The contributions of contaminant sources are difficult to resolve in the sediment record using concentration gradients and flux reconstruction alone. In this study, we demonstrate that source partitioning using lead isotopes provide complementary and unique information to concentration gradients to evaluate point-source releases, transport, and recovery of metal mining pollution in the environment. We analyzed eight sediment cores, collected within 24 km of two gold mines, for Pb stable isotopes, Pb concentration, and sediment chronology. Stable Pb isotope ratios (²⁰⁶Pb/²⁰⁷Pb, ²⁰⁸Pb/²⁰⁴Pb) of mining ore were different from those of background (pre-disturbance) sediment, allowing the use of a quantitative mixing model. As previously reported for some Arctic lakes, Pb isotope ratios indicated negligible aerosol inputs to sediment from regional or long-range pollution sources, possibly related to low annual precipitation. Maximum recorded Pb flux at each site reached up to 63 mg m⁻² yr⁻¹ in the period corresponding to early years of mining when pollution mitigation measures were at a minimum (1950s–1960s). The maximum contribution of mining-derived Pb to these fluxes declined with distance from the mines from 92 ± 8% to 8 ± 4% at the farthest site. Mining-derived Pb was still present at the sediment surface within 9 km of Giant Mine more than ten years after mine closure (5–26 km, 95% confidence interval) and model estimates suggest it could be present for another ∼50–100 years. These results highlight the persistence of Pb pollution in freshwater sediment and the usefulness of Pb stable isotopes to quantify spatial and temporal trends of contamination from mining pollution, particularly as concentrations approach background.

To characterise the mass concentration, size-distribution, and respiratory deposition of selected trace metals (Cr, Mn, Fe, Ni, Cu, Zn, Ba, and Pb) in size-segregated PM₂.₅, a long-term monitoring campaign was undertaken at an urban background site in Como (Northern Italy). 96-h aerosol samples were collected weekly, from May 2015 to March 2016, using a 13-stage low pressure impactor and analysed via laser ablation-inductively coupled plasma-mass spectrometry. Significantly higher levels of trace metals were generally found during the heating season (two to more than four times) compared to the non-heating period at all size ranges, especially for concentrations in PM₀.₁–₁. Distinct distribution profiles characterised the different elements, even though the corresponding heating and non-heating shapes always exhibited similar features, with negligible seasonal shifts in the average mass median aerodynamic diameters. Fe, Ba, and Cu had >70% of their mass in PM₁–₂.₅, whereas Pb, Zn, and Ni showed higher contributions in the accumulation mode (>60%). Finally, broad size-distributions were found for Cr and Mn. The multiple-path particle dosimetry model estimated the overall deposition fractions in human airways varying between 27% (Pb) and 48% (Ba). The greatest deposition variability was always registered in the head region of the respiratory system, with the highest contributions for those metals predominantly accumulated in the PM₂.₅ coarse modes. In contrast, the deposition in the deepest respiratory tract maintained nearly constant proportions over time, becoming notably important for Pb, Ni, and Zn (∼13%) with respect to their total deposition. The comparison with national limits established for Pb and Ni suggested the absence of significant risks for the local population, as expected, with average concentrations two orders of magnitude lower than the corresponding annual limit and objective value. Similar findings were reported for all the other metals, for which the estimated hazard quotients were always well <1.

The new-generation geostationary satellites feature higher radiometric, spectral, and spatial resolutions, thereby making richer data available for the improvement of PM₂.₅ predictions. Various aerosol optical depth (AOD) data assimilation methods have been developed, but the accurate representation of the AOD-PM₂.₅ relationship remains challenging. Empirical statistical methods are effective in retrieving ground-level PM₂.₅, but few have been evaluated in terms of whether and to what extent they can help improve PM₂.₅ predictions. Therefore, an empirical and statistics-based scheme was developed for optimizing the estimation of the initial conditions (ICs) of aerosol in WRF-Chem (Weather Research and Forecasting/Chemistry) and for improving the PM₂.₅ predictions by integrating Himawari-8 data and ground observations. The proposed method was evaluated via two one-year experiments that were conducted in parallel over eastern China. The contribution of the satellite data to the model performance was evaluated via a 2-week control experiment. The results demonstrate that the proposed method improved the PM₂.₅ predictions throughout the year and mitigated the underestimation during pollution episodes. Spatially, the performance was highly correlated with the amount of valid data.

