27848633
Intercomparison of NO x emission inventories over East Asia
Abstract. We compare nine emission inventories of nitrogen oxides including four satellite-derived NOx inventories and the following bottom-up inventories for East Asia: REAS (Regional Emission inventory in ASia), MEIC (Multi-resolution Emission Inventory for China), CAPSS (Clean Air Policy Support System) and EDGAR (Emissions Database for Global Atmospheric Research). Two of the satellite-derived inventories are estimated by using the DECSO (Daily Emission derived Constrained by Satellite Observations) algorithm, which is based on an extended Kalman filter applied to observations from OMI or from GOME-2. The other two are derived with the EnKF algorithm, which is based on an ensemble Kalman filter applied to observations of multiple species using either the chemical transport model CHASER and MIROC-chem. The temporal behaviour and spatial distribution of the inventories are compared on a national and regional scale. A distinction is also made between urban and rural areas. The intercomparison of all inventories shows good agreement in total NOx emissions over mainland China, especially for trends, with an average bias of about 20 % for yearly emissions. All the inventories show the typical emission reduction of 10 % during the Chinese New Year and a peak in December. Satellite-derived approaches using OMI show a summer peak due to strong emissions from soil and biomass burning in this season. Biases in NOx emissions and uncertainties in temporal variability increase quickly when the spatial scale decreases. The analyses of the differences show the importance of using observations from multiple instruments and a high spatial resolution model for the satellite-derived inventories, while for bottom-up inventories, accurate emission factors and activity information are required. The advantage of the satellite-derived approach is that the emissions are soon available after observation, while the strength of the bottom-up inventories is that they include detailed information of emissions for each source category.
16376395
Impact of different emission inventories on simulated tropospheric ozone over China: a regional chemical transport model evaluation
The importance of emission inventory uncertainty on the simulation of summertime tropospheric ozone over China has been analyzed using a regional chemical transport model. Three independent emissions inventories, that are (i) emission estimates from the Emission Database for Global Atmospheric Research (EDGAR) for the year 1995, (ii) a regional emission inventory used in the Transport and Chemical Evolution over the Pacific (TRACE-P) program with emissions for the year 2000 and (iii) a national emission inventory used in the China Ozone Research Program (CORP) with emission estimates for the year 1995, are used for model simulation over a summer period. Methods used for the development of the inventories are discussed and differences in simulated ozone and its precursors with these emission inventories are analyzed. Comparison of the emission inventories revealed large differences in the emission estimates (up to 50% for NOx, ~100% for NMVOC and ~1000% for CO). Application of the different emission inventories in three model simulations showed minor differences in both surface O3 in rather unpolluted areas in China and at higher altitudes (500mbar). In polluted areas, differences in surface O3 are 30-50% between the different model simulations which seem rather small taking into account the large differences in the emission inventories. Additional sensitivity runs showed that the difference in NOx emissions as well NMVOC emissions is a dominant factor which controls the differences in simulated O3 concentrations while the impact of differences in CO emissions is relatively small. Although the CO emission estimate by CORP seems to be underestimated, there is no confidence to highlight one emission inventory better than the others.
33615109
Real-time air quality forecasting, part II: State of the science, current research needs, and future prospects
The review of major 3-D global and regional real-time air quality forecasting (RT-AQF) models in Part I identifies several areas of improvement in meteorological forecasts, chemical inputs, and model treatments of atmospheric physical, dynamic, and chemical processes. Part II highlights several recent scientific advances in some of these areas that can be incorporated into RT-AQF models to address model deficiencies and improve forecast accuracies. Current major numerical, statistical, and computational techniques to improve forecasting skills are assessed. These include bias adjustment techniques to correct biases in forecast products, chemical data assimilation techniques for improving chemical initial and boundary conditions as well as emissions, and ensemble forecasting approaches to quantify the uncertainties of the forecasts. Several case applications of current 3-D RT-AQF models with the state-of-the-science model treatments, a detailed urban process module, and an advanced combined ensemble/data assimilation technique are presented to illustrate current model skills and capabilities. Major technical challenges and research priorities are provided. A new generation of comprehensive RT-AQF model systems, to emerge in the coming decades, will be based on state-of-the-science 3-D RT-AQF models, supplemented with efficient data assimilation techniques and sophisticated statistical models, and supported with modern numerical/computational technologies and a suite of real-time observational data from all platforms.
6996555
Global partitioning of NOx sources using satellite observations: relative roles of fossil fuel combustion, biomass burning and soil emissions.
We use space-based observations of NO2 columns from the Global Ozone Monitoring Experiment (GOME) to derive monthly top-down NOx emissions for 2000 via inverse modeling with the GEOS-CHEM chemical transport model. Top-down NOx sources are partitioned among fuel combustion (fossil fuel and biofuel), biomass burning and soils by exploiting the spatio-temporal distribution of remotely sensed fires and a priori information on the location of regions dominated by fuel combustion. The top-down inventory is combined with an a priori inventory to obtain an optimized a posteriori estimate of the relative roles of NOx sources. The resulting a posteriori fuel combustion inventory (25.6 TgN year(-1)) agrees closely with the a priori (25.4 TgN year(-1)), and errors are reduced by a factor of 2, from +/- 80% to +/- 40%. Regionally, the largest differences are found over Japan and South Africa, where a posteriori estimates are 25% larger than a priori. A posteriori fuel combustion emissions are aseasonal, with the exception of East Asia and Europe where winter emissions are 30-40% larger relative to summer emissions, consistent with increased energy use during winter for heating. Global a posteriori biomass burning emissions in 2000 resulted in 5.8 TgN (compared to 5.9 TgN year(-1) in the a priori), with Africa accounting for half of this total. A posteriori biomass burning emissions over Southