Elevated lead mobility in sediments of a eutrophic drinking water reservoir during spring and summer seasons: Insights from isotopic signatures.

Lead (Pb) pollution in sediments remains a major concern for ecosystem quality due to the robust interaction at the sediment/water interface, particularly in shallow lakes. However, understanding the mechanism behind seasonal fluctuations in Pb mobility in these sediments is lacking. Here, the seasonal variability of Pb concentration and isotopic ratio were investigated in the uppermost sediments of a shallow eutrophic drinking lake located in southeast China. Results reveal a sharp increase in labile Pb concentration during autumn-winter period, reaching ∼ 3-fold higher levels than during the spring-summer seasons. Despite these fluctuations, there was a notable overlap in the Pb isotopic signatures within the labile fraction across four seasons, suggesting that anthropogenic sources are not responsible for the elevated labile Pb concentration in autumn-winter seasons. Instead, the abnormally elevated labile Pb concentration during autumn-winter was probably related to reduction dissolution of Fe/Mn oxides, while declined labile Pb concentration during spring-summer may be attributed to adsorption/precipitation of Fe/Mn oxides. These large seasonal changes imply the importance of considering seasonal effects when conducting sediment sampling. We further propose a solution that using Pb isotopic signatures within the labile fraction instead of the bulk sediment can better reflect the information of anthropogenic Pb sources.

Coupling isotopic signatures and partial extraction method to examine lead pollution in mangrove sediments.

Elevated lead (Pb) has been widely observed in mangrove sediments due to human activities, yet understanding the sources of Pb in these sediments and the factors influencing Pb accumulation is challenging. Here, we combined Pb isotopes with partial extraction methods to study Pb contamination levels in mangrove sediments from the eastern and western parts of the Maowei Sea, China. Our results showed that the Pb in the leachate and residual fraction was mainly from anthropogenic and natural sources, respectively. The use of 204Pb isotope analysis can reveal some overlooked differences between anthropogenic and natural sources. Calculation by Bayesian mixing model showed no significant difference in the total anthropogenic contribution between the two sites, but the relative contribution of each end member differed. The contribution of Pb/Zn ores was much higher in the eastern sites (30.9 ± 5.1%) than in the west (18.4 ± 5.5%), while that of agricultural activities was much lower in the east (5.2 ± 3.1%) than in the west (13.5 ± 4.6%). The elevated anthropogenic Pb accumulation in mangrove sediments was ascribed to organic matter. This study provides more data on Pb isotopic composition and new insights into Pb biogeochemistry in the mangrove environment.

Isotopic signatures unveil the lead sources and migration in surface mangrove sediments.

Mangrove sediments act as both sinks and secondary sources for lead (Pb), yet the sources, migration, and transformations of Pb in mangrove environments are poorly understood. In this study, Pb concentration in three mangrove sediments adjacent to different land-use types was evaluated. The Pb sources were quantitatively identified using Pb isotopes. Our data indicated minor Pb contamination in the mangrove sediments, possibly due to the relative lack of developed industry in this region. The Pb isotopic ratios suggested, on average, natural sources, coal combustion, agricultural activities, and traffic-related emissions respectively contributed approximately 61.4 %, 18.8 %, 14.0 %, and 5.8 % of the Pb accumulation in the mangrove sediments, suggesting that coal combustion and agriculture were important anthropogenic Pb sources. Significant relationships were observed between the 206Pb/207Pb ratios and total organic content (TOC) in mangrove sediments, which implied contrasting Pb cycling in two mangrove environments. We further suggested that organic matter and sulfur content significantly reduced Pb mobility and bioavailability in mangrove sediments. Our study provides isotopic method to investigate the Pb sources and migration in the mangrove environment.

Slight transition in Chinese atmospheric Pb isotopic fingerprinting due to increasing foreign Pb.

Atmospheric lead (Pb) pollution negatively affects human health and ecosystem, and extensive research is required to identify its sources and develop robust mitigation methods. In this study, the concentration and isotopic composition of Pb in fine particulate matter (PM2.5) at five sites in the China's Beijing-Tianjin-Hebei (BTH) region were analyzed. The results showed that the Pb concentration in the BTH region declined along the northwest direction in winter owing to the East Asian monsoon. Pb isotopic signatures confirmed that anthropogenic activities significantly contributed to Pb pollution, compared with natural sources. With the increasing import of foreign Pb (with a relatively lower 208Pb/206Pb ratio) to China, we hypothesized that the unique isotopic signature of Pb in Chinese aerosols may decline over time. Therefore, the application of the isotopic approach for quantifying Pb transported from China should be carefully appraised in future research to provide a realistic estimate of the contribution of local sources and the transboundary effect consistent with air mass trajectories analysis. This study provides a theoretical reference for supporting the utilization of Δ208Pb values for better clarify the transboundary impact of Pb pollution and to reduce international disputes.

Tracing the transboundary transport of atmospheric Particulate Bound Mercury driven by the East Asian monsoon.

Taking Beijing-Tianjin-Hebei (BTH) with severe atmospheric mercury (Hg) and PM2.5 pollution as a typical region, this study clarified the characteristics and transboundary transport of atmospheric Particulate Bound Mercury (PBM2.5) affected by the East Asian monsoon. Five sampling sites were conducted in rural, suburban, urban, industrial, and coastal areas of BTH from northwest to southeast along the East Asian monsoon direction. PBM2.5 showed increasing concentrations from northwest to southeast and negative δ202Hg values, indicating significant contributions from anthropogenic sources. However, the mean Δ199Hg values of PBM2.5 at the five sites were significantly positive, probably triggered by the photoreduction of Hg(II) during long-range transport driven by the East Asian monsoon. Apart from local anthropogenic emissions as the primary sources, the transboundary transport of PBM2.5, driven by west and northwest air masses originating in Central Asia and Russia, contributed significantly to the PBM2.5 pollution of BTH. Moreover, these air masses reaching BTH would carry elevated PBM2.5 concentrations further transported to the ocean by the East Asian monsoon. In contrast, the southeast air masses transported from the ocean by the East Asian monsoon in summer diluted inland PBM2.5 pollution. This study provides insight into the atmospheric Hg circulation affected by the East Asian monsoon.

The isotopic patterns and source apportionment of nitrate and ammonium in atmospheric aerosol.

Nitrate (NO3-) and ammonium (NH4+) are the major components in inorganic aerosol. However, their sources and formation processes remain unclear. This study conducted a year-round field measurement of TSP, PM2.5 and PM1.0 in five different sites in the Beijing-Tianjin-Hebei (BTH) region to determine the concentrations of water-soluble inorganic ions (WSIIs) and the isotopic compositions of inorganic nitrogen (δ15N-NH4+, δ15N-NO3-, and δ18O-NO3-). The results showed the highest concentration of WSIIs in winter and lowest in summer. δ15N-NO3-, δ18O-NO3-, and δ15N-NH4+ were in the range of -6.1-18.2, 52.2-103.8, and -28.7-36.2‰, respectively. The seasonal variations of δ15N-NO3- and δ15N-NH4+ were an indication of relative contributions of the main sources and effects of meteorological conditions. The source apportionment identified fossil fuel combustion (38.2-50.6%), agricultural emissions (18-24.7%), biomass burning (16.3-22.7%), and road dust/soil (8.7-23.4%) were the main sources of inorganic aerosols. The local sources and regional migration contributed to the level of inorganic aerosol pollution. In winter, the aerosol in the BTH region was affected by the air mass from the northwest. While in spring and summer, the air mass was mainly from the South China. The low temperature and high relative humidity favored to the formation of inorganic nitrogen aerosol, and solar radiation affected the formation processes of inorganic aerosols by changing the oxidation pathway of NO3- and accelerating the volatilization and dissociation of ammonium nitrate (NH4NO3). This study discovered the main source contributions of inorganic nitrogen aerosol using N and O isotopes composition, and the obtained information has a great importance in understanding the effects of meteorological conditions on formation and the contribution of regional transport.

Atmospheric lead pollution in a typical megacity: Evidence from lead isotopes.

Atmospheric lead (Pb) pollution has adverse health effects on humans, while the sources and atmospheric process of Pb are key scientific problems. In this study, the concentrations and isotopic composition of Pb in fine particulate matter (PM2.5), coal and street dust samples collected from a typical megacity Beijing were analyzed to identify the sources of atmospheric Pb. Results showed that the Pb concentrations in PM2.5 were high in winter (168.1 ± 32.0 ng/m3) and low in summer (27.7 ± 9.1 ng/m3), whereas Pb isotopic values presented opposite variation trends. The abnormally elevated Pb concentrations in winter were probably related to coal combustion, while declined Pb concentration in summer may be attributed to favorable meteorological parameters such as high temperature, high wind speed, and frequent rain events. Pb isotopic ratios indicated that anthropogenic sources (coal combustion and vehicle exhaust) and natural sources were the main contributors to Pb in PM2.5. Combined with the binary model, the anthropogenic sources predominantly contributed to Pb in the Beijing atmosphere by approximately 85% annually, while the natural sources accounted for the rest of 15%. More specifically, the contribution of natural sources was about 9.4% in spring, 29.7% in summer, 16.0% in autumn and 6.1% in winter, suggesting that natural sources might contribute more lead into the atmosphere during clear days. Furthermore, the contribution of the vehicle exhaust to atmospheric Pb was nonnegligible in megacity, highlighting that the ownership of motor vehicles in megacity should be regulated and more efforts should be paid to strengthen vehicle emission standard. This study may enrich the reservoir of Pb isotopic composition in nature and provides a new method to investigate the Pb migration and transformation in the environment, and also serve as a theoretical reference for pollution control measures.