The soil–air exchange characteristics of total gaseous mercury from a large-scale municipal landfill area

The cycle of mercury (Hg) from a gigantic landfill area (area ∼2.72 km²) was investigated by conducting micrometeorological measurements of its exchange rates across soil–air boundary during the spring season of 2000. Based on this field campaign, we attempted to provide various insights into the Hg exchange processes, especially with respect to the decoupling of the mixed signatures of complex source processes. According to our analysis, the cycle of Hg in the study site appeared to be affected significantly by the vent processes; excessive amount of Hg was expected to be released via ventpipes penetrating up to 60 m depths of the deep landfilled waste layer. The influence of these vent source processes was reflected very sensitively by the windrose pattern. The data collected during the non-easterly winds were representing the typical pattern for a strong source area in which upward emission is predominant in both strength and frequency. On the other hand, the data collected from the easterly winds were characterized by excessive deposition of Hg which we suspect is due mostly to the nearest vent located easterly from our measurement spot. The unique characteristics of each data group, divided by windrose pattern, were consistent from apparent difference in: (1) the absolute magnitude of gradient/flux data sets, (2) frequency of exchange for each of two vertical directions, and (3) E/D (emission/deposition) ratios for most relevant parameters. The analysis of the short-term variability of exchange patterns over a 24-h scale, also exhibited that the patterns for two different conditions were quite contrasting as a function of time. The magnitude of bidirectional fluxes in the present study is significantly high with values of 254±224 (N=71 emissions out of 79 fluxes quantified during non-easterly winds) and −1164±1276 ng m⁻² h⁻¹ (N=14 depositions out of 16 fluxes during easterly winds), respectively. If the computed emission rate is extrapolated, we estimate that annual emission of Hg from the study area can amount to approximately 6 kg which is comparable with the estimates for other areas around the globe under strong Hg-pollution.     

An observational study of the HONO–NO2 coupling at an urban site in Guangzhou City,South China

The temporal behavior of HONO and NO₂ was investigated at an urban site in Guangzhou city, China, by means of a DOAS system during the Pearl River Delta 2006 intensive campaign from 10 to 24 July 2006. Within the whole measurement period, unexpected high HONO mixing ratios up to 2 ppb were observed even during the day. A nocturnal maximum concentration of about 8.43 ± 0.4 ppb was detected on the night of 24 July 2006. Combining the data simultaneously observed by different instruments, the coupling of HONO–NO₂ and the possible formation sources of HONO are discussed. During the measurement period, concentration ratios of HONO to NO₂ ranged from (0.03 ± 0.1) to (0.37 ± 0.09), which is significantly higher than previously reported values (0.01–0.1). Surprisingly, in most cases a strong daytime correlation between HONO and NO₂ was found, contrary to previous observations in China. Aerosol was found to have a minor impact on HONO formation during the whole measurement period. Using a pseudo steady state approach for interpreting the nocturnal conversion of NO₂ to HONO suggests a non-negligible role of the relative humidity for the heterogeneous HONO formation from NO₂.     

The spatial–temporal chemical footprint of pesticides in China from 1999 to 2018

Environmental Science and Pollution Research - The massive use of pesticides brings considerable environmental and human health impacts. This study conducted an overall assessment of the ecological...     

Trends in anthropogenic mercury emissions estimated for South Africa during 2000–2006

Recent studies suggest an increase in mercury (Hg) emissions to the global environment, particularly as a result of anthropogenic activities. This has prompted many countries to complete Hg emission inventories, based on country-specific Hg sources. In this study, information on annual coal consumption and Hg-containing commodities produced in South Africa, was used to estimate Hg emissions during 2000–2006. Based on the information, the UNEP toolkit was used to estimate the amount of Hg released to air and general waste from each activity; using South Africa specific and toolkit based emission factors. In both atmospheric and solid waste releases, coal-fired power plants were estimated to be the largest contributors of Hg emissions, viz. 27.1 to 38.9 tonnes y^?1 in air, and 5.8 to 7.4 tonnes y^?1 in waste. Cement production was estimated to be the second largest atmospheric Hg emission contributor (2.2–3.9 tonnes y^?1), while coal gasification was estimated to be the second largest Hg contributor in terms of general waste releases (2.9–4.2 tonnes y^?1). Overall, there was an increase in total atmospheric Hg emissions from all activities, estimated at ca. 34 tonnes in 2000, to 50 tonnes in 2006, with some fluctuations between the years. Similarly, the total Hg emissions released to general waste was estimated to be 9 tonnes in 2000, with an increase to 12 tonnes in 2006.     

The distribution and sea–air transfer of volatile mercury in waste post-desulfurization seawater discharged from a coal-fired power plant

The waste seawater discharged in coastal areas from coal-fired power plants equipped with a seawater desulfurization system might carry pollutants such as mercury from the flue gas into the adjacent seas. However, only very limited impact studies have been carried out. Taking a typical plant in Xiamen as an example, the present study targeted the distribution and sea–air transfer flux of volatile mercury in seawater, in order to trace the fate of the discharged mercury other than into the sediments. Samples from 28 sampling sites were collected in the sea area around two discharge outlets of the plant, daily and seasonally. Total mercury, dissolved gaseous mercury and dissolved total mercury in the seawater, as well as gaseous elemental mercury above the sea surface, were investigated. Mean concentrations of dissolved gaseous mercury and gaseous elemental mercury in the area were 183 and 4.48 ng m^?3 in summer and 116 and 3.92 ng m^?3 in winter, which were significantly higher than those at a reference site. Based on the flux calculation, the transfer of volatile mercury was from the sea surface into the atmosphere, and more than 4.4 kg mercury, accounting for at least 2.2 % of the total discharge amount of the coal-fired power plant in the sampling area (1 km²), was emitted to the air annually. This study strongly suggested that besides being deposited into the sediment and diluted with seawater, emission into the atmosphere was an important fate for the mercury from the waste seawater from coal-fired power plants.     

The temporal variability of the profile of carcinogenic polycyclic aromatic hydrocarbons in urban air: a study in a medium traffic area in Rome, 1993–1998

The constancy, both temporal and spatial, of the profile of polycyclic aromatic hydrocarbons (PAHs) relative to benzo[a]pyrene (BaP) is a prerequisite to using the BaP-indicator approach in the carcinogenic risk assessment for PAHs. The principal aim of this study was to provide a contribution to validate this approach, by studying the variability of the profile at a typical urban site through a multi-year data set and by comparing the profiles available for different cities. Seven carcinogenic PAHs (benz[a]anthracene, benzo[b+j+k]fluoranthenes, BaP, indeno[1,2,3-cd]pyrene, dibenz[a,h]anthracene) were determined in PM₁₀ 24-h samples collected every third day at a road site; moreover, benzo[e]pyrene was determined as a reference PAH due to its stability. The profile was found stable from year to year. Besides, it was similar to those recently found in other European cities (observed differences within a factor of four) and to those elaborated from earlier (1970s–1980s) investigations. The substantial similarity of profiles, both temporal (on an annual basis) and spatial, supports the validity of the BaP-indicator approach. Large PAH-to-PAH differences were, however, found in the seasonal pattern of profile: they were explained by the different atmospheric degradability of PAHs, whose effect is enhanced under the meteoclimatic conditions typical of the European Mediterranean countries. PAH annual means showed a slight declining trend since 1994. In the last sampling year, mean concentration of BaP was 1.2 ng m⁻³. Within-year differences among monthly averaged PAH concentrations were observed, as large as up to 44-fold for BaP, underlining the need for whole-year monitoring.     

Abundance,characteristics, and spatial–temporal distribution of microplastics in sea salts along the Cox’s Bazar coastal area,Bangladesh

Environmental Science and Pollution Research - Microplastics (MPs), together with microfibers, have emerged as a contaminant of concern all around the globe. MPs have been detected in freshwater,...     

Long-range transport episodes of fine particles in southern Finland during 1999–2007

The frequency, strength and sources of long-range transport (LRT) episodes of fine particles (PM_2.5) were studied in southern Finland using air quality monitoring results, backward air mass trajectories, remote sensing of fire hot spots, transport and dispersion modelling of smoke and chemical analysis of particle samples (black carbon, monosaccharide anhydrides, oxalate, succinate, malonate, SO₄^2?, NO₃^?, K⁺ and NH₄⁺). At an urban background site in Helsinki, the daily WHO guideline value (24-h PM_2.5 mean 25 μg m^?3) was exceeded during 1–7 LRT episodes per year in 1999–2007. The 24-h mean maximum concentrations varied between 25 and 49 μg m^?3 during the episodes, which was 3–6 times higher than the local mean concentration (8.7 μg m^?3) in 1999–2007. The highest particle concentrations (max. 1-h mean 163 μg m^?3) and the longest episodes (max. 9 days) were mainly caused by the emissions from open biomass burning, especially during springs and late-summers in 2002 and 2006. During the period 2001–2007, the satellite remote sensing of active fire hot spots and transport and dispersion modelling of smoke indicated that approximately half of the episodes were caused partly by the emissions from wildfires and/or agricultural waste burning in fields in Eastern Europe, especially in Russia, Belarus and Ukraine. Other episodes were mainly caused by the LRT of ordinary anthropogenic pollutants, e.g. from energy production, traffic, industry and wood combustion. During those ‘other episodes’, air masses also arrived from Eastern Europe, including Poland. The highest concentrations of biomass-burning tracers, such as monosaccharide anhydrides (levoglucosan + mannosan + galactosan) and K⁺, were observed during open biomass-burning episodes, but quite high values were also measured during some winter episodes due to wood combustion emissions. Our results indicate that open biomass burning in Eastern Europe causes high fine particle concentration peaks in large areas of Europe almost every year.     