In this study, size-fractionated particulate matters (PM) down to ultrafine (PM₀.₁) particles were collected using a cascade air sampler with a PM₀.₁ stage, in Hat Yai city, Songkhla province, southern Thailand during the year 2018. The particle-bound carbonaceous aerosols (CA) as elemental carbon (EC) and organic carbon (OC) were quantified with the thermal/optical reflectance method following the IMPROVE_TOR protocol. The concentrations of different temperature carbon fractions (OC1-OC4, EC1-EC3 and PyO) in the size-fractionated PM were evaluated to discern OC and EC correlations as well as those between char-EC and soot-EC. The results showed that biomass burning, motor vehicle, and secondary organic aerosols (SOC) all contributed to the size-fractionated PM. The OC/EC ratios ranged from 2.90 to 4.30 over the year, with the ratios of PM₂.₅₋₁₀ being the highest, except during the open biomass burning period. The concentration of CA was found to increase during the pre-monsoon season and had its peak value in the PM₀.₅₋₁.₀ fraction. The long-range transport of PMs from Indonesia, southwest of Thailand toward southern Thailand became more obvious during the pre-monsoon season. Transported plumes from biomass burning in Indonesia may increase the concentration of OC and EC both in the fine (PM₀.₅₋₁.₀ and PM₁.₀₋₂.₅) and coarse (PM₂.₅₋₁₀ and PM>₁₀) fractions. The OC fraction in PM₀.₁ was also shown to be significantly affected by the transported plumes during the pre-monsoon season. Good OC and EC correlations (R² = 0.824–0.915) in the fine particle fractions indicated that they had common sources such as fossil fuel combustion. However, the lower and moderate correlations (R² = 0.093–0.678) among the coarser particles suggesting that they have a more complex pattern of emission sources during the dry and monsoon seasons. This indicates the importance of focusing emission control strategies on different PM particle sizes in southern Thailand.

Oxygenated volatile organic compounds (OVOCs) are critical precursors of atmospheric ozone (O₃) and secondary organic aerosols (SOA). Although China is experiencing increasing O₃ pollution from north to south, understanding the major sources of OVOCs in this region is still limited due to their active photochemical behaviors. In this study, five critical OVOCs at a northern urban site (Beijing) and a southern urban site (Shenzhen) were monitored in summer using proton transfer reaction-mass spectrometry (PTR-MS). The mean total concentration of VOCs measured in Beijing (39.4 ppb) was much higher than that measured in Shenzhen (16.7 ppb), with methanol and formaldehyde being the most abundant in concentration at both sites. The source apportionment of daytime OVOCs was conducted effectively using a photochemical age-based parameterization method. Biogenic and anthropogenic secondary sources were the main sources of formaldehyde, acetaldehyde, and acetone at both sites, with a total contribution of 46–82%; acetone also had a large regional-scale background contribution (36–38%); methanol and methyl ethyl ketone (MEK) were mainly derived from anthropogenic primary sources (35–55%) at both sites. In addition, the regional background levels of OVOCs measured in North China were shown to be much higher than those measured in South China. The calculation of the total O₃ formation potential (OFP) of OVOCs highlights the comparable contributions from anthropogenic and biogenic sources in both Beijing and Shenzhen, indicating the important role of biogenic OVOC sources even in polluted environments. Since biogenic sources are already important but uncontrollable, anthropogenic emissions in China need to be restricted even more critically in the future.

