Analysis of 3-year observations of CFC-11, CFC-12 and CFC-113 from a semi-rural site in China

In-situ measurements of atmospheric chlorofluorocarbons (CFCs) can be used to the assess their global and regional emissions and to check for compliance with phase-out schedules under Montreal protocol and its amendments. The atmospheric mixing ratios of CFC-11 (CCl₃F), CFC-12 (CCl₂F₂) and CFC-113 (CCl₂F–CClF₂) have been measured by an automated in-situ GC-ECDs system at the regional Chinese Global Atmosphere Watch (GAW) station Shangdianzi (SDZ), from November 2006 to October 2009. The time series for these three principal CFCs showed large episodic events and background conditions occurred for approximately 30% (CFC-11), 52% (CFC-12) and 56% (CFC-113) of the measurements. The mean background mixing ratios for CFC-11, CFC-12 and CFC-113 were 244.8 ppt (parts per trillion, 10^?12, molar) 539.6 ppt and 76.8 ppt, respectively, for 2006–2009. The enhanced CFC mixing ratios compared to AGAGE sites such as Trinidad Head (THD), US and Mace Head (MHD), Ireland suggest regional influences even during background conditions at SDZ, which is much closer to highly-populated areas. Between 2006 and 2009 background CFCs exhibited downward trends at rates of ?2.0 ppt yr^?1 for CFC-11, ?2.5 ppt yr^?1 for CFC-12 and ?0.7 ppt yr^?1 for CFC-113. De-trended 3-year average background seasonal cycles displayed small fluctuations with peak-to-trough amplitudes of 1.0 ± 0.02 ppt (0.4%) for background CFC-11, 1.3 ± 2.1 ppt (0.3%) for CFC-12 and 0.2 ± 0.4 ppt (0.3%) for CFC-113. On the other hand, during pollution periods these CFCs showed much larger seasonal cycles of 11.2 ± 10.7 ppt (5%) for CFC-11, 7.5 ± 6.5 ppt (2%) for CFC-12 and 1.0 ± 1.2 ppt (1.2%) for CFC-113, with apparent winter minima and early summer maxima. This enhancement was attributed to prevailing wind directions from urban regions in summer and to enhanced anthropogenic sources during the warm season. In general, horizontal winds from northeast showed negative contribution to atmospheric CFCs loading, whereas South Western advection (urban sector: Beijing) had positive contributions.     

Degradation rates of CFC-11, CFC-12 and CFC-113 in anoxic shallow aquifers of Araihazar, Bangladesh

Chlorofluorocarbons CFC-11 (CCl(3)F), CFC-12 (CCl(2)F(2)), and CFC-113 (CCl(2)F-CClF(2)) are used in hydrology as transient tracers under the assumption of conservative behavior in the unsaturated and saturated soil zones. However, laboratory and field studies have shown that these compounds are not stable under anaerobic conditions. To determine the degradation rates of CFCs in a tropical environment, atmospheric air, unsaturated zone soil gas, and anoxic groundwater samples were collected in Araihazar upazila, Bangladesh. Observed CFC concentrations in both soil gas and groundwater were significantly below those expected from atmospheric levels. The CFC deficits in the unsaturated zone can be explained by gas exchange with groundwater undersaturated in CFCs. The CFC deficits observed in (3)H/(3)He dated groundwater were used to estimate degradation rates in the saturated zone. The results show that CFCs are degraded to the point where practically no (<5%) CFC-11, CFC-12, or CFC-113 remains in groundwater with (3)H/(3)He ages above 10 yr. In groundwater sampled at our site CFC-11 and CFC-12 appear to degrade at similar rates with estimated degradation rates ranging from approximately 0.25 yr(-1) to approximately 6 yr(-1). Degradation rates increased as a function of reducing conditions. This indicates that CFC dating of groundwater in regions of humid tropical climate has to be carried out with great caution.     

The use of CFC-12, CFC-11 and CH3CCl3 to trace terrestrial airborne pollutant transport by land–sea breezes

Time-series observations of the atmospheric concentrations of the halocarbons, trichlorofluorocarbon (CFC-11), dichlorofluorocarbon (CFC-12), 1,2-trichlorofluoroethane (CFC-113), methyl chloroform (CH₃CCl₃) and carbon tetrachloride (CCl₄) were conducted at a site in Lukang, in Central Taiwan between April and August 2004. Fluctuations in atmospheric concentrations of CFC-11, CFC-12 and CH₃CCl₃ were generally driven by diurnal land–sea breeze and anthropogenic activity in this area. Elevated levels of CFC-11, CFC-12, and CH₃CCl₃ frequently occurred when the air was stagnant and the prevailing seaward land breeze was dominant. Atmospheric concentrations of CFC-113 and CCl₄ were much less variable relative to CFC-11, CFC-12 and CH₃CCl₃ during the same period, indicating that emissions of these two species from anthropogenic activities were small. The time-series distributions of atmospheric levels of CFC-12, CFC-11, CH₃CCl₃ and CO were characterized as a diurnal cycle with an elevated level at night and a low level during the daytime for most of the observed periods. As CFC-12, CFC-11 and CH₃CCl₃ behave as traffic- and industry-derived airborne pollutants in the urban atmosphere, they provide as a useful tracer in the application for the study of terrestrial airborne pollutants transport across the coastal area driven by land–sea breezes in this area.     

Characteristics of chlorofluorocarbons (CFCs) emitted from a municipal waste treatment facility

The emission concentrations of several chlorofluorocarbons (CFCs) were measured from a municipal waste treatment facility (located in Seoul, Republic of Korea) to investigate the emission characteristics of CFCs in the urban environment. To this end, a total of five CFCs (CFC-10, CFC-11, CFC-20, CFC-30, and CFC-113) were analyzed by the thermal desorption-gas chromatography-mass spectrometry (TD-GC-MS) method. The results of this study indicate that the formation of CFC-11 (8.21 ± 1.68 ppb in spring) and CFC-20 (3.92 ± 3.93 ppb in spring) proceeded very actively within the facility. Moreover, CFC-113 was also found in relatively high concentrations (3.34 ± 1.31 ppb in spring) in the treatment facility. Unlike other CFCs, CFC-10 was observed mainly at ambient (and reference) locations and one point inside the treatment facility. In conclusion, emissions of some important CFCs are a prominent process, as they were measured either frequently or abundantly both in winter and spring. It is further indicated that certain CFCs (like CFC-11 and CFC-30) are subject to highly significant seasonal variations.     

Characteristics of chlorofluorocarbons (CFCs) emitted from a municipal waste treatment facility

The emission concentrations of several chlorofluorocarbons (CFCs) were measured from a municipal waste treatment facility (located in Seoul, Republic of Korea) to investigate the emission characteristics of CFCs in the urban environment. To this end, a total of five CFCs (CFC-10, CFC-11, CFC-20, CFC-30, and CFC-113) were analyzed by the thermal desorption–gas chromatography–mass spectrometry (TD–GC–MS) method. The results of this study indicate that the formation of CFC-11 (8.21 ± 1.68 ppb in spring) and CFC-20 (3.92 ± 3.93 ppb in spring) proceeded very actively within the facility. Moreover, CFC-113 was also found in relatively high concentrations (3.34 ± 1.31 ppb in spring) in the treatment facility. Unlike other CFCs, CFC-10 was observed mainly at ambient (and reference) locations and one point inside the treatment facility. In conclusion, emissions of some important CFCs are a prominent process, as they were measured either frequently or abundantly both in winter and spring. It is further indicated that certain CFCs (like CFC-11 and CFC-30) are subject to highly significant seasonal variations.     

