Beyond the material grave: Life Cycle Impact Assessment of leaching from secondary materials in road and earth constructions

In industrialized countries, large amounts of mineral wastes are produced. They are re-used in various ways, particularly in road and earth constructions, substituting primary resources such as gravel. However, they may also contain pollutants, such as heavy metals, which may be leached to the groundwater. The toxic impacts of these emissions are so far often neglected within Life Cycle Assessments (LCA) of products or waste treatment services and thus, potentially large environmental impacts are currently missed. This study aims at closing this gap by assessing the ecotoxic impacts of heavy metal leaching from industrial mineral wastes in road and earth constructions. The flows of metals such as Sb, As, Pb, Cd, Cr, Cu, Mo, Ni, V and Zn originating from three typical constructions to the environment are quantified, their fate in the environment is assessed and potential ecotoxic effects evaluated. For our reference country, Germany, the industrial wastes that are applied as Granular Secondary Construction Material (GSCM) carry more than 45,000 t of diverse heavy metals per year. Depending on the material quality and construction type applied, up to 150 t of heavy metals may leach to the environment within the first 100 years after construction. Heavy metal retardation in subsoil can potentially reduce the fate to groundwater by up to 100%. One major challenge of integrating leaching from constructions into macro-scale LCA frameworks is the high variability in micro-scale technical and geographical factors, such as material qualities, construction types and soil types. In our work, we consider a broad range of parameter values in the modeling of leaching and fate. This allows distinguishing between the impacts of various road constructions, as well as sites with different soil properties. The findings of this study promote the quantitative consideration of environmental impacts of long-term leaching in Life Cycle Assessment, complementing site-specific risk assessment, for the design of waste management strategies, particularly in the construction sector.     

Measurement of Ultrafine Particle Size Distributions from Coal-, Oil-, and Gas-Fired Stationary Combustion Sources

Abstract

Currently, we have limited knowledge of the physical and chemical properties of emitted primary combustion aerosols and the changes in those properties caused by nucleation, condensation growth of volatile species, and particle coagulations under dilution and cooling in the ambient air. A dilution chamber was deployed to sample exhaust from a pilot-scale furnace burning various fuels at a nominal heat input rate of 160 kW/h^?1 and 3% excess oxygen. The formation mechanisms of particles smaller than 420 nm in electrical mobility diameter were experimentally investigated by measurement with a Scanning Mobility Particle Sizer (SMPS) as a function of aging times, dilution air ratios, combustion exhaust temperatures, and fuel types. Particle formation in the dilution process is a complex mixture of nucleation, coagulation, and condensational growth, depending on the concentrations of available condensable species and solid or liquid particles (such as soot, ash) in combustion exhausts. The measured particle size distributions in number concentrations measured show peaks of particle number concentrations for medium sulfur bituminous coal, No. 6 fuel oil, and natural gas at 40-50 nm, 70-100 nm, and 15-25 nm, respectively. For No. 6 fuel oil and coal, the particle number concentration is constant in the range of a dilution air ratio of 50, but the number decreases as the dilution air ratio decreases to 10. However, for natural gas, the particle number concentration is higher at a dilution air ratio of 10 and decreases at dilution air ratios of 20-50. At a dilution air ratio of 10, severe particle coagulation occurs in a relatively short time. Samples taken at different combustion exhaust temperatures for these fuel types show higher particle number concentrations at 645 K than at 450 K. As the aging time of particles increases, the particles increase in size and the number concentrations decrease. The largest gradient of particle number distribution occurs within the first 10 sec after dilution but shows only minor differences between 10 and 80 sec. The lifetimes of the ultrafine particles are relatively short, with a scale on the order of a few seconds. Results from this study suggest that an aging time of 10 sec and a dilution air ratio of 20 are sufficient to obtain representative primary particle emission samples from stationary combustion sources.     

