[1] We present a global tabulation of black carbon (BC) and primary organic carbon (OC) particles emitted from combustion. We include emissions from fossil fuels, biofuels, open biomass burning, and burning of urban waste. Previous ''bottom-up'' inventories of black and organic carbon have assigned emission factors on the basis of fuel type and economic sector alone. Because emission rates are highly dependent on combustion practice, we consider combinations of fuel, combustion type, and emission controls and their prevalence on a regional basis. Central estimates of global annual emissions are 8.0 Tg for black carbon and 33.9 Tg for organic carbon. These estimates are lower than previously published estimates by 25-35%. The present inventory is based on 1996 fuel-use data, updating previous estimates that have relied on consumption data from 1984. An offset between decreased emission factors and increased energy use since the base year of the previous inventory prevents the difference between this work and previous inventories from being greater. The contributions of fossil fuel, biofuel, and open burning are estimated as 38%, 20%, and 42%, respectively, for BC, and 7%, 19%, and 74%, respectively, for OC. We present a bottom-up estimate of uncertainties in source strength by combining uncertainties in particulate matter emission factors, emission characterization, and fuel use. The total uncertainties are about a factor of 2, with uncertainty ranges of 4.3-22 Tg/yr for BC and 17-77 Tg/yr for OC. Low-technology combustion contributes greatly to both the emissions and the uncertainties. Advances in emission characterization for small residential, industrial, and mobile sources and topdown analysis combining field measurements and transport modeling with iterative inventory development will be required to reduce the uncertainties further.
An inventory of air pollutant emissions in Asia in the year 2000 is developed to support atmospheric modeling and analysis of observations taken during the TRACE‐P experiment funded by the National Aeronautics and Space Administration (NASA) and the ACE‐Asia experiment funded by the National Science Foundation (NSF) and the National Oceanic and Atmospheric Administration (NOAA). Emissions are estimated for all major anthropogenic sources, including biomass burning, in 64 regions of Asia. We estimate total Asian emissions as follows: 34.3 Tg SO2, 26.8 Tg NOx, 9870 Tg CO2, 279 Tg CO, 107 Tg CH4, 52.2 Tg NMVOC, 2.54 Tg black carbon (BC), 10.4 Tg organic carbon (OC), and 27.5 Tg NH3. In addition, NMVOC are speciated into 19 subcategories according to functional groups and reactivity. Thus we are able to identify the major source regions and types for many of the significant gaseous and particle emissions that influence pollutant concentrations in the vicinity of the TRACE‐P and ACE‐Asia field measurements. Emissions in China dominate the signature of pollutant concentrations in this region, so special emphasis has been placed on the development of emission estimates for China. China's emissions are determined to be as follows: 20.4 Tg SO2, 11.4 Tg NOx, 3820 Tg CO2, 116 Tg CO, 38.4 Tg CH4, 17.4 Tg NMVOC, 1.05 Tg BC, 3.4 Tg OC, and 13.6 Tg NH3. Emissions are gridded at a variety of spatial resolutions from 1° × 1° to 30 s × 30 s, using the exact locations of large point sources and surrogate GIS distributions of urban and rural population, road networks, landcover, ship lanes, etc. The gridded emission estimates have been used as inputs to atmospheric simulation models and have proven to be generally robust in comparison with field observations, though there is reason to think that emissions of CO and possibly BC may be underestimated. Monthly emission estimates for China are developed for each species to aid TRACE‐P and ACE‐Asia data interpretation. During the observation period of March/April, emissions are roughly at their average values (one twelfth of annual). Uncertainties in the emission estimates, measured as 95% confidence intervals, range from a low of ±16% for SO2 to a high of ±450% for OC.
[1] Estimates of biomass burning in Asia are developed to facilitate the modeling of Asian and global air quality. A survey of national, regional, and international publications on biomass burning is conducted to yield consensus estimates of ''typical'' (i.e., nonyear-specific) estimates of open burning (excluding biofuels). We conclude that 730 Tg of biomass are burned in a typical year from both anthropogenic and natural causes. Forest burning comprises 45% of the total, the burning of crop residues in the field comprises 34%, and 20% comes from the burning of grassland and savanna. China contributes 25% of the total, India 18%, Indonesia 13%, and Myanmar 8%. Regionally, forest burning in Southeast Asia dominates. National, annual totals are converted to daily and monthly estimates at 1°Â 1°spatial resolution using distributions based on AVHRR fire counts for 1999-2000. Several adjustment schemes are applied to correct for the deficiencies of AVHRR data, including the use of moving averages, normalization, TOMS Aerosol Index, and masks for dust, clouds, landcover, and other fire sources. Good agreement between the national estimates of biomass burning and adjusted fire counts is obtained (R 2 = 0.71-0.78). Biomass burning amounts are converted to atmospheric emissions, yielding the following estimates: 0.37 Tg of SO 2 , 2.8 Tg of NO x , 1100 Tg of CO 2 , 67 Tg of CO, 3.1 Tg of CH 4 , 12 Tg of NMVOC, 0.45 Tg of BC, 3.3 Tg of OC, and 0.92 Tg of NH 3 . Uncertainties in the emission estimates, measured as 95% confidence intervals, range from a low of ±65% for CO 2 emissions in Japan to a high of ±700% for BC emissions in India.
[1] Measurements obtained during the NASA Transport and Chemical Evolution over the Pacific (TRACE-P) experiment are used in conjunction with regional modeling analysis to evaluate emission estimates for Asia. A comparison between the modeled values and the observations is one method to evaluate emissions. Based on such analysis it is concluded that the inventory performs well for the light alkanes, CO, ethyne, SO 2 , and NO x . Furthermore, based on model skill in predicting important photochemical species such as O 3 , HCHO, OH, HO 2 , and HNO 3 , it is found that the emissions inventories are of sufficient quality to support preliminary studies of ozone production. These are important finding in light of the fact that emission estimates for many species (such as speciated NMHCs and BC) for this region have only recently been estimated and are highly uncertain. Using a classification of the measurements built upon trajectory analysis, we compare observed species distributions and ratios of species to those modeled and to ratios estimated from the emissions inventory. It is shown that this technique can reconstruct a spatial distribution of propane/benzene that looks remarkably similar to that calculated from the emissions inventory. A major discrepancy between modeled and observed behavior is found in the Yellow Sea, where modeled values are systematically underpredicted. The integrated analysis suggests that this may be related to an underestimation of emissions from the domestic sector. The emission is further tested by comparing observed and measured species ratios in identified megacity plumes. Many of the model derived ratios (e.g., BC/CO, SO x /C 2 H 2 ) fall within $25% of those observed and all fall outside of a factor of 2.5.
[1] Data obtained during the TRACE-P experiment is used to evaluate how well the CFORS/STEM-2K1 regional-scale chemical transport model is able to represent the aircraft observations. Thirty-one calculated trace gas and aerosol parameters are presented and compared to the in situ data. The regional model is shown to accurately predict many of the important features observed. The mean values of all the model parameters in the lowest 1 km are predicted within ±30% of the observed values. The correlation coefficients (R) for the meteorological parameters are found to be higher than those for the trace species. For example, for temperature, R > 0.98. Among the trace species, ethane, propane, and ozone show the highest values (0.8 < R < 0.9), followed by CO, SO 2 , and NO y . NO and NO 2 had the lowest values (R < 0.4). Analyses of pollutant transport into the Yellow Sea by frontal events are presented and illustrate the complex nature of outflow. Biomass burning from SE Asia is transported in the warm conveyor belt at altitudes above $2 km and at latitudes below 30N. Outflow of pollution emitted along the east coast of China in the postfrontal regions is typically confined to the lower $2 km and results in high concentrations with plume-like features in the Yellow Sea. During these situations the model underpredicts CO and black carbon (among other species). An analysis of ozone production in this region is also presented. In and around the highly industrialized regions of East Asia, where fossil fuel usage dominates, ozone is NMHC-limited. South of $30-35N, ozone production is NO x -limited, reflecting the high NMHC/NO x ratios due to the large contributions to the emissions from biomass burning, biogenics sources, and biofuel usage in central China and SE Asia.
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