Ambient halocarbon mixing ratios in 45 Chinese cities

During this study 158 whole air samples were collected in 45 Chinese cities in January and February 2001. The spatial distribution of different classes of halocarbons in the Chinese urban atmosphere, including chlorofluorocarbons (CFCs), hydrochlorofluorocarbons (HCFCs), hydrofluorocarbons (HFCs), Halon-1211, and other chlorinated compounds is presented and discussed. Most of these compounds were enhanced compared to background levels. However, the mean enhancement of CFCs was relatively small, with CFC-12 and CFC-11 increases of 6% (range 1–31%) and 10% (range 2–89%), respectively, with respect to the global background. On the contrary, strongly enhanced levels of CFC replacement compounds and halogenated compounds used as solvents were measured. The average Halon-1211 concentration exceeded the background of 4.3 pptv by 75% and was higher than 10 pptv in several cities. Methyl chloride mixing ratios were also strongly elevated (78% higher than background levels), which is likely related to the widespread use of coal and biofuel in China.     

Historic emissions of fluorotrichloromethane (CFC-11) based on a market survey

Releases of CFCs occur promptly from applications such as aerosol sprays, or over a period of several years from refrigeration and air conditioning or more slowly still from use as blowing agents for closed cell plastic foams. As a consequence of the Montreal Protocol, the emissions have fallen and their pattern is continuing to change. To help quantify these changes the emissions from closed cell foam blowing have been re-examined in a comprehensive market survey, developing a lifecycle assessment for each foam type, production method and foaming agent.The original model for the time series of emissions from foam applications was shown to remain a robust representation in general terms. There is an “immediate” loss when the foam is manufactured, a slow emission from the foam itself during use and a loss on disposal of the artefact made with the foam. The original model used an initial loss rate of 10% and a subsequent loss of 4.5% yr⁻¹ over 20 yr.The new survey showed a wide range of initial and service loss rates. Immediate release ranges from 95% down to 4%; similarly, the rate of loss during service varies from 0.5% to 5% yr⁻¹ and the service lifetimes of the artefacts made with the foams varies from 12 to 50 yr. The apparent emission function, in terms of the mean value of the annual fractional release from the bank of CFC-11 residing in foams, was calculated from the survey to be 0.043±0.008 over 28 yr. There is a small and non-significant fall in this function with time; so that over the last ten years of the data record the more appropriate value is 0.0366±0.0008. However, up to the early 1990s, it is the original emission function that is consistent with the observed atmospheric concentrations. Thenceforth this function seriously overpredicts the concentrations but, if the new emissions function for foams is used from 1993 onwards in conjunction with the original emission functions for all other uses, the fit becomes better. This suggests that the emission functions for prompt and short term releases remain valid and should be coupled with the new function to calculate emissions of CFC-11 or other fluorocarbon foam blowing agents from the early 1990s onwards.     

Surface measurements of trace gases in the tropical region near hyderabad

Surface air samples were collected near Hyderabad during the period of 12–27 March 1985. These samples were analysed for CFC-11, CFC-12, CFC-114, CFC-12B1, CH₄ and CO using gas Chromatographic techniques. Results show lower mixing ratios of these halogenated hydrocarbons near Hyderabad compared with concentrations observed at other places in the tropical/extratropical regions. However, the concentration of methane observed near Hyderabad is the same as the annual average observed in the same latitude region as well as the global average. This indicates that there is no significant regional source of these species in the Hyderabad region.     

