO42-, NO3-, Br-, Cl-, F-, Mg2+, Ca2+, K+, NH4+, Na+, and Li+) to assess the chemistry. The mean pH of rainwater varied among the years, which was maximum in 2018 (6.18 ± 0.72) and minimum in the year 2014 (5.39 ± 0.54), and the variations were significant at p < 0.0001. Ridgeline plots were drawn to visualize interannual variations, which revealed that Ca2+ was the dominant cation in the early years, whereas NH4+ prevailed in the latter years. Mann-Kendall analysis and Sen's slope statistical tests were employed, and it was found that all the ions showed positive S values indicating increasing trends. Enrichment factors (EF) of K+, SO42-, and NO3- were found to be high with respect to both soil and seawater suggesting the influence of emissions from fossil fuel and biomass burning in the chemistry of rainwater. Principal component analysis (PCA) was applied to identify the sources of rain constituents, and five factors were obtained explaining crustal dust, biomass burning, fossil fuel combustion, agricultural emissions, and coal burning as possible sources. Airmass back trajectory clusters and Potential Source Contribution Function (PSCF) were computed by application of HYbrid Single-Particle Lagrangian Integrated Trajectory model to appreciate the terrestrial influence on the chemistry. The results indicated inputs from both local and regional dust and anthropogenic constituents that influenced the monsoonal rainwater chemistry over Brahmaputra Valley.

Levels, Sources and Toxicity Risks of Polycyclic Aromatic Hydrocarbons at an Island Site in the Gulf of Tonkin.

The varying concentrations of polycyclic aromatic hydrocarbons (PAHs) at remote islands is an important indicator, demonstrating the contributions from different regional combustion sources. In this study, gaseous and particulate PAHs were measured at Weizhou Island in the Gulf of Tonkin from 15th March to 14th April, 2015. The concentrations of PAHs ranged from 116.22 to 186.74 ng/m3 and from 40.19 to 61.86 ng/m3 in gas and particulate phase, respectively, which were much higher than those of some remote sites in Asia. Phenanthrene, fluoranthene, pyrene, and chrysene, which were mainly found in diesel vehicle emissions, had relatively high concentrations in both gas and particulate phases. According to the comprehensive results of back trajectory cluster analysis and diagnostic ratios, the local vessel emission was probably the main source of PAHs, which was much more important than the coal and biomass combustion sources from remoter regions. The toxicities represented by ∑PAH7, benzo(a)pyrene-equivalent carcinogenic power, and 2,3,7,8-tetrachlorodibenzo-p-dioxin-based total toxicity potency are much higher in particulate phase than those in gas phase. However, the toxicities of gas phase should not be neglected from the point of view of indirect-acting mutagenicities due to the high contribution of fluoranthene.

Source apportionment and seasonal variation in particulate PAHs levels at a coastal site in Belgium.

In the present study, estimation of the atmospheric polycyclic aromatic hydrocarbons (PAHs) was done in particulate samples collected from De Haan, Belgium, during different seasons. The sampling site was situated very close to the north sea and far from the influence of local or industrial activities. The levels of PAHs depicted a distinct seasonal trend, being highest during the spring season. The observations of the study indicated a mean value of 2.6 ng m-3 for concentration of all the 16 US EPA PAHs, thus being significantly lower when compared to results of previous studies focused on other sites. The dominating PAHs species reported were naphthalene, fluoranthene, benzo[a]anthracene, chrysene, and indeno[1,2,3c,d] pyrene. Assessment of the seasonal variation of the PAH levels was also done with respect to diagnostic ratio-based source identification, analysis of back trajectories, and principle component analysis. Burning of fossil fuels was observed to be the prominent source of atmospheric PAHs in the study area. Further, lifetime cancer risk assessment was performed to assess the detrimental health impacts on humans on being exposed to atmospheric PAHs. Particulate PAHs present in the ambient air of Belgium shows no carcinogenic health impacts. However, considering the industrial expansion in the region, efforts are required to prevent the environmental contamination of PAHs. Graphical abstract.

Chemical characteristics and source apportionment of PM2.5 between heavily polluted days and other days in Zhengzhou, China.