Atmospheric concentrations,gaseous–particulate distribution,and carcinogenic potential of polycyclic aromatic hydrocarbons in Assiut,Egypt

The concentrations of 15 priority PAHs were determined in the atmospheric gaseous and particulate phases from nine sites across Assiut City, Egypt. While naphthalene, acenaphthene, and fluorene were the most abundant in the gaseous phase with average concentrations of 377, 184, and 181 ng/m³, benzo[b]fluoranthene, chrysene, and benzo[g,h,i]perylene showed the highest levels in the particulate phase with average concentrations of 76, 6, and 52 ng/m³. The average total atmospheric concentration of target PAHs (1,590 ng/m³) indicates that Assiut is one of the highest PAH-contaminated areas in the world. Statistical analysis revealed a significant difference between the levels of PAHs in the atmosphere of urban and suburban sites (P?=?0.029 and 0.043 for gaseous and particulate phases, respectively). Investigation of diagnostic PAH concentration ratios revealed vehicular combustion and traffic exhaust emissions as the major sources of PAHs with a higher contribution of gasoline rather than diesel vehicles in the sampled areas. Benzo[a]pyrene has the highest contribution (average?=?32, 4 % for gaseous and particulate phases) to the total carcinogenic activity (TCA) of atmospheric PAHs. While particulate phase PAHs have higher contribution to the TCA, gaseous phase PAHs present at higher concentrations in the atmosphere are more capable of undergoing atmospheric reactions to form more toxic derivatives.     

Temporal patterns of atmospheric mercury species in northern Mississippi during 2011–2012: Influence of sudden population swings

Gaseous elemental mercury (GEM), gaseous oxidized mercury (GOM) and particulate bound mercury (PBM) were measured on the University of Mississippi campus from July 2011 to June 2012. It is believed to be the first time that concentrations of atmospheric mercury species have been documented in northern Mississippi, and at a location with relatively large and sudden swings in population. The mean concentration (±1SD) of GEM was 1.54 ± 0.32 ng m⁻³; levels were lower and generally more stable during the winter (1.48 ± 0.22) and spring (1.46 ± 0.27) compared with the summer (1.56 ± 0.32) and fall (1.63 ± 0.42). Mean concentrations for GOM and PBM were 3.87 pg m⁻³ and 4.58 pg m⁻³, respectively; levels tended to be highest in the afternoon and lowest in the early morning hours. During the fall and spring academic semesters concentrations and variability of GOM and PBM both increased, possibly from vehicle exhaust. There were moderate negative correlations with wind speed (all species) and humidity (GOM and PBM). Backward air mass trajectory modeling for the ten highest peaks for each mercury species revealed that the majority of these events occurred from air masses that passed through the northern continental US region. Overall, this study illustrates the complexity of temporal fluctuations of airborne mercury species, even in a small town environment.     

Measurements of atmospheric mercury species during an international study of mercury depletion events at Ny-Ålesund,Svalbard, spring 2003. How reproducible are our present methods?

Six groups participated in an international study of springtime atmospheric mercury depletion events (AMDEs) at Ny-Ålesund in the Norwegian Arctic during April and May 2003 with the aim to compare analytical methods for measurements of atmospheric mercury species and study the physical and chemical processes leading to AMDEs. Five groups participated in the method comparison that was conducted at three different locations within Ny-Ålesund. Various automated and manual instrumentation were used to sample, measure and compare gaseous elemental mercury (GEM), reactive gaseous mercury (RGM) and mercury associated with particles (Hg-P). The concentration of GEM was reproducible during background conditions. For the first time using ambient air, the statistics associated with round robin test procedures were applied. This was found to be an appropriate tool to investigate the reproducibility of GEM measurements in ambient air. The precision for each group measuring GEM concentrations was found to be consistently good (within 5%). Five AMDEs were recorded during the study. Using four different methods, including single and replicate samples, all groups recorded higher values of RGM and Hg-P during AMDEs. The results show that measuring comparable atmospheric mercury species at both the same and different locations (within the Ny-Ålesund area) is difficult. Not only do site location and site characteristics create challenges when trying to intercompare results but there are difficulties, as well, in obtaining comparable results with similar sampling and analysis methods. Nevertheless, with our current procedures for atmospheric mercury identification we can differentiate with certainty between “high” and “low” concentration values of RGM and Hg-P.     

Concentrations and accumulation rates of polychlorinated biphenyls in soil along an urban–rural gradient in Shanghai

Environmental Science and Pollution Research - This study proposed an in situ soil experimental system to quantify concentration and accumulation rates of polychlorinated biphenyl (PCB) congeners...     