Reductive dechlorination of chlorofluorocarbons and hydrochlorofluorocarbons in sewage sludge and aquifer sediment microcosms

The reductive transformation of the 10 most-widely distributed fluorinated volatile compounds and of tetrachloroethene was investigated for up to 177 days under anaerobic conditions in sewage sludge and aquifer sediment slurries. Concentrations of parent compounds and of degradation products were identified by GC-MS. We observed transformation of CFC-11 to HCFC-21 and HCFC-31, of CFC-113 to HCFC-123a, chlorotrifluoroethene and trifluoroethene, of CFC-12 to HCFC-22, of HCFC-141b to HCFC-151b, and of tetrachloroethene to vinyl chloride and ethene. CFC-114, CFC-115, HCFC-142b, HFC-134a and HCFC-22 were not transformed. The results suggest that with both inocula studied here, hydrogenolysis is the primary reductive dechlorination reaction. CFC-113 was the only compound where a dichloro-elimination was observed, leading to the formation of chlorotrifluoroethene as temporal intermediate and to trifluoroethene as end product. The relative reduction rates of chlorofluoromethanes compared reasonably well with theoretical rates calculated based on thermochemical data according to the Marcus theory. Some of the accumulating HCFCs and haloethenes observed in this study are toxic and may be of practical relevance in anaerobic environments.     

Mercury concentrations and air/soil fluxes in Wuchuan mercury mining district,Guizhou province,China

Wuchuan Hg mine, located in the Circum-Pacific Global Mercuriferous Belt, is one of the important Hg production centers in Guizhou province, China. Soil Hg concentrations in this area are elevated by 2–4 orders of magnitude compared to the national background value in soil which is 0.038 μg g⁻¹. In situ air Hg concentrations and air/soil Hg fluxes were measured at five sampling sites in Wuchuan Hg mining area (WMMA) from 19 to 26 December 2003 and from 18 to 25 December 2004. The results showed that air Hg concentrations were 2–4 orders of magnitude higher than those observed in background areas in Europe and North America due to a large amount of Hg emission from artisanal Hg smelting activities. The average in situ Hg fluxes at site Laohugou, Jiaoyan, Luoxi, Sankeng and Huanglong were −5493, 124, −924, −13 and 140 ng m⁻² h⁻¹, respectively. Diurnal pattern of Hg flux was not found and a number of negative Hg fluxes were observed in our sampling campaigns. The correlations between Hg fluxes and meteorological parameters such as solar irradiation, air temperature, soil temperature and relative humidity and air Hg concentrations were investigated. The commonly observed significant correlations between Hg fluxes and meteorological parameters observed in many previous studies were not obtained in WMMA. However, significantly negative correlations between Hg flux and air Hg concentration were observed at all sites. Our study demonstrated that highly elevated air Hg concentrations could suppress Hg emission processes even from Hg-enriched soil. At specific conditions in WMMA, air Hg concentrations play a dominant role in controlling Hg emission from soil.     

Transport of hydrocarbons from an emplaced fuel source experiment in the vadose zone at Airbase Vaerløse, Denmark

An emplaced hydrocarbon source field experiment was conducted in the relatively homogeneous sandy geology of the vadose zone at Airbase Vaerl?se, Denmark. The source (10.2 l of NAPL) consisted of 13 hydrocarbons (n-, iso- and cyclo-alkanes and aromates) and CFC-113 as a tracer. Monitoring in the 107 soil gas probes placed out to 20 m from the centre of the source showed spreading of all the compounds in the pore air and all compounds were measured in the pore air within a few hours after source emplacement. Seven of the fourteen compounds were depleted from the source within the 1 year of monitoring. The organic vapours in the pore air migrated radially from the source. The CFC-113 concentrations seemed to be higher in the deeper soil gas probes compared with the hydrocarbons, indicating a high loss of CFC-113 to the atmosphere and the lack of degradation of CFC-113. For the first days after source emplacement, the transport of CFC-113, hexane and toluene was successfully simulated using a radial gas-phase diffusion model for the unsaturated zone. Groundwater pollution caused by the vadose zone hydrocarbon vapours was only detected in the upper 30 cm of the underlying groundwater and only during the first 3 months of the experiment. Only the most water-soluble compounds were detected in the groundwater and concentrations decreased sharply with depth (approximately one order of magnitude within 10 cm depth) to non-detect at 30 cm depth. The groundwater table varied more than 1 m within the measurement period. However that did not influence the direction of the groundwater flow. Approximately 7 months after source emplacement the groundwater table rose more than 1 m within 1 month. That did not cause additional pollution of the groundwater.     