PM2.5 samples were collected in Zhengzhou during 3years of observation, and chemical characteristics and source contribution were analyzed. Approximately 96% of the daily PM2.5 concentrations and annual average values exceeded the Chinese National Ambient Air Quality Daily and Annual Standards, indicating serious PM2.5 pollution. The average concentration of water-soluble inorganic ions was 2.4 times higher in heavily polluted days (daily PM2.5 concentrations>250µg/m3 and visibility <3km) than that in other days, with sulfate, nitrate, and ammonium as major ions. According to the ratio of NO3-/SO42-, stationary sources are still the dominant source of PM2.5 and vehicle emission could not be ignored. The ratio of secondary organic carbon to organic carbon indicated that photochemical reactivity in heavily polluted days was more intense than in other days. Crustal elements were the most abundant elements, accounting for more than 60% of 23 elements. Chemical Mass Balance results indicated that the contributions of major sources (i.e., nitrate, sulfate, biomass, carbon and refractory material, coal combustion, soil dust, vehicle, and industry) of PM2.5 were 13%, 16%, 12%, 2%, 14%, 8%, 7%, and 8% in heavily polluted days and 20%, 18%, 9%, 2%, 27%, 14%, 15%, and 9% in other days, respectively. Extensive combustion activities were the main sources of polycyclic aromatic hydrocarbons during the episode (Jan 1-9, 2015) and the total benzo[a]pyrene equivalency concentrations in heavily polluted days present significant health threat. Because of the effect of regional transport, the pollution level of PM2.5 in the study area was aggravated.

Source regions of ragweed pollen arriving in south-western Poland and the influence of meteorological data on the HYSPLIT model results.

We have investigated the relationship between the inflow of air masses and the ragweed pollen concentration in SW Poland (Wroclaw) for a 10-year period of 2005-2014. The HYSPLIT trajectory model was used to verify whether episodes of high concentrations can be related to regions outside of the main known ragweed centres in Europe, like Pannonian Plain, northern Italy and Ukraine. Furthermore, we used two different meteorological data sets (the global GDAS data set and from the WRF mesoscale model; the meteorological parameters were: U and V wind components, temperature and relative humidity) into HYSPLIT to evaluate the influence of meteorological input on calculated trajectories for high concentration ragweed episodes. The results show that the episodes of high pollen concentration (above 20 pm-3) represent a great part of total recorded ragweed pollen in Wroclaw, but occur rarely and not in all years. High pollen episodes are connected with air masses coming from south and south-west Europe, which confirms the existence of expected ragweed centres but showed that other centres near Wroclaw are not present. The HYSPLIT simulations with two different meteorological inputs indicated that footprint studies on ragweed benefit from a higher resolution meteorological data sets.

The long-range transport of Pinaceae pollen: an example in Kraków (southern Poland).

High Pinaceae pollen concentrations in the air and on the surface of puddles before the main pollen season started were observed in Kraków (southern Poland) in May 2013. The paper presents the results of detailed studies of the composition and source of the "yellow rain" in 2013, and as a comparison, the Pinaceae pollen concentrations and samples collected from the ground surface in 2014 were considered. The air samples were collected using the volumetric method (Hirst-type device), while pollen grains sampled from the ground surface were processed using a modified Erdtman acetolysis method. Finally, all samples were studied using a light microscope. In 2013, the period of higher Abies, Picea and Pinus pollen concentrations was observed from the 5 to 12 of May, earlier than the main pollen season occurred. The presence of rainfall on the 12 and 13 of May 2013 caused the pollen deposition on the ground surface, where the prevalence of Pinaceae pollen was found. The synoptic situation and the analysis of the back-trajectories and air mass advection at the beginning of May 2013 indicated that Pinaceae pollen grains could have been transported from Ukraine, Romania, Hungary and Slovakia. In contrast, Pinaceae pollen grains deposited on the ground surface as a "yellow" film in May 2014, originated from local sources.

Airborne Quercus pollen in SW Spain: Identifying favourable conditions for atmospheric transport and potential source areas.

The pollen grains of Quercus spp. (oak trees) are allergenic. This study investigates airborne Quercus pollen in SW Spain with the aim identifying favourable conditions for atmospheric transport and potential sources areas. Two types of Quercus distribution maps were produced. Airborne Quercus pollen concentrations were measured at three sites located in the Extremadura region (SW Spain) for 3 consecutive years. The seasonal occurrence of Quercus pollen in the air was investigated, as well as days with pollen concentrations ≥80Pm(-3). The distance that Quercus pollen can be transported in appreciable numbers was calculated using clusters of back trajectories representing the air mass movement above the source areas (oak woodlands), and by using a state-of-the-art dispersion model. The two main potential sources of Quercus airborne pollen captured in SW Spain are Q. ilex subsp. ballota and Q. suber. The minimum distances between aerobiological stations and Quercus woodlands have been estimated as: 40km (Plasencia), 66km (Don Benito), 62km (Zafra) from the context of this study. Daily mean Quercus pollen concentration can exceed 1,700Pm(-3), levels reached not less than 24 days in a single year. High Quercus pollen concentration were mostly associated with moderate wind speed events (6-10ms(-1)), whereas that a high wind speed (16-20ms(-1)) seems to be associated with low concentrations.

The long distance transport of airborne Ambrosia pollen to the UK and the Netherlands from Central and south Europe.

The invasive alien species Ambrosia artemisiifolia (common or short ragweed) is increasing its range in Europe. In the UK and the Netherlands, airborne concentrations of Ambrosia pollen are usually low. However, more than 30 Ambrosia pollen grains per cubic metre of air (above the level capable to trigger allergic symptoms) were recorded in Leicester (UK) and Leiden (NL) on 4 and 5 September 2014. The aims of this study were to determine whether the highly allergenic Ambrosia pollen recorded during the episode could be the result of long distance transport, to identify the potential sources of these pollen grains and to describe the conditions that facilitated this possible long distance transport. Airborne Ambrosia pollen data were collected at 10 sites in Europe. Back trajectory and atmospheric dispersion calculations were performed using HYSPLIT_4. Back trajectories calculated at Leicester and Leiden show that higher altitude air masses (1500 m) originated from source areas on the Pannonian Plain and Ukraine. During the episode, air masses veered to the west and passed over the Rhône Valley. Dispersion calculations showed that the atmospheric conditions were suitable for Ambrosia pollen released from the Pannonian Plain and the Rhône Valley to reach the higher levels and enter the airstream moving to northwest Europe where they were deposited at ground level and recorded by monitoring sites. The study indicates that the Ambrosia pollen grains recorded during the episode in Leicester and Leiden were probably not produced by local sources but transported long distances from potential source regions in east Europe, i.e. the Pannonian Plain and Ukraine, as well as the Rhône Valley in France.

Potential sources of airborne Alternaria spp. spores in South-west Spain.

Fungi belonging to the genus of Alternaria are recognised as being significant plant pathogens, and Alternaria allergens are one of the most important causes of respiratory allergic diseases in Europe. This study aims to provide a detailed and original analysis of Alternaria transport dynamics in Badajoz, SW Spain. This was achieved by examining daily mean and hourly observations of airborne Alternaria spores recorded during days with high airborne concentrations of Alternaria spores (>100 s m(-3)) from 2009 to 2011, as well as four inventory maps of major Alternaria habitats, the overall synoptic weather situation and analysis of air mass transport using Hybrid Single Particle Lagrangian Integrated Trajectory model and geographic information systems. Land use calculated within a radius of 100 km from Badajoz shows that crops and grasslands are potentially the most important local sources of airborne Alternaria spores recorded at the site. The results of back trajectory analysis show that, during the examined four episodes, the two main directions where Alternaria source areas were located were: (1) SW-W; and (2) NW-NE. Regional scale and long distance transport could therefore supplement the airborne catch recorded at Badajoz with Alternaria conidia originating from sources such as crops and orchards situated in other parts of the Iberian Peninsula.

Characterisation of atmospheric deposited particles during a dust storm in urban areas of Eastern Australia.

The characteristics of dust particles deposited during the 2009 dust storm in the Gold Coast and Brisbane regions of Australia are discussed in this paper. The study outcomes provide important knowledge in relation to the potential impacts of dust storm related pollution on ecosystem health in the context that the frequency of dust storms is predicted to increase due to anthropogenic desert surface modifications and climate change impacts. The investigated dust storm contributed a large fraction of fine particles to the environment with an increased amount of total suspended solids, compared to dry deposition under ambient conditions. Although the dust storm passed over forested areas, the organic carbon content in the dust was relatively low. The primary metals present in the dust storm deposition were aluminium, iron and manganese, which are common soil minerals in Australia. The dust storm deposition did not contain significant loads of nickel, cadmium, copper and lead, which are commonly present in the urban environment. Furthermore, the comparison between the ambient and dust storm chromium and zinc loads suggested that these metals were contributed to the dust storm by local anthropogenic sources. The potential ecosystem health impacts of the 2009 dust storm include, increased fine solids deposition on ground surfaces resulting in an enhanced capacity to adsorb toxic pollutants as well as increased aluminium, iron and manganese loads. In contrast, the ecosystem health impacts related to organic carbon and other metals from dust storm atmospheric deposition are not considered to be significant.