There is currently great interest in replacing fossil-oil with renewable fuels in energy production. Fast pyrolysis bio-oil (FPBO) made of lignocellulosic biomass is one such alternative to replace fossil oil, such as heavy fuel oil (HFO), in energy boilers. However, it is not known how this fuel change will alter the quantity and quality of emissions affecting human health. In this work, particulate emissions from a real-scale commercially operated FPBO boiler plant are characterized, including extensive physico-chemical and toxicological analyses. These are then compared to emission characteristics of heavy fuel-oil and wood fired boilers. Finally, the effects of the fuel choice on the emissions, their potential health effects and the requirements for flue gas cleaning in small-to medium-sized boiler units are discussed.The total suspended particulate matter and fine particulate matter (PM₁) concentrations in FPBO boiler flue gases before filtration were higher than in HFO boilers and lower or on a level similar to wood-fired grate boilers. FPBO particles consisted mainly of ash species and contained less polycyclic aromatic hydrocarbons (PAH) and heavy metals than had previously been measured from HFO combustion. This feature was clearly reflected in the toxicological properties of FPBO particle emissions, which showed less acute toxicity effects on the cell line than HFO combustion particles. The electrostatic precipitator used in the boiler plant efficiently removed flue gas particles of all sizes. Only minor differences in the toxicological properties of particles upstream and downstream of the electrostatic precipitator were observed, when the same particulate mass from both situations was given to the cells.

This work investigates the absorption properties of soluble brown carbon (BrC), extracted in methanol and water, from ambient aerosol (PM₁₀) samples, collected over an urban background site in Mumbai, India. The diurnal variability was investigated in samples collected in the morning (7–11 a.m.) and afternoon (12–4 p.m.) periods. Absorption properties of BrC (in the 300–600-nm wavelength range) were measured in filter extracts of water-soluble organic carbon (WSOC) and methanol-soluble organic carbon (MSOC). WSOC and MSOC accounted for on average 52% and 77%, respectively, of the measured OC, potentially indicating unextracted BrC and rendering these values the lower bound. Compared with afternoon samples, the morning samples of MSOC and WSOC had increased BrC concentrations and absorption coefficients (bₐbₛ365; 40%–65%). The correlation between bₐbₛ365 and EC, ns-K⁺, and NO₃⁻ in the morning samples indicated contributions from primary sources, including both biomass and vehicular sources. The decreased bₐbₛ365 in the afternoon samples was partly explained by mixing layer dilution, accompanied by a reduction in the concentrations of primary aerosol constituents. Furthermore, in the afternoon samples, ¹HNMR spectroscopy revealed the presence of more oxidized functional groups and significantly higher OC/EC and WSOC/OC ratios, indicating the greater aging of afternoon aerosol. The MAC₃₆₅ (m²gC⁻¹) for both WSOC and MSOC extracts decreased significantly by 20%–34% in the afternoon samples compared with the morning samples, indicating degradation in the absorption properties of the particles and potentially a change in the constituent BrC chromophores.

Biomass burning (BB) is one of the largest sources of carbonaceous aerosols with adverse impacts on air quality, visibility, health and climate. BB emits a few specific aromatic acids (p-hydroxybenzoic, vanillic, syringic and dehydroabietic acids) which have been widely used as key indicators for source identification of BB-derived carbonaceous aerosols in various environmental matrices. In addition, measurement of p-hydroxybenzoic and vanillic acids in snow and ice cores have revealed the historical records of the fire emissions. Despite their uniqueness and importance as tracers, our current understanding of analytical methods, concentrations, diagnostic ratios and degradation processes are rather limited and scattered in literature. In this review paper, firstly we have summarized the most established methods and protocols for the measurement of these aromatic acids in aerosols and ice cores. Secondly, we have highlighted the geographical variability in the abundances of these acids, their diagnostic ratios and degradation processes in the environments. The review of the existing data indicates that the concentrations of aromatic acids in aerosols vary greatly with locations worldwide, typically more abundant in urban atmosphere where biomass fuels are commonly used for residential heating and/or cooking purposes. In contrast, their concentrations are lowest in the polar regions which are avoid of localized emissions and largely influenced by long-range transport. The diagnostic ratios among aromatic acids can be used as good indicators for the relative amounts and types of biomass (e.g. hardwood, softwood and herbaceous plants) as well as photochemical oxidation processes. Although studies suggest that the degradation processes of the aromatic acids may be controlled by light, pH and hygroscopicity, a more careful investigation, including closed chamber studies, is highly appreciated.