Destruction of Chlorofluorocarbons in a Cement Kiln

Abstract

One of the thermal oxidation technologies recommended by the United Nations Environment Programme (UNEP) is destruction of chlorofluorocarbons (CFCs) in a cement kiln. The destruction of CFC12, CFC11 and CFC113 was studied in a cement kiln plant in actual commercial operation. CFCs were completely destroyed in the kiln under normal operating conditions. Hydrogen fluoride and hydrogen chloride generated by CFC decomposition were absorbed by cement materials. No formation of toxic ha-logenated organic compounds, such as polychlorinated dibenzo-p-dioxins or dibenzofurans (PCDDs/PCDFs), was observed in the CFC incineration.     

Observed trends in ambient concentrations of C2–C8 hydrocarbons in the United Kingdom over the period from 1993 to 2004

Hourly measurements of up to 26 C₂–C₈ hydrocarbons have been made at eight urban background sites, three urban-industrial sites, a kerbside and a rural site in the UK from 1993 onwards up until the end of December 2004. Average annual mean benzene and 1,3-butadiene concentrations at urban background locations have declined at about −20% per year and the observed declines have exactly mimicked the inferred declines in benzene and 1,3-butadiene emissions over the same period. Ninety-day rolling mean concentrations of ethylene, propylene, n- and i-butane, n- and i-pentane, isoprene and propane at urban and rural sites have also declined steadily by between −10% and −30% per year. Rolling mean concentrations of acetylene, 2- and 3-methylpentane, n-hexane, n-heptane, cis- and trans-but-2-ene, cis- and trans-pent-2-ene, toluene, ethylbenzene and o-, m- and p-xylene at a roadside location in London have all declined at between −14% and −21% per year. These declines demonstrate that motor vehicle exhaust catalysts and evaporative canisters have effectively and efficiently controlled vehicular emissions of hydrocarbons in the UK. Urban ethane concentrations arising largely from natural gas leakage have remained largely unchanged over this same period.     

Decomposition of organohalogen compounds in municipal solid waste incineration plants. Part I: Chlorofluorocarbons

Disposal of chlorofluorocarbons in a municipal solid waste incinerator has been studied. Destruction of CFC-11 (trichloromonofluoromethane) and CFC-113 (trichlorotrifluoroethane) was found to be better than 99.9%. Neither emission limits for hydrogen chloride or hydrogen fluoride specified in the 17^th BImSchV are exceeded during CFC incineration nor could formation of toxic halogenated organic compounds like dibenzo-p-dioxins or dibenzofurans be observed.     

Spatial variation of airborne pollutant concentrations in Brisbane,Australia and its potential impact on population exposure assessment

Spread of air pollution sources and non-uniform mixing conditions in urban or regional air sheds often result in spatial variation of pollutant concentrations over different parts of the air sheds. A comprehensive understanding of this variation of concentrations is imperative for informed planning, monitoring and assessment in a range of critical areas including assessment of monitoring network efficiency or assessment of population exposure variation as a function of the location in the city. The aims of this work were to study the citywide variability of pollutants as measured by “urban background” type monitoring stations and to interpret the results in relation to the applicability of the data to population exposure assessments and the network efficiency. A comparison between ambient concentrations of NO_x, ozone and PM₁₀ was made for three stations in the Brisbane air shed network. The best correlated between the three stations were ozone concentrations followed by NO_x concentration, with the worst correlations observed for PM₁₀. With a few exceptions correlations of all pollutants between the stations were statistically significant. Marginally better were the correlations for the lower concentrations of pollutants that represent urban background, over the correlations for higher concentrations, representing peak values. Implications of these findings on application of the monitoring data to air-quality management, as well as the need for further investigations has been discussed.     

An empirical model for predicting urban roadside nitrogen dioxide concentrations in the UK

An annual mean concentration of 40 μg m⁻³ has been proposed as a limit value within the European Union Air Quality Directives and as a provisional objective within the UK National Air Quality Strategy for 2010 and 2005, respectively. Emissions reduction measures resulting from current national and international policies are likely to deliver significant reductions in emissions of oxides of nitrogen from road traffic in the near future. It is likely that there will still be exceedances of this target value in 2005 and in 2009 if national measures are considered in isolation, particularly at the roadside. It is envisaged that this `policy gap’ will be addressed by implementing local air quality management to reduce concentrations in locations that are at risk of exceeding the objective. Maps of estimated annual mean NO₂ concentrations in both urban background and roadside locations are a valuable resource for the development of UK air quality policy and for the identification of locations at which local air quality management measures may be required. Maps of annual mean NO₂ concentrations at both background and roadside locations for 1998 have been calculated using modelling methods, which make use of four mathematically straightforward, empirically derived linear relationships. Maps of projected concentrations in 2005 and 2009 have also been calculated using an illustrative emissions scenario. For this emissions scenario, annual mean urban background NO₂ concentrations in 2005 are likely to be below 40 μg m⁻³, in all areas except for inner London, where current national and international policies are expected to lead to concentrations in the range 40–41 μg m⁻³. Reductions in NO_x emissions between 2005 and 2009 are expected to reduce background concentrations to the extent that our modelling results indicate that 40 μg m⁻³ is unlikely to be exceeded in background locations by 2009. Roadside NO₂ concentrations in urban areas in 2005 and 2009 are expected to be significantly higher than in background locations. 21% of urban major road links are expected to have roadside NO₂ greater than or equal to 40 μg m⁻³ in 2005 for our illustrative emissions scenario. The continuing downward trend in traffic emissions is likely to further reduce the number of links exceeding this value by 2009, with about 6% of urban major road links predicted to have concentrations higher than 40 μg m⁻³. The majority of these links are in the London area. The remaining links are generally confined to the most heavily trafficked roads in other big cities.     

A semi-empirical model for urban PM10 concentrations,and its evaluation against data from an urban measurement network

We have developed a model for evaluating the mass-based concentrations of urban particulate matter. The basic model assumption is that local vehicular traffic is responsible for a substantial fraction of the street-level concentrations of both PM₁₀ and NO_x, either due to primary emissions or resuspension from street surfaces. The modelling system utilises the data from an air quality monitoring network in the Helsinki Metropolitan Area. We have determined linear relationships between the measured urban PM₁₀ data against those of NO_x in various urban surroundings, based on continuously measured hourly concentration values. The data was obtained from two stations in central Helsinki and one suburban station in the Helsinki Metropolitan Area during a period of 3 yr, from 1996 to 1998. The model also includes a treatment of the regional background concentrations, and resuspended particulate matter. The model performance was evaluated against the measured PM₁₀ data from the above-mentioned three stations and from two other stations, using data that was measured in 1999. We used two alternative model versions, one based on separate correlation parameters (PM₁₀ vs. NO_x) for each station, and another based on parameters averaged over the stations considered. We analysed the agreement between the measured and predicted hourly concentration time series, utilising the values of the fractional bias (FB) and the so-called index of agreement (IA). As expected, the model predicts relatively well the yearly mean concentrations of PM₁₀: the FB values range from −0.05 to +0.09. Model performance is also relatively good when predicting the yearly mean values that are classified separately for each hour of the day: the corresponding IA values range from 0.85 to 0.96. However, model performance is substantially worse in predicting the hourly time series of the year: the IA values using the station-specific parameters range from 0.46 to 0.65. The model was applied in evaluating the yearly average spatial concentration distribution of PM₁₀ in central Helsinki, based on the corresponding modelled NO_x concentrations. With re-evaluation of a few parameters that can be determined empirically, the model could be evaluated, and most probably applied, in other urban areas as well.     

Ten years measuring PCDDs/PCDFs in ambient air in Catalonia (Spain)

This work summarizes the results of a ten year surveillance programme on PCDD/F in ambient air carried out in Catalonia (Spain). The study has been conducted by the Dioxin Laboratory of Spanish Council for Scientific Research (CSIC) in collaboration with the Environment Department of the Catalonian Government. 175 samples have been collected throughout Catalonia from 1994 to 2004. Different sampling locations classified as industrial, traffic, urban, suburban and rural sites have been monitored in order to find the most contaminated zones as well as the ones with expected background concentrations. The highest concentrations found in this study were determined at the industrial locations. Concentrations ranging from 5 to 1196 fg I-TEQ/m3, with a mean value of 140 fg I-TEQ/m3 and from 10 to 357 fg I-TEQ/m3, with a mean value of 72 fg I-TEQ/m3 were determined in industrial and traffic sampling points, respectively. In contrast, the lowest concentrations were found in rural stations, ranging from 5 to 45 fg I-TEQ/m3, with a mean value of 28 fg I-TEQ/m3. The PCDD/F concentration trend in Catalonian ambient air shown a clear drop of the median values occurred during the study sampling period. A decline of about 70% was observed from 1997-1998 to 2003-2004.     

A Thermal Desorption Procedure for Determining Residual Blowing Agent (CFC-11) in Rigid Foam

A method for measuring the cell gas content in rigid foams has been developed. A unique foam extraction device and a thermal desorption system were developed to expedite gas extraction and analysis. CFC-11 found by this method was in excellent agreement with the calculated value in a commercially formulated foam (7.1 versus 7.8 percent). Average method precision (i.e., relative standard deviation) from processing nine foam samples (in duplicate) was 1.9 percent. The method has also been successfully applied to foams containing non-GFC blowing agents.     

PM2.5 concentrations in London for 2008–A modeling analysis of contributions from road traffic

We report on the analysis of contributions from road traffic emissions to fine particulate matter (PM_2.5) concentrations within London for 2008 with the OSCAR Air Quality Assessment System. A spatiotemporal evaluation of the OSCAR system has been conducted with measurements from the London air quality network (LAQN). For the predicted and measured hourly time series of concentrations at 18 sites in London, the medians of correlation, mean absolute error, index of agreement, and factor of two (FAC2) of all stations were 0.80, 4.1 μg/m³, 0.86, and 74%, respectively. Spatial evaluation of modeled and observed annual mean concentrations also showed a fairly good agreement, with all the values falling within the FAC2 range. According to model predictions, the urban increment (including the contributions from urban traffic and other urban sources) was evaluated to be on the average 18%, 33%, 39%, and 43% of the total PM_2.5 in suburban environments, in the urban background, near roads, and near busy roads, respectively. However, the highest values of the urban traffic increment can be around 50% of the total PM_2.5 concentrations near motorways and major roads. The total concentrations (including regional background, and the contributions from urban traffic and other urban sources) can therefore be almost three times the regional background. The total urban increment close to busy roads was around 7–8 μg/m³, in which the estimated traffic contribution is more than 2 μg/m³. On the average, urban traffic contributes approximately 1 μg/m³ of PM_2.5 to the urban background across London. According to modeling, approximately two-thirds of the traffic increment originated from exhaust emissions and most of the rest was due to brake and tire wear.

Implications: The urban increment and traffic contribution to the total PM_2.5 are significant and spatially heterogeneous across London. The highly heterogeneous distribution of PM_2.5 hence requires detailed modeling studies to be carried out at high spatial resolution, which can be particularly important for exposure and health impact assessment. This type of information can be used to quantify health impacts resulting from specific sources of PM_2.5 such as traffic emissions, to aid city and national decision makers when formulating pollution control strategies.