Measurement of black carbon aerosols near two Chinese megacities and the implications for improving emission inventories

Knowledge of the distribution and sources of black carbon (BC) is essential to understanding its impact on radiative forcing and the establishment of a control strategy. In this study, we analyze atmospheric BC and its relationships with fine particles (PM_2.5) and trace gases (CO, NO_y and SO₂) measured in the summer of 2005 in two areas frequently influenced by plumes from Beijing and Shanghai, the two largest cities in China. The results revealed different BC source characteristics for the two megacities. The average concentration of BC was 2.37 (±1.79) and 5.47 (±4.00) μg m^?3, accounting for 3.1% and 7.8% of the PM_2.5 mass, in Beijing and Shanghai, respectively. The good correlation between BC, CO and NO_y (R² = 0.54–0.77) and the poor correlation between BC and SO₂ suggest that diesel vehicles and marine vessels are the dominant sources of BC in the two urban areas during summer. The BC/CO mass ratio in the air mass from Shanghai was found to be much higher than that in the air mass from Beijing (0.0101 versus 0.0037 ΔgBC/ΔgCO), which is attributable to a larger contribution from diesel burning (diesel-powered vehicles and marine vessels) in Shanghai. Based on the measured ratios of BC/CO and annual emissions of CO, we estimate that the annual emissions of BC in Beijing and Shanghai are 9.51 Gg and 18.72 Gg, respectively. The improved emission rates of BC will help reduce the uncertainty in the assessment of the impact of megacities on regional climate.     

Trends,temporal and spatial characteristics,and uncertainties in biomass burning emissions in the Pearl River Delta,China

Multi-year inventories of biomass burning emissions were established in the Pearl River Delta (PRD) region for the period 2003–2007 based on the collected activity data and emission factors. The results indicated that emissions of sulfur dioxide (SO₂), nitrogen oxide (NO_x), ammonia (NH₃), methane (CH₄), organic carbon (OC), non-methane volatile organic compounds (NMVOC), carbon monoxide (CO), and fine particulate matter (PM_2.5) presented clear declining trends. Domestic biofuel burning was the major contributor, accounting for more than 60% of the total emissions. The preliminary temporal profiles were established with MODIS fire count information, showing that higher emissions were observed in winter (from November to March) than other seasons. The emissions were spatially allocated into grid cells with a resolution of 3 km × 3  km, using GIS-based land use data as spatial surrogates. Large amount of emissions were observed mostly in the less developed areas in the PRD region. The uncertainties in biomass burning emission estimates were quantified using Monte Carlo simulation; the results showed that there were higher uncertainties in organic carbon (OC) and elemental carbon (EC) emission estimates, ranging from ?71% to 133% and ?70% to 128%, and relatively lower uncertainties in SO₂, NO_x and CO emission estimates. The key uncertainty sources of the developed inventory included emission factors and parameters used for estimating biomass burning amounts.     

Anthropogenic emissions of SO2 and NOx in Asia: Emission inventories

The anthropogenic emissions of SO₂ and NO_x for 25 Asian countries east of Afghanistan and Pakistan have been calculated for 1975, 1980, 1985, 1986 and 1987 based on fuel consumption, sulfur content in fuels and emission factors for used fuels in each emission category. The provincial- and regional-based calculations have also been made for China and India. The total SO₂ emissions in these parts of Asia have been calculated to be 18.3 and 29.1 Tg in 1975 and 1987, respectively. The calculated total NO_x emissions were 9.4 and 15.5 Tg in 1975 and 1987, respectively. The SO₂ and NO_x emissions in East Asia (China, Japan, South Korea, North Korea and Taiwan) were 23.4 and 10.7 Tg in 1975 and 1987, respectively.Keyword: Emission inventories, sulfur dioxide emissions, nitrogen oxide emissions, Asian emissions, anthropogenic emissions.     

Emissions profile from new and in-use handheld, 2-stroke engines

The objective of this study was to characterize exhaust emissions from a series of handheld, 2-stroke small engines. A total of 23 new and used engines from model years 1981–2003 were studied; these engines spanned three phases of emission control (pre-control, phase-1, phase-2). Measured emissions included carbon monoxide (CO), carbon dioxide (CO₂), nitrogen oxides (NO_x), hydrocarbons (HC), fine particulate matter (PM_2.5), and sulfur dioxide (SO₂). Emissions reductions in CO (78%) and HC (52%) were significant between pre-control and phase-2 engines. These reductions can be attributed to improvements in engine design, reduced scavenging losses, and implementation of catalytic exhaust control. Total hydrocarbon emissions were strongly correlated with fuel consumption rates, indicating varying degrees of scavenging losses during the intake/exhaust stroke. The use of a reformulated gasoline containing 10% ethanol resulted in a 15% decrease in HC and a 29% decrease in CO emissions, on average. Increasing oil content of 2-stroke engine fuels results in a substantial increase of PM_2.5 emissions as well as smaller increases in HC and CO emissions. Results from this study enhance existing emission inventories and appear to validate predicted improvements to ambient air quality through implementation of new phase-2 handheld emission standards.     

Estimating Future NO2 Levels in the Greater Los Angeles Area by Source–Type Contribution

Two indicator pollutants, carbon monoxide (CO) for mobile source influence and sulfur dioxide (SO₂) for stationary source influence, were used to estimate source-type contributions to ambient NO₂ levels in a base year and to predict NO₂ concentrations in a future year. For a specific source-receptor pair, the so-called influence coefficient of each of three source categories (mobile sources, power plants, and other stationary sources) was determined empirically from concurrent measurements of CO and SO₂ concentrations at the receptor site and CO and SO₂ emissions from each source category in the source area. Those coefficients, which are considered time invariant, were used in conjunction with the base year and future year NO _x emission values to estimate source-type contribution to ambient NO₂ levels at seven study sites selected from the Greater Los Angeles area for both the base year period, 1974 through 1976, and the future goal year of 1987 in which the air quality standards for NO₂ are to be attained. The estimated NO₂ air quality at the seven sites is found to meet the national annual standard of 5 pphm and over 99.9% of total hours, the California 1-hr NO₂ standard of 25 pphm in 1987. The estimated power plant contributions to ambient NO₂ levels are found to be considerably smaller than those to total NO _x emissions in the area. Providing that reasonably complete air quality and emissions data are available, the present analysis method may prove to be a useful tool in evaluating source contributions to both short-term peak and long-term average NO₂ concentrations for use in control strategy development.     

Spatial and temporal variations in PM10 and PM2.5 source contributions and comparison to emissions during the 1995 integrated monitoring study

The ambient PM₁₀ and PM_2.5 data collected during the fall and winter portions of the 1995 Integrated Monitoring Study (IMS95) were used to conduct Chemical Mass Balance (CMB) Modeling to determine source contribution estimates. Data from the core and saturation monitoring sites provided an extensive database for evaluating the spatial and temporal variations of contributing sources. Geological sources dominated fall samples, while secondary ammonium nitrate and carbonaceous sources were the largest contributors for winter samples. Secondary ammonium nitrate concentrations were uniform across all sites during both the fall and winter. Site-to-site variability was primarily due to differences in geological contributions in the fall, and carbonaceous source contributions in the winter. During the winter, diurnal profiles of particulate matter (PM) were driven by variations in carbonaceous sources at urban sites, and by variations in secondary ammonium nitrate at rural sites. Although records of day-specific PM activities were recorded during the study, no correlation was observed between 24-h CMB results and specific activities. The ambient data collected during IMS95 was also used to evaluate the adequacy of the emissions inventory. Comparison of ambient and emissions based ratios of NMHC/NO_x, PM/NO_x, CO/NO_x, and SO_x/NO_x suggested that emissions of NMHC and CO in some locations may be underestimated, while emissions for PM and SO_x may be overestimated. Comparison of fractional primary CMB source contribution estimates to corresponding fractional emissions estimates indicated that geological sources were overemphasized in the inventory, while carbonaceous sources were underrepresented.     

Emission Factors for High-Emitting Vehicles Based on On-Road Measurements of Individual Vehicle Exhaust with a Mobile Measurement Platform

ABSTRACT

Fuel-based emission factors for 143 light-duty gasoline vehicles (LDGVs) and 93 heavy-duty diesel trucks (HDDTs) were measured in Wilmington, CA using a zero-emission mobile measurement platform (MMP). The frequency distributions of emission factors of carbon monoxide (CO), nitrogen oxides (NO_x), and particle mass with aerodynamic diameter below 2.5 μm (PM_2.5) varied widely, whereas the average of the individual vehicle emission factors were comparable to those reported in previous tunnel and remote sensing studies as well as the predictions by Emission Factors (EMFAC) 2007 mobile source emission model for Los Angeles County. Variation in emissions due to different driving modes (idle, low- and high-speed acceleration, low- and high-speed cruise) was found to be relatively small in comparison to intervehicle variability and did not appear to interfere with the identification of high emitters, defined as the vehicles whose emissions were more than 5 times the fleet-average values. Using this definition, approximately 5% of the LDGVs and HDDTs measured were high emitters. Among the 143 LDGVs, the average emission factors of NO_x, black carbon (BC), PM_2.5, and ultrafine particle (UFP) would be reduced by 34%, 39%, 44%, and 31%, respectively, by removing the highest 5% of emitting vehicles, whereas CO emission factor would be reduced by 50%. The emission distributions of the 93 HDDTs measured were even more skewed: approximately half of the NO_x and CO fleet-average emission factors and more than 60% of PM_2.5, UFP, and BC fleet-average emission factors would be reduced by eliminating the highest-emitting 5% HDDTs. Furthermore, high emissions of BC, PM_2.5, and NO_x tended to cluster among the same vehicles.

IMPLICATIONS This study presents the characterization of on-road vehicle emissions in Wilmington, CA, by sampling individual vehicle plumes. Approximately 5% of the vehicles were high emitters, whose emissions were more than 5 times the fleet-average values. These high emitters were responsible for 30% and more than 50% of the average emission factors of LDGVs and HDDVs, respectively. It is likely that as the overall fleet becomes cleaner due to more stringent regulations, a small fraction of the fleet may contribute a growing and disproportionate share of the overall emissions. Therefore, long-term changes in on-road emissions need to be monitored.     

A Comprehensive Inventory of the Ship Traffic Exhaust Emissions in the Baltic Sea from 2006 to 2009

This study addresses the exhaust emissions of CO₂, NO_x, SO_x, CO, and PM_2.5 originated from Baltic Sea shipping in 2006–2009. Numerical results have been computed using the Ship Traffic Emissions Assessment Model. This model is based on the messages of the automatic identification system (AIS), which enable the positioning of ships with a high spatial resolution. The NO_x emissions in 2009 were approximately 7 % higher than in 2006, despite the economic recession. However, the SO_x emissions in 2009 were approximately 14 % lower, when compared to those in 2006, mainly caused by the fuel requirements of the SO_x emission control area (SECA) which became effective in May 2006, but affected also by changes in ship activity. Results are presented on the differential geographic distribution of shipping emissions before (Jan–April 2006) and after (Jan–April 2009) the SECA regulations. The predicted NO_x emissions in 2009 substantially exceeded the emissions in 2006 along major ship routes and at numerous harbors, mostly due to the continuous increase in the number of small vessels that use AIS transmitters. Although the SO_x emissions have been reduced in 2009 in most major ship routes, these have increased in the vicinity of some harbors and on some densely trafficked routes. A seasonal variation of emissions is also presented, as well as the distribution of emissions in terms of vessel flag state, type, and weight.     

A highly resolved temporal and spatial air pollutant emission inventory for the Pearl River Delta region, China and its uncertainty assessment