To better understand the mechanism of PM₂.₅ explosive growth (EG), we conducted concurrent measurements of gaseous pollutants, PM₂.₅ and its chemical composition (inorganic ions, organic carbon, and element carbon) with a time resolution of 1 h in Shanghai in late autumn and winter from 2014 to 2017. In this study, the EG events, which are defined as the net increase in the mass concentration of PM₂.₅ by more than 100 μg m⁻³ within hours, are separately discussed for 3, 6, or 9 h. The number of EG events decreased from 19 cases in 2014 to 6 cases in 2017 and the corresponding PM₂.₅ concentration on average decreased from 183.6 μg m⁻³ to 128.8 μg m⁻³. Both regional transport and stagnant weather (windspeed < 2.0 m s⁻¹) could lead to EG events. The potential source contribution function (PSCF) shows that the major high-pollution region is in East China (including Zhejiang, Jiangsu, Shandong, and Anhui Province) and the North China Plain. The contribution of stagnant conditions to EG episode hours of 55% (198 h, 156.9 μg m⁻³) is higher than that of regional transport (45%, 230 h, 163.0 μg m⁻³). To study the impact of local emission, chemical characteristics and driving factors of EG were discussed under stagnant conditions. The major components contributing to PM₂.₅ are NO₃⁻ (17.9%), organics (14.1%), SO₄²⁻ (13.1%), and NH₄⁺ (13.1%). The driving factors of EG events are the secondary aerosol formation of sulfate and nitrate and primary emissions (vehicle emissions, fireworks, and biomass burning), but the secondary transformation contributes more to EG events. The formation of sulfate and nitrate is dominated by gas-phase oxidation and heterogeneous reactions, which are enhanced by a high relative humidity. The current study helps to understand the chemical mechanism of haze and provides a scientific basis for air pollution control in Shanghai.

Potential impacts of change in climate on Indian agriculture may be significantly adverse, if not disastrous. There are projections of potential loss in wheat yield due to the rise in daily minimum (Tmin) and maximum (Tmax) temperature, but only few researchers have considered the extent of such loss on a spatial scale. We therefore, systematically studied the effect of change in Tmax, Tmean (daily average temperature) and Tmin, solar radiation (Srad) and precipitation (RAIN) during wheat growing seasons (from 1986 to 2015) on wheat crop yield over five wheat growing zones across India, taking into account the effect modification by aerosol loading (in terms of aerosol optical depth, 2001–2015). We note that for the entire India, 1 °C rise in Tmean resulted a 7% decrease in wheat yield which varied disproportionately across the crop growing zones by a range of −9% (peninsular zone, PZ) to 4% (northern hills zone, NHZ). The effect of Tmean on wheat yield was identical to the marginal effect of Tmax and Tmin, while 1% increase in Srad enhance wheat yield by 4% for all India with small geographical variations (2–5%), except for the northern hill region (−4%). Rise in 1 °C Tmean exclusively during grain filling duration was noted positive for all the wheat growing regions (0–2%) except over central plain zone (−3%). When estimates of weather variables on wheat yield was combined with the estimated impact of aerosols on weather, the most significant impact was noted over the NHZ (−23%), which otherwise varied from −7% to −4%. Overall, the study brings out the conclusive evidence of negative impact of rising temperature on wheat yield across India, which we found spatially inconsistent and highly uncertain when integrated with the compounding effect of aerosols loading.