Towards the analysis of urban livability in China: spatial–temporal changes,regional types,and influencing factors

Environmental Science and Pollution Research - The increasing drift of urbanization and its impact on urban human settlements are of major concern for China cities. Therefore, demystifying the...     

Airborne black carbon concentrations over an urban region in western India—temporal variability, effects of meteorology, and source regions

This study characterizes over 5 years of high time resolution (5 min), airborne black carbon (BC) concentrations (July 2003 to December 2008) measured over Ahmedabad, an urban region in western India. The data were used to obtain different time averages of BC concentrations, and these averages were then used to assess the diurnal, seasonal, and annual variability of BC over the study region. Assessment of diurnal variations revealed a strong association between BC concentrations and vehicular traffic. Peaks in BC concentration were co-incident with the morning (0730 to 0830, LST) and late evening (1930 to 2030, LST) rush hour traffic. Additionally, diurnal variability in BC concentrations during major festivals (Diwali and Dushera during the months of October/November) revealed an increase in BC concentrations due to fireworks displays. Maximum half hourly BC concentrations during the festival days were as high as 79.8 μg m^?3. However, the high concentrations rapidly decayed suggesting that local meteorology during the festive season was favorable for aerosol dispersion. A multiple linear regression (MLR) model with BC as the dependent variable and meteorological parameters as independent variables was fitted. The variability in temperature, humidity, wind speed, and wind direction accounted for about 49% of the variability in measured BC concentrations. Conditional probability function (CPF) analysis was used to identify the geographical location of local source regions contributing to the effective BC measured (at 880 nm) at the receptor site. The east north-east (ENE) direction to the receptor was identified as a major source region. National highway (NH8) and two coal-fired thermal power stations (at Gandhinagar and Sabarmati) were located in the identified direction, suggesting that local traffic and power plant emissions were likely contributors to the measured BC.     

Levels of black carbon and their relationship with particle number levels—observation at an urban roadside in Taipei City

Information on the relationship between black carbon (BC) and particle number levels in urban areas is limited. Therefore, investigating the relationship between BC and particle number levels in different particle size ranges at an urban area is worthwhile. This study used an aethalometer and scanning mobility particle sizer to measure the levels of BC and particle number simultaneously at an urban roadside in Taipei City. Measurement results show that hourly BC levels are 0.62–8.80 μg m^?3 (mean?=?3.50 μg m^?3) and hourly particle number levels are 4.21?×?10³–4.64?×?10⁴ particles cm^?3 (mean?=?2.00?×?10⁴ particles cm^?3) in Taipei urban area. The BC and particle number levels peak during morning (7:00–9:00) and evening (16:00–18:00) rush hours on weekdays. Low BC and particle number levels exist in the early morning hours. Time variations in BC levels are the same as those of particle number levels in this study, clearly indicating that BC and particles are likely released from the same emission source. Additionally, BC levels in the urban area are more strongly associated with ultrafine particle levels than with total particle number levels, particularly in the size range of 56–180 nm. According to measurement results, most BC in aerosols in urban areas can be in the ultrafine size range.     

Characterization of PM2.5-bound polycyclic aromatic hydrocarbons in Atlanta—Seasonal variations at urban,suburban, and rural ambient air monitoring sites

Twenty-eight polycyclic aromatic hydrocarbons (PAH) and methylated PAHs (Me-PAH) were measured in daily PM_2.5 samples collected at an urban site, a suburban site, and a rural site in and near Atlanta during 2004 (5 samples/month/site). The suburban site, located near a major highway, had higher PM_2.5-bound PAH concentrations than did the urban site, and the rural site had the lowest PAH levels. Monthly variations are described for concentrations of total PAHs (∑PAHs) and individual PAHs. PAH concentrations were much higher in cold months than in warm months, with average monthly ∑PAH concentrations at the urban and suburban-highway monitoring sites ranging from 2.12 to 6.85 ng m^?3 during January–February and November–December 2004, compared to 0.38–0.98 ng m^?3 during May–September 2004. ∑PAH concentrations were found to be well correlated with PM_2.5 and organic carbon (OC) within seasons, and the fractions of PAHs in PM_2.5 and OC were higher in winter than in summer. Methyl phenanthrenes were present at higher levels than their un-substituted homologue (phenanthrene), suggesting a petrogenic (unburned petroleum products) input. Retene, a proposed tracer for biomass burning, peaked in March, the month with the highest acreage and frequency of prescribed burning and unplanned fires, and in December, during the high residential wood-burning season, indicating that retene might be a good marker for burning of all biomass materials. In contrast, potassium peaked only in December, indicating that it might be a more specific tracer for wood-burning.