Anthropogenic and natural CO2 emission sources in an arid urban environment

Recent research has shown the Phoenix, AZ metropolitan region to be characterized by a CO2 dome that peaks near the urban center. The CO2 levels, 50% greater than the surrounding non-urban areas, have been attributed to anthropogenic sources and the physical geography of the area. We quantified sources of CO2 emissions across the metropolitan region. Anthropogenic CO2 emission data were obtained from a variety of government and NGO sources. Soil CO2 efflux from the dominant land-use types was measured over the year. Humans and automobile activity produced more than 80% input of CO2 into the urban environment. Soil CO2 efflux from the natural desert ecosystems showed minimal emissions during hot and dry periods, but responded rapidly to moisture. Conversely, human maintained vegetation types (e.g. golf courses, lawns, irrigated agriculture) have greater efflux and are both temperature and soil moisture dependent. Landfills exhibited the most consistent rates, but were temperature and moisture independent. We estimate the annual CO2 released from the predominant land-use types in the Phoenix region and present a graphical portrayal of soil CO2 emissions and the total natural and anthropogenic CO2 emissions in the metropolitan region using a GIS-based approach. The results presented here do not mimic the spatial pattern shown in previous studies. Only, with sophisticated mixing models will we be able to address the total effect of urbanization on CO2 levels and the contribution to regional patterns.     

The long-range dispersion of a plume from an isolated point source

The dispersion of the plume from a sulphide smelter at Mount Isa, Australia, has been determined at distances of up to 1000 km from the source. Simultaneous measurements by an airborne correlation spectrometer, flame photometer and aitken counter have allowed accurate determinations of plume width at these large distances.Radiosonde and pilot-balloon data from four positions spanning the region have been used to calculate the trajectories of each of the plumes measured in the study. In each case the measured plume position was in good agreement with the position predicted on the basis of the wind data.A simple model based on the diurnal variation of the structure of the atmosphere, as well as the turning of the wind with height, is shown to account adequately for the measurements of plume width during well-mixed atmospheric conditions at distances of between 25 and 1000 km from the source.     

Occurrence and source characterization of perfluorochemicals in an urban watershed

Perfluorochemicals (PFCs) are used in numerous applications, mainly as surfactants, and occur ubiquitously in the environment as complex mixtures. This study was undertaken to characterize the occurrence and sources of commonly detected PFC compounds in surface waters of the Marina catchment, a watershed that drains an urbanized section of Singapore. Of the 19 target PFCs, 13 were detected with perfluorooctanoic acid (PFOA) (5-31 ng L⁻¹) and perfluorooctane sulfonate (PFOS) (1-156 ng L⁻¹) being the dominant components. Other compounds detected included perfluoroalkyl carboxylates (C7-C12) and perfluoroalkyl sulfonates (C6 and C8). Sulfonamide compounds detected 2-(N-ethylperfluorooctanesulfonamido) acetic acid (N-EtFOSAA), 2-(N-methylperfluorooctanesulfonamido) acetic acid (N-MeFOSAA), perfluorooctanesulfonamido acetic acid (FOSAA) and perfluorooctanesulfonamide (FOSA) were putative transformation products of N-EtFOSE and N-MeFOSE, the N-ethylated and N-methylated ethyl alcohol derivatives, respectively. Surface water concentrations were generally higher during dry weather than during storm water flow: the median concentrations of total PFCs in dry and wet weather were 57 and 138 ng L⁻¹ compared to 42 and 79 ng L⁻¹, respectively, at Stamford and Alexandra canal, suggesting the presence of a continuous source(s) which is subject to dilution during storm events. In rain water, median concentrations were 6.4 ng L⁻¹, suggesting rain contributed from 12-25% to the total PFC load for non-point source sites. The longitudinal concentration profile along one of the canals revealed a point source of sulfonated PFCs (PFOS), believed to originate from aqueous film-forming foam (AFFF). Sources were characterized using principal component analysis (PCA) and by plotting PFHxS/PFOA against PFOS/PFOA. Typical surface waters exhibit PFOS/PFOA and PFHxS/PFOA ratios below 0.9 and 0.5, respectively. PCA plots reveal waters impacted by “non-typical” PFC sources in Alexandra canal.     

Elevated atmospheric CO2 concentration and temperature across an urban–rural transect

The heat island effect and the high use of fossil fuels in large city centers are well documented, but by how much fossil fuel consumption is elevating atmospheric CO₂ concentrations and whether elevations in both atmospheric CO₂ and air temperature from rural to urban areas are consistently different from year to year are less well known. Our aim was to record atmospheric CO₂ concentrations, air temperature and other environmental variables in an urban area and compare it to suburban and rural sites to see if urban sites are experiencing climates expected globally in the future with climate change. A transect was established from Baltimore city center (Urban site), to the outer suburbs of Baltimore (suburban site) and out to an organic farm (rural site). At each site a weather station was set-up to monitor environmental variables for 5 years. Atmospheric CO₂ was consistently and significantly increased on average by 66 ppm from the rural to the urban site over the 5 years of the study. Air temperature was also consistently and significantly higher at the urban site (14.8 °C) compared to the suburban (13.6 °C) and rural (12.7 °C) sites. Relative humidity was not different between sites whereas the vapor pressure deficit (VPD) was significantly higher at the urban site compared to the suburban and rural sites. An increase in nitrogen deposition at the rural site of 0.6% and 1.0% compared to the suburban and urban sites was small enough not to affect soil nitrogen content. Dense urban areas with large populations and high vehicular traffic have significantly different microclimates compared to outlying suburban and rural areas. The increases in atmospheric CO₂ and air temperature are similar to changes predicted in the short term with global climate change, therefore providing an environment suitable for studying future effects of climate change on terrestrial ecosystems.     

Depositional flux of polychlorinated dibenzo-p-dioxins and polychlorinated dibenzofurans in an urban setting

Dry and wet deposition fluxes of the PCDD/F substituted congeners were measured at two different sites (Clinton Drive and Lang Road) in Houston, TX between December 2003 and April 2004. Average total dry deposition fluxes of 351 and 125pgm(-2)d(-1) were found at Clinton Drive and Lang Road, respectively. A wet deposition flux of 2.873pgm(-2)d(-1) was measured at the Clinton Drive site. The results indicated that the dry deposition process exhibited spatial variability. In addition, the results also demonstrated that precipitation, although intermittent, is the most important mechanism for the removal of dioxins from atmosphere in the area of study. Combining the contributions of the dry and wet deposition processes at Clinton Drive resulted in a total bulk deposition flux of 527pg m(-2)d(-1). The total dry and wet deposition fluxes were dominated by OCDD followed by 1,2,3,4,6,7,8-HpCDD at both sites. Overall average dry deposition velocities of 0.35 and 0.15cms(-1) were calculated at Clinton Drive and Lang Road sites, respectively. While these velocities were similar to velocities observed in other geographical areas, the contribution of OCDD to the total deposition flux in Houston was significantly higher, probably reflecting the unique nature and character of Houston dioxin sources. The results also showed that lower chlorinated congeners, primarily present in the gas phase, are more likely to be removed from the atmosphere by precipitation. Relationships between the detected congeners in the dry deposition samples and other routinely measured air pollutants/meteorological parameters were found. The results showed that in general, the dry deposition of these congeners was consistently negatively correlated with SO(2) and NO(x) concentrations in the air and positively correlated with relative humidity. However, more research is needed to ascertain those correlations.     

An intensive two-week study of an urban CO2 dome in Phoenix,Arizona, USA

Atmospheric CO₂ concentrations were measured prior to dawn and in the middle of the afternoon at a height of 2 m above the ground along four transects through the metropolitan area of Phoenix, Arizona on 14 consecutive days in January 2000. The data revealed the existence of a strong but variable urban CO₂ dome, which at one time exhibited a peak CO₂ concentration at the center of the city that was 75% greater than that of the surrounding rural area. Mean city-center peak enhancements, however, were considerably lower, averaging 43% on weekdays and 38% on weekends; and averaged over the entire commercial sector of the city, they were lower still, registering 30% on weekdays and 23% on weekends. Over the surrounding residential areas, on the other hand, there are no weekday–weekend differences in boundary-layer CO₂ concentration. Furthermore, because of enhanced vertical mixing during the day, near-surface CO₂ concentrations in the afternoon are typically reduced from what they are prior to sunrise. This situation is additionally perturbed by the prevailing southwest-to-northeast flow of air at that time of day, which lowers afternoon CO₂ concentrations on the southern and western edges of the city still more, as a consequence of the importation of pristine rural air. The southwest-to-northeast flow of air also sometimes totally compensates for the afternoon vertical-mixing-induced loss of CO₂ from areas on the northern and eastern sides of the city, as a consequence of the northeastward advection of CO₂ emanating from the central, southern and western sectors of the city. Hence, although complex, the nature of the urban CO₂ dome of Phoenix, Arizona, is readily understandable in terms of basic meteorological phenomena and their interaction with human activities occurring at the land/air interface.     

Mercury exposure in terrestrial birds far downstream of an historical point source

Mercury (Hg) is a persistent environmental contaminant found in many freshwater and marine ecosystems. Historical Hg contamination in rivers can impact the surrounding terrestrial ecosystem, but there is little known about how far downstream this contamination persists. In 2009, we sampled terrestrial forest songbirds at five floodplain sites up to 137 km downstream of an historical source of Hg along the South and South Fork Shenandoah Rivers (Virginia, USA). We found that blood total Hg concentrations remained elevated over the entire sampling area and there was little evidence of decline with distance. While it is well known that Hg is a pervasive and long-lasting aquatic contaminant, it has only been recently recognized that it also biomagnifies effectively in floodplain forest food webs. This study extends the area of concern for terrestrial habitats near contaminated rivers for more than 100 km downstream from a waterborne Hg point source.     

Effect of point source removal on mercury bioaccumulation in an industrial pond

A one hectare pond on the headwaters of a mercury-contaminated creek in Oak Ridge, Tennessee acted as a biochemical reactor for the production of methylmercury, increasing waterborne methylmercury concentrations in the stream below the pond discharge. The flow of the creek was diverted around the pond in order to eliminate this input. Waterborne total mercury, methylmercury, and mercury in fish, were monitored in the pond and stream before and after bypass. Waterborne methylmercury concentration in the creek downstream from the pond decreased over 800% following diversion of streamflow around the pond, but mercury in redbreast sunfish in the pond tailwater did not decline similarly. Within the pond, now isolated from fresh waterborne mercury inputs from the stream, methylmercury concentrations in the water column remained similar to levels present before bypass. However, mercury concentrations in sunfish in the pond decreased approximately 75% following bypass, despite the continued presence of highly contaminated sediments (approximately 50 mg Hg/kg dry weight). We concluded that a decrease in the fraction of 'dissolved methylmercury' in the isolated pond relative to pre-bypass conditions explained the decrease in mercury in fish within the pond. That observation also indicates that mercury associated with pond sediments was relatively unavailable for eventual bioaccumulation when compared to 'fresh' mercury contributed by upstream sources. The lack of a post-bypass decrease in mercury concentrations in tailwater fish was also likely to be associated with the particle-associated nature of waterborne methylmercury exported from the pond.     

Lead concentrations and source strength in the atmosphere of an urban site

A series of atmospheric lead concentration measurements in the Oviedo urban area have been carried out. A linear correlation between lead and large positive ion concentrations has been obtained (r² = 0.88). From this correlation and by use of a box diffusion model, the lead source strength has been calculated. As an application, measurements of large positive ion concentrations can provide an easy method for lead monitoring in an urban site.     

Spatial distribution of submicrometre particles and CO in an urban microscale environment

Traffic is the major source of submicrometre particles in an urban environment but the spatial distribution of particles around an urban site has not been measured. The aim of this paper was to investigate the relationship of CO and particles at a busy central urban location surrounded by buildings. This study measured the concentration and size distribution of submicrometre particles at a fixed location and concentrations of submicrometre particles and CO at 10 locations around a square site in the Brisbane Central Business District (CBD). Changes in concentration were assessed as a function of traffic volume and wind direction and speed.Fixed site measurements of submicrometre particle number concentration varied between 7.9×10² (±40) and 2.6×10⁵ (±1.3×10⁴) cm⁻³ and showed a strong positive correlation with traffic flow rate, confirming that vehicles were the major source of urban submicrometre particles. The particle concentration decreased exponentially with increasing wind speed.Average particle concentrations around the site ranged between 19.7×10³ (±8.2×10³) and 32.5×10³ (±16.6×10³) cm⁻³. Analysis of the particle measurements around the site showed that time and location both had a statistically significant effect on mean particle concentration around the square over the period of the study.Around the site, CO concentration was relatively constant (within instrument error), ranging between 2.2 (±1.9) and 4.5 (±3.0) ppm. Again both time and location had a statistically significant effect on CO concentration during the measurement period. However, CO concentration was not significantly correlated to particle number concentration around the site and examination of between-site comparisons with the two pollutants showing different spatial and temporal trends.The significant difference in the concentration trends between the locations around the square indicates that there is considerable inhomogeneity in the particle concentration around the site. One implication of this is that careful thought must be given to locations of air intakes of air-conditioning systems in urban environments.     

Nonpoint source pollution of urban stormwater runoff: a methodology for source analysis

The characterization and control of runoff pollution from nonpoint sources in urban areas are a major issue for the protection of aquatic environments. We propose a methodology to quantify the sources of pollutants in an urban catchment and to analyze the associated uncertainties. After describing the methodology, we illustrate it through an application to the sources of Cu, Pb, Zn, and polycyclic aromatic hydrocarbons (PAH) from a residential catchment (228 ha) in the Paris region. In this application, we suggest several procedures that can be applied for the analysis of other pollutants in different catchments, including an estimation of the total extent of roof accessories (gutters and downspouts, watertight joints and valleys) in a catchment. These accessories result as the major source of Pb and as an important source of Zn in the example catchment, while activity-related sources (traffic, heating) are dominant for Cu (brake pad wear) and PAH (tire wear, atmospheric deposition).     

SO2 dosages in an urban area

Five winter-semesters of data of SO₂ concentration at three sites in the urban area of Milan were analyzed to generate statistics of dosage which describe the dosage distributions, the temporal structure, the dependence upon concentration thresholds and the six-month-average concentration. By considering the joint distributions of dosages and their durations it is found that the basic ambiguity between dosages and their durations can be resolved since for each dosage value only a limited range of durations is observed. It is also found that the six-month-average concentration has a dominating role on the statistics of dosages; previous works have reported a similar influence on concentration statistics, durations and extreme values. For most of the statistics it has been possible to develop simple and accurate empirical models.     

Outdoor air pollution in close proximity to a continuous point source

Data are lacking on human exposure to air pollutants occurring in ground-level outdoor environments within a few meters of point sources. To better understand outdoor exposure to tobacco smoke from cigarettes or cigars, and exposure to other types of outdoor point sources, we performed more than 100 controlled outdoor monitoring experiments on a backyard residential patio in which we released pure carbon monoxide (CO) as a tracer gas for continuous time periods lasting 0.5–2 h. The CO was emitted from a single outlet at a fixed per-experiment rate of 120–400 cc min^?1 (～140–450 mg min^?1). We measured CO concentrations every 15 s at up to 36 points around the source along orthogonal axes. The CO sensors were positioned at standing or sitting breathing heights of 2–5 ft (up to 1.5 ft above and below the source) and at horizontal distances of 0.25–2 m. We simultaneously measured real-time air speed, wind direction, relative humidity, and temperature at single points on the patio. The ground-level air speeds on the patio were similar to those we measured during a survey of 26 outdoor patio locations in 5 nearby towns. The CO data exhibited a well-defined proximity effect similar to the indoor proximity effect reported in the literature. Average concentrations were approximately inversely proportional to distance. Average CO levels were approximately proportional to source strength, supporting generalization of our results to different source strengths. For example, we predict a cigarette smoker would cause average fine particle levels of approximately 70–110 μg m^?3 at horizontal distances of 0.25–0.5 m. We also found that average CO concentrations rose significantly as average air speed decreased. We fit a multiplicative regression model to the empirical data that predicts outdoor concentrations as a function of source emission rate, source–receptor distance, air speed and wind direction. The model described the data reasonably well, accounting for ～50% of the log-CO variability in 5-min CO concentrations.     

Characteristics influencing the variability of urban CO2 fluxes in Melbourne,Australia

Urban areas are significant contributors to global carbon dioxide emissions. Vehicle emissions and other anthropogenic related activities are a frequent source of CO₂ to the atmosphere, contributing to global warming. Micrometeorological techniques used for observations in Northern Hemisphere cities have found that urban CO₂ fluxes are consistently a source. This study investigates CO₂ fluxes in an Australian city, adding to the global database of CO₂ fluxes in a bid to aid in future development of planning policies concerning reductions in CO₂ emissions. Using the eddy covariance approach, fluxes of CO₂ were measured at a suburban site (Preston) in Melbourne, Australia from February 2004 to June 2005 to investigate temporal variability. A second site (Surrey Hills) with differing surface characteristics (in particular, greater vegetation cover) was also established in Melbourne and ran simultaneously for 6 months (February 2004–July 2004). Results showed that both sites were a net source of CO₂ to the atmosphere. Diurnal patterns of fluxes were largely influenced by traffic volumes, with two distinct peaks occurring at the morning and evening traffic peak hours, with the winter morning peak averaging 10.9 μmol m⁻² s⁻¹ at Preston. Summer time fluxes were lower than during winter due to greater vegetative influence and reduced natural gas combustion. Vegetation limited the source of CO₂ in the afternoon, yet was not enough to combat the strong local anthropogenic emissions. Surrey Hills showed higher fluxes of CO₂ despite greater vegetation cover because of higher local traffic volumes. Annual emissions from Preston were estimated at 84.9 t CO₂ ha⁻¹ yr⁻¹. Magnitudes and patterns of suburban CO₂ fluxes in Melbourne were similar to those observed in Northern Hemisphere suburban areas.     

Assessment of the fate of sulfur dioxide from a point source

A simplified plume transport model is adopted to assess reaction and scavenging processes. Experimental data on the conversion rate of SO₂ to SO₄²⁻ and the uptake rates by vegetation and soil are used to calculate the relative importance of the various fates of sulfur dioxide. Meteorological parameters include wind speed, day and night mixing heights, night diffusion above the mixing height and plume dispersion angle. Other parameters considered are length of day and night, region, season, type of canopy, and emission rate of SO₂ from a point source.     

世界化石能源部门CO2排放源状况及案例分析

能源部门是CO2排放的主要来源,1990-2005年,电力和热力是能源部门CO2排放的主要排放源,其次是交通运输业.从2005年经济合作与发展组织(OECD)和非OECD国家主要地区的能源部门各排放源对人均CO2排放的贡献率的情况看,北美OECD地区是电力和热力人均CO2排放量最高的地区,其他各排放源不同程度地高出世界平均水平;整体上,非OECD国家主要地区的能源部门各排放源对人均CO2排放的贡献率差异较大,各地区的经济结构、能源结构和生活水平影响能源部门各排放源对人均CO2排放的贡献率.从2005年主要国家的能源部门各排放源对人均CO2排放的贡献率的情况看,除印度外,电力和热力是大多数国家能源部门的CO2主要排放源.中国的电力和热力对能源部门人均CO2排放的贡献率最大.各国对能源部门人均CO2排放的贡献率的次排放源情况相差较大,美国和欧盟(27)主要是交通运输业等服务型产业,中国主要是制造业和建筑业等第二产业,其他国家的次排放源分布相对均衡.     

A passive sampling method for radiocarbon analysis of atmospheric CO2 using molecular sieve

Radiocarbon (¹⁴C) analysis of atmospheric CO₂ can provide information on CO₂ sources and is potentially valuable for validating inventories of fossil fuel-derived CO₂ emissions to the atmosphere. We tested zeolite molecular sieve cartridges, in both field and laboratory experiments, for passively collecting atmospheric CO₂. Cartridges were exposed to the free atmosphere in two configurations which controlled CO₂ trapping rate, allowing collection of sufficient CO₂ in between 1.5 and 10 months at current levels. ¹⁴C results for passive samples were within measurement uncertainty of samples collected using a pump-based system, showing that the method collected samples with ¹⁴C contents representative of the atmosphere. δ¹³C analysis confirmed that the cartridges collected representative CO₂ samples, however, fractionation during passive trapping means that δ¹³C values need to be adjusted by an amount which we have quantified. Trapping rate was proportional to atmospheric CO₂ concentration, and was not affected by exposure time unless this exceeded a threshold. Passive sampling using molecular sieve cartridges provides an easy and reliable method to collect atmospheric CO₂ for ¹⁴C analysis.