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.     

An ultracompact photo-ionization time-of-flight mass spectrometer with a novel vacuum ultraviolet light source for on-line detection of organic trace compounds and as a detector for gas chromatography

A recently developed novel intense rare-gas excimer vacuum ultraviolet (VUV) light source, the electron beam-pumped excimer lamp (EBEL), has been applied to the soft single-photon ionization (SPI) of organic molecules in a compact orthogonal acceleration time-of-flight mass spectrometer (oaTOFMS). The SPI-oaTOFMS system was applied to the on-line monitoring of tobacco smoke. With this setup, it was possible to analyze the composition of individual puffs of cigarette smoke. Furthermore, a gas chromatograph (GC) was coupled to the EBEL SPIoaTOFMS system. Soft photo-ionization represents an additional separation dimension. By combination of the gas chromatographic and the soft-ionization mass spectroscopic separation dimensions, a truly multidimensional comprehensive analytical method could be derived.     

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.     

Copper availability in seven Israeli soils incubated with and without biosolids

Land application is becoming a preferred option for disposal of sewage sludge (biosolids) from wastewater treatment plants. However, it creates potential risks due to the heavy metal contents of these materials, with copper (Cu) being of chief concern. The long-term fate of biosolid metals applied to agricultural soils is not well understood, particularly in the soils of the Middle East. This investigation was conducted to determine whether the availability of Cu changes with time in biosolid-amended and nonamended soils from Israel. Seven soils, typifying the span of properties and formation environments encountered in Israel, were incubated with and without biosolids for 7 yr, and changes in organic carbon (OC) content and labile Cu concentration were determined. Isotopic exchange techniques, using 64Cu, and ion activity measurements, using a Cu2+ ion selective electrode, revealed that the available Cu concentration remained relatively low and stable over the 7-yr incubation. This was despite substantial reductions in OC. This study shows that, with regard to Cu, application of such biosolids to these soils at rates of up to 250 Mg ha(-1) does not pose a threat to the environment in the short to medium term.     

How has a shortage of census and geological information impeded the regularization of artisanal and small‐scale mining?

There is growing consensus that a combination of laissez‐faire policies, ad hoc regulation and debilitating support services has perpetuated socio‐economic and environmental deterioration in the artisanal and small‐scale mining (ASM) industry. However, a lack of anthropological and geological information on ASM prevents many governments both from improving the policy environment of the industry, and from providing more robust extension services to its operators. This article aims to examine more precisely how a deficiency of baseline census and geological data has inhibited industry formalization and undermined many of the measures implemented to address pressing problems at ASM sites. Specifically, it is argued that insufficient knowledge of artisanal mining populations — including their demographic structure — and of areas suitable for ASM activities affects the ability of a government to regularize, as well as to improve, the organization of this largely informal sector of industry. Case studies of Ghana and Zimbabwe are used to illustrate how the undertaking of low‐budget projects in areas of geological prospecting and population analysis could improve the efficiency of ASM assistance.