Multi-year hourly PM2.5 carbon measurements in New York: Diurnal,day of week and seasonal patterns

Multi-year hourly measurements of PM_2.5 elemental carbon (EC) and organic carbon (OC) from a site in the South Bronx, New York were used to examine diurnal, day of week and seasonal patterns. The hourly carbon measurements also provided temporally resolved information on sporadic EC spikes observed predominantly in winter. Furthermore, hourly EC and OC data were used to provide information on secondary organic aerosol formation. Average monthly EC concentrations ranged from 0.5 to 1.4 μg m^?3 with peak hourly values of several μg m^?3 typically observed from November to March. Mean EC concentrations were lower on weekends (approximately 27% lower on Saturday and 38% lower on Sunday) than on weekdays (Monday to Friday). The weekday/weekend difference was more pronounced during summer months and less noticeable during winter. Throughout the year EC exhibited a similar diurnal pattern to NO_x showing a pronounced peak during the morning commute period (7–10 AM EST). These patterns suggest that EC was impacted by local mobile emissions and in addition by emissions from space heating sources during winter months. Although EC was highly correlated with black carbon (BC) there was a pronounced seasonal BC/EC gradient with summer BC concentrations approximately a factor of 2 higher than EC. Average monthly OC concentrations ranged from 1.0 to 4.1 μg m^?3 with maximum hourly concentrations of 7–11 μg m^?3 predominantly in summer or winter months. OC concentrations generally correlated with PM_2.5 total mass and aerosol sulfate and with NO_x during winter months. OC showed no particular day of week pattern. The OC diurnal pattern was typically different than EC except in winter when OC tracked EC and NO_x indicating local primary emissions contributed significantly to OC during winter at the urban location. On average secondary organic aerosol was estimated to account for 40–50% of OC during winter and up to 63–73% during summer months.     

Distribution of organochlorine compounds in the sea-surface microlayer, water column and sediment of Singapore's coastal environment

Hexachlorocyclohexanes (HCHs), dichlorodiphenylethanes (DDTs) and 38 PCB congeners were determined in the water column (sea-surface microlayer, subsurface, mid-depth and bottom water) and sediments from Singapore's coastal environment. The concentration ranges for summationHCHs, summationDDTs and summationPCBs in the seawater dissolved phase (DP) were 101-6110 (mean 1833), <5-405 (mean 76) and 60-6979 (mean 1611)pg/l, respectively. The concentration ranges for summationHCHs, summationDDTs and summationPCBs in the suspended particulate matter (SPM) were 26-2395 (mean 243), <5-124 (mean 19) and 38-3793 (mean 715) pg/l, respectively. Concentration levels in sediments ranged between 521 and 1758 (mean 1094), 50 and 290 (mean 88) and 339 and 1356 (mean 858) pg/g for summationHCHs, summationDDTs and summationPCBs, respectively. It was shown that the interfaces of the sea-surface microlayer (SML) and near bottom water are important compartments for the distribution of organochlorine compounds (OCs) in the water column. In comparison with data from China, the concentration levels in the water column and sediments of Singapore can be considered as low, but the reported levels were higher compared to available data from Europe.     

Abiotic degradation (photodegradation and hydrolysis) of imidazolinone herbicides

The abiotic degradation of the imidazolinone herbicides imazapyr, imazethapyr and imazaquin was investigated under controlled conditions. Hydrolysis, where it occurred, and photodegradation both followed first-order kinetics for all herbicides. There was no hydrolysis of any of the herbicides in buffer solutions at pH 3 or pH 7; however, slow hydrolysis occurred at pH 9. Estimated half-lives for the three herbicides in solution in the dark were 6.5, 9.2 and 9.6 months for imazaquin, imazethapyr and imazapyr, respectively. Degradation of the herbicides in the light was considerably more rapid than in the dark with half lives for the three herbicides of 1.8, 9.8 and 9.1 days for imazaquin, imazethapyr and imazapyr, respectively. The presence of humic acids in the solution reduced the rate of photodegradation for all three herbicides, with higher concentrations of humic acids generally having greater effect. Photodegradation of imazethapyr was the least sensitive to humic acids. The enantioselectivity of photodegradation was investigated using imazaquin, with photodegradation occurring at the same rate for both enantiomers. Abiotic degradation of imidazolinone herbicides on the soil surface only occurred in the presence of light. The rate of degradation for all herbicides was slower than in solution, with half-lives of 15.3, 24.6 and 30.9 days for imazaquin, imazethapyr and imazapyr, respectively. Abiotic degradation of these herbicides is likely to be slow in the environment and is only likely to occur in clear water or on the soil surface.