A highly resolved temporal and spatial Pearl River Delta (PRD) regional emission inventory for the year 2006 was developed with the use of best available domestic emission factors and activity data. The inventory covers major emission sources in the region and a bottom–up approach was adopted to compile the inventory for those sources where possible. The results show that the estimates for SO₂, NO_x, CO, PM₁₀, PM_2.5 and VOC emissions in the PRD region for the year 2006 are 711.4 kt, 891.9 kt, 3840.6 kt, 418.4 kt, 204.6 kt, and 1180.1 kt, respectively. About 91.4% of SO₂ emissions were from power plant and industrial sources, and 87.2% of NO_x emissions were from power plant and mobile sources. The industrial, mobile and power plant sources are major contributors to PM₁₀ and PM_2.5 emissions, accounting for 97.7% of the total PM₁₀ and 97.2% of PM_2.5 emissions, respectively. Mobile, biogenic and VOC product-related sources are responsible for 90.5% of the total VOC emissions. The emissions are spatially allocated onto grid cells with a resolution of 3 km × 3 km, showing that anthropogenic air pollutant emissions are mainly distributed over PRD central-southern city cluster areas. The preliminary temporal profiles were established for the power plant, industrial and on-road mobile sources. There is relatively low uncertainty in SO₂ emission estimates with a range of −16% to +21% from power plant sources, medium to high uncertainty for the NO_x emissions, and high uncertainties in the VOC, PM_2.5, PM₁₀ and CO emissions.     

Estimation of vehicular emission inventories in China from 1980 to 2005

Multi-year inventories of vehicular emissions at a high spatial resolution of 40 km×40 km were established in China using the GIS methodology for the period 1980–2005, based on provincial statistical data from yearbooks regarding vehicles and roads, and on the emission factors for each vehicle category in each province calculated by COPERT III program. Results showed that the emissions of CH₄, CO, CO₂, NMVOC, NO_x, PM₁₀, and SO₂ increased from 5, 1066, 19 893, 169, 174, 26, and 16 thousand tons in 1980 to 377, 36 197, 674 629, 5911, 4539, 983, and 484 thousand tons in 2005 at an annual average rate of 19%, 15%, 15%, 15%, 14%, 16%, and 15%, respectively. Statistical analysis of vehicular emissions and GDP showed that they were well positively correlated, which revealed that increase of pollutant emissions has been accompanying the growth of GDP. Spatial distribution of pollutant emissions was rather unbalanced: over three-quarters of the total emissions concentrated in developed regions of China's southeastern, northern and central areas covering only 35.2% of China's territory, while the remaining emissions were distributed over the southwestern, northwestern and northeastern regions covering as much as 64.8% of the territory. In 2005, the Beijing–Tianjin–Hebei region, the Yangtze River Delta, and the Pearl River Delta covering only 2.3%, 2.2%, and 1.9%, respectively, of the territory, generated about 10%, 19%, and 12%, respectively, of the total emissions. Since 1990, motorcycles have been the major contributors to the CH₄, CO, NMVOC, and PM₁₀ emissions, due to the large population. Heavy-duty vans were the major contributors to the NO_x and SO₂ emissions because of high emission factors. Passenger cars contributed about one third of the emissions of each pollutant. Contributions of vehicle categories to emissions varied from province to province, due to the diversity of vehicle compositions among provinces.     

Emissions from India's transport sector: Statewise synthesis

A decentralized emission inventories are prepared for road transport sector of India in order to design and implement suitable technologies and policies for appropriate mitigation measures. Globalization and liberalization policies of the government in 90's have increased the number of road vehicles nearly 92.6% from 1980–1981 to 2003–2004. These vehicles mainly consume non-renewable fossil fuels, and are a major contributor of green house gases, particularly CO₂ emission. This paper focuses on the statewise road transport emissions (CO₂, CH₄, CO, NO_x, N₂O, SO₂, PM and HC), using region specific mass emission factors for each type of vehicles. The country level emissions (CO₂, CH₄, CO, NO_x, N₂O, SO₂ and NMVOC) are calculated for railways, shipping and airway, based on fuel types. In India, transport sector emits an estimated 258.10 Tg of CO₂, of which 94.5% was contributed by road transport (2003–2004). Among all the states and Union Territories, Maharashtra's contribution is the largest, 28.85 Tg (11.8%) of CO₂, followed by Tamil Nadu 26.41 Tg (10.8%), Gujarat 23.31 Tg (9.6%), Uttar Pradesh 17.42 Tg (7.1%), Rajasthan 15.17 Tg (6.22%) and, Karnataka 15.09 Tg (6.19%). These six states account for 51.8% of the CO₂ emissions from road transport.     

Real-world emissions of in-use off-road vehicles in Mexico

Off-road vehicles used in construction and agricultural activities can contribute substantially to emissions of gaseous pollutants and can be a major source of submicrometer carbonaceous particles in many parts of the world. However, there have been relatively few efforts in quantifying the emission factors (EFs) and for estimating the potential emission reduction benefits using emission control technologies for these vehicles. This study characterized the black carbon (BC) component of particulate matter and NOx, CO, and CO₂ EFs of selected diesel-powered off-road mobile sources in Mexico under real-world operating conditions using on-board portable emissions measurements systems (PEMS). The vehicles sampled included two backhoes, one tractor, a crane, an excavator, two front loaders, two bulldozers, an air compressor, and a power generator used in the construction and agricultural activities. For a selected number of these vehicles the emissions were further characterized with wall-flow diesel particle filters (DPFs) and partial-flow DPFs (p-DPFs) installed. Fuel-based EFs presented less variability than time-based emission rates, particularly for the BC. Average baseline EFs in working conditions for BC, NOx, and CO ranged from 0.04 to 5.7, from 12.6 to 81.8, and from 7.9 to 285.7 g/kg-fuel, respectively, and a high dependency by operation mode and by vehicle type was observed. Measurement-base frequency distributions of EFs by operation mode are proposed as an alternative method for characterizing the variability of off-road vehicles emissions under real-world conditions. Mass-based reductions for black carbon EFs were substantially large (above 99%) when DPFs were installed and the vehicles were idling, and the reductions were moderate (in the 20–60% range) for p-DPFs in working operating conditions. The observed high variability in measured EFs also indicates the need for detailed vehicle operation data for accurately estimating emissions from off-road vehicles in emissions inventories.

Implications: Measurements of off-road vehicles used in construction and agricultural activities in Mexico using on-board portable emissions measurements systems (PEMS) showed that these vehicles can be major sources of black carbon and NO_X. Emission factors varied significantly under real-world operating conditions, suggesting the need for detailed vehicle operation data for accurately estimating emissions inventories. Tests conducted in a selected number of sampled vehicles indicated that diesel particle filters (DPFs) are an effective technology for control of diesel particulate emissions and can provide potentially large emissions reduction in Mexico if widely implemented.     

Estimation of road vehicle exhaust emissions from 1992 to 2010 and comparison with air quality measurements in Genoa,Italy

An investigation into road transport exhaust emissions in the Genoa urban area was performed by comparing the quantities of carbon monoxide (CO), nitrogen oxides (NO_x), nitrogen dioxide (NO₂) and particulate matter (PM) emitted by different vehicle categories with air quality measurements referred to the same pollutants. Exhaust emissions were evaluated by applying the PROGRESS (computer PROGramme for Road vehicle EmiSSions evaluation) code, developed by the Internal Combustion Engines Group of the University of Genoa, to eight different years (from 1992 to 2010), considering spark ignition and Diesel passenger cars and light duty vehicles, heavy duty vehicles and buses, motorcycles and mopeds. Changes in terms of vehicles number, mileage and total emissions are presented together with relative distributions among the various vehicle categories. By comparing 1992 and 2010 data, calculated trends show a 7% increase in the number of vehicles, with total mileage growing at a faster rate (approx. 22%); total emissions decrease considerably, by approximately 50% for NO_x and PM, 70% for HC and 80% for CO, due to improvements in engines and fuels forced by the stricter European legislation and the fleet renewal, while primary NO₂ emission will be very close to 1992 level, after a decrease of about 18% in 2000.Air quality was analysed by selecting traffic and background measuring stations from the monitoring network managed by the Environmental Department of the Province of Genoa: average annual concentrations of considered pollutants from 1994 to 2007 were calculated in order to obtain the relative historical trends and compare them with European public health limits and with road vehicle emissions. Though an important reduction in pollutant concentrations has been achieved as a consequence of cleaner vehicles, some difficulties in complying with present and/or future NO₂ and PM₁₀ limits are also apparent, thus requiring suitable measures to be taken by the local authorities.     

Sub-region (district) and sector level SO2 and NOx emissions for India: assessment of inventories and mitigation flexibility

Sub-regional and sector level distribution of SO₂ and NO_x emissions inventories for India have been estimated for all the 466 Indian districts using base data for years 1990 and 1995. Although, national level emissions provide general guidelines for assessing mitigation alternatives, but significant regional and sectoral variability exist in Indian emissions. Districts reasonably capture this variability to a fine grid as 80% of these districts are smaller than 1°×1° resolution with 60% being smaller than even 1/2°×1/2°. Moreover, districts in India have well-established administrative and institutional mechanisms that would be useful for implementing and monitoring measures. District level emission estimates thus offer a finer regional scale inventory covering the combined interests of the scientific community and policy makers. The inventory assessment methodology adopted is similar to that prescribed by the Intergovernmental Panel on Climate Change (IPCC) for greenhouse gas (GHG) emissions. The sectoral decomposition at district level includes emissions from fossil fuel combustion, non-energy emissions from industrial activities and agriculture. Total SO₂ and NO_x emissions from India were 3542 and 2636 Gg, respectively (1990) and 4638 and 3462 Gg (1995) growing at annual rate of around 5.5%. The sectoral composition of SO₂ emissions indicates a predominance of electric power generation sector (46%). Power and transport sector emissions equally dominate NO_x emissions contributing nearly 30% each. However, majority of power plants are situated in predominantly rural districts while the latter are concentrated in large urban centers. Mitigation efforts for transport sector NO_x emissions would therefore be higher. The district level analysis indicates diverse spatial distribution with the top 5% emitting districts contributing 46.5 and 33.3% of total national SO₂ and NO_x emissions, respectively. This skewed emission pattern, with a few districts, sectors and point sources emitting significant SO₂ and NO_x, offers mitigation flexibility to policy makers for cost-effective mitigation.     

On-road remote sensing measurements and fuel-based motor vehicle emission inventory in Hangzhou,China

Motor vehicles are one of the largest sources of air pollutants worldwide. Despite their importance, motor vehicle emissions are inadequately understood and quantified, esp. in developing countries. In this study, the real-world emissions of carbon monoxide (CO), hydrocarbons (HC) and nitrogen oxide (NO) were measured using an on-road remote sensing system at five sites in Hangzhou, China in 2004 and 2005. Average emission factors of CO, HC and NO_x for petrol vehicles of different model year, technology class and vehicle type were calculated in grams of pollutant per unit of fuel use (g l⁻¹) from approximately 32,260 petrol vehicles. Because the availability of data used in traditional on-road mobile source estimation methodologies is limited in China, fuel-based approach was implemented to estimate motor vehicle emissions using fuel sales as a measure of vehicle activity, and exhaust emissions factors from remote sensing measurements. The fuel-based exhaust emission inventories were also compared with the results from the recent international vehicle emission (IVE) model. Results show that petrol vehicle fleet in Hangzhou has significantly high CO emissions, relatively high HC and low NO_x, with the average emission factors of 193.07±15.63, 9.51±2.40 and 5.53±0.48 g l⁻¹, respectively. For year 2005 petrol vehicles exhaust emissions contributed with 182,013±16,936, 9107±2255 and 5050±480 metric ton yr⁻¹ of CO, HC and NO_x, respectively. The inventories are 45.5% higher, 6.6% higher and 53.7% lower for CO, HC and NO_x, respectively, than the estimates using IVE travel-based model. In addition, a number of insights about the emission distributions and formation mechanisms have been obtained from an in-depth analysis of these results.     

Characteristics of gaseous pollutants from biofuel-stoves in rural China

The research team analyzed the emission characteristics of gaseous pollutants, including volatile organic compounds (VOCs), from biomass combustion in improved stoves in rural China. The research included measurements from five biofuels and two stove types in the months of January, April, and September. The measurements were conducted according to U.S. EPA Method 25 using a collection system with a cooling device and two-level filters. CO, CO₂, NO_x, CH₄ and THC analyzers were used for in-field, real-time emission measurements. The emission data indicate that gaseous pollutants were emitted at higher concentrations in the early combustion stage and lower concentrations in the later stage. CH₄ and THC, as well as CO and CO₂, presented positive relationships during the whole entire combustion process for all tests. The chemical profiles of flue gas samples were analyzed by GC/MS and GC/FID/ECD. Aromatics, carbonyls, and alkenes & alkynes dominated the VOC emissions, respectively accounting for 37%, 33%, and 23% of total VOC emissions by volume. Benzene was the most abundant VOC species, consisting of 17.3 ± 8.1% of VOCs, followed by propylene (11.3 ± 3.5%), acetone (10.8 ± 8.2%), toluene (7.3 ± 5.7%) and acetaldehyde (6.5 ± 7.3%). Carbon mass balance approach was applied to calculate CO, CO₂, CH₄, NO_x, and VOC species emission factors. This analysis includes a discussion of the differences among VOC emission factors of different biofuel-stove combinations.     

Current and future emission estimates of exhaust gases and particles from shipping at the largest port in Korea

The emissions of exhaust gases (NO _x , SO₂, VOCs, and CO₂) and particles (e.g., PM) from ships traversing Busan Port in Korea were estimated over three different years (the years 2006, 2008, and 2009). This analysis was performed according to the ship operational modes (“at sea,” “maneuvering,” and “in port”) and ship types based on an activity-based method. The ship emissions for current (base year 2009) and future scenarios (years 2020 and 2050) were also compared. The annual emissions of SO₂, VOCs, PM, and CO₂ were highest (9.6?×?10³, 374, 1.2?×?10³, and 5.6?×?10⁵ ton year^?1, respectively) in 2008. In contrast, the annual NO _x emissions were highest (11.7?×?10³ ton year^?1) in 2006 due mainly to the high NO _x emission factor. The emissions of air pollutants for each ship operational mode differed considerably, with the largest emission observed in “in port” mode. In addition, the largest fraction (approximately 45–67 %) of the emissions of all air pollutants during the study period was emitted from container ships. The future ship emissions of most pollutants (except for SO₂ and PM) in 2020 and 2050 are estimated to be 1.4–1.8 and 4.7–6.1 times higher than those in 2009 (base year), respectively.     

Spatiotemporal analysis of traffic emissions in over 5000 municipal districts in Brazil

Exposure to traffic emission is harmful to human health. Emission inventories are essential to public health policies aiming at protecting human health, especially in areas with incomplete or nonexistent air pollution monitoring networks. In Brazil, for example, only 1.7% of municipal districts have a monitoring network, and only a few studies have reported data on vehicle emission inventories. No studies have presented emission inventories by municipality. In this study, we predicted vehicular emissions for 5570 municipal districts in Brazil during the period 2001–2012. We used a top-down method to estimate emissions. Carbon dioxide (CO₂) is the pollutant with the highest emissions, with approximately 190 million tons per year during the period 2001–2012). For the other traffic-related pollutants, we predicted annual emissions of 1.5 million tons for carbon monoxide (CO), 1.2 million tons of nitrogen oxides (NO_x), 209,000 tons of nonmethane hydrocarbons (NMHC), 58,000 tons of particulate matter (PM), and 42,000 tons for methane (CH₄). From 2001 to 2012, CO, NMHC, and PM emissions decreased by 41, 33, and 47%, respectively, whereas those CH₄, NO_x, and CO₂ increased by 2, 4, and 84%, respectively. We estimated uncertainties in our study and found that NO_x was the pollutant with the lowest percentage difference, 8%, and NMHC with the highest one, 30%. For CO, CH₄, CO₂, and PM, the values were 22, 14, 21, and 20%, respectively. Finally, we found that during 2001 and 2012 emissions increased in the Northwest and Northeast. In contrast, pollutant emissions, except for CO₂, decreased in the Southeast, South, and part of Midwest. Our predictions can be critical to efforts developing cost-effective public policies tailored to individual municipal districts in Brazil.

Implications: Emission inventories may be an alternative approach to provide data for air quality forecasting in areas where air quality data are not available. This approach can be an effective tool in developing spatially resolved emission inventories.     

Aircraft measurements of O3, NOx,CO, VOCs,and SO2 in the Yangtze River Delta region

In this study, air pollutants, including ozone (O₃), nitrogen oxides (NO_x = NO + NO₂), carbon monoxides (CO), sulfur dioxide (SO₂), and volatile organic compounds (VOCs) measured in the Yangtze River Delta (YRD) region during several air flights between September/30 and October/11 are analyzed. This measurement provides horizontal and vertical distributions of air pollutants in the YRD region. The analysis of the result shows that the measured O₃ concentrations range from 20 to 60 ppbv. These values are generally below the US national standard (84 ppbv), suggesting that at the present, the O₃ pollutions are modest in this region. The NO_x concentrations have strong spatial and temporal variations, ranging from 3 to 40 ppbv. The SO₂ concentrations also have large spatial and temporal variations, ranging from 1 to 35 ppbv. The high concentrations of CO are measured with small variations, ranging from 3 to 7 ppmv. The concentrations of VOCs are relatively low, with the total VOC concentrations of less than 6 ppbv. The relative small VOC concentrations and the relative large NO_x concentrations suggest that the O₃ chemical formation is under a strong VOC-limited regime in the YRD region. The measured O₃ and NO_x concentrations are strongly anti-correlated, indicating that enhancement in NO_x concentrations leads to decrease in O₃ concentrations. Moreover, the O₃ concentrations are more sensitive to NO_x concentrations in the rural region than in the city region. The ratios of Δ[O₃]/Δ[NO_x] are ?2.3 and ?0.25 in the rural and in the city region, respectively. In addition, the measured NO_x and SO₂ concentrations are strongly correlated, highlighting that the NO_x and SO₂ are probably originated from same emission sources. Because SO₂ emissions are significantly originated from coal burnings, the strong correlation between SO₂ and NO_x concentrations suggests that the NO_x emission sources are mostly from coal burned sources. As a result, the future automobile increases could lead to rapid enhancements in O₃ concentrations in the YRD region.     

Evaluation of thermal optical analysis method of elemental carbon for marine fuel exhaust

The awareness of black carbon (BC) as the second largest anthropogenic contributor in global warming and an ice melting enhancer has increased. Due to prospected increase in shipping especially in the Arctic reliability of BC emissions and their invented amounts from ships is gaining more attention. The International Maritime Organization (IMO) is actively working toward estimation of quantities and effects of BC especially in the Arctic. IMO has launched work toward constituting a definition for BC and agreeing appropriate methods for its determination from shipping emission sources. In our study we evaluated the suitability of elemental carbon (EC) analysis by a thermal-optical transmittance (TOT) method to marine exhausts and possible measures to overcome the analysis interferences related to the chemically complex emissions. The measures included drying with CaSO_4, evaporation at 40–180ºC, H₂O treatment, and variation of the sampling method (in-stack and diluted) and its parameters (e.g., dilution ratio, Dr). A reevaluation of the nominal organic carbon (OC)/EC split point was made. Measurement of residual carbon after solvent extraction (TC-C_SOF) was used as a reference, and later also filter smoke number (FSN) measurement, which is dealt with in a forthcoming paper by the authors. Exhaust sources used for collecting the particle sample were mainly four-stroke marine engines operated with variable loads and marine fuels ranging from light to heavy fuel oils (LFO and HFO) with a sulfur content range of <0.1–2.4% S. The results were found to be dependent on many factors, namely, sampling, preparation and analysis method, and fuel quality. It was found that the condensed H₂SO₄ + H₂O on the particulate matter (PM) filter had an effect on the measured EC content, and also promoted the formation of pyrolytic carbon (PyC) from OC, affecting the accuracy of EC determination. Thus, uncertainty remained regarding the EC results from HFO fuels.

Implications: The work supports one part of the decision making in black carbon (BC) determination methodology. If regulations regarding BC emissions from marine engines will be implemented in the future, a well-defined and at best unequivocal method of BC determination is required for coherent and comparable emission inventories and estimating BC effects. As the aerosol from marine emission sources may be very heterogeneous and low in BC, special attention to the effects of sampling conditions and sample pretreatments on the validity of the results was paid in developing the thermal-optical analysis methodology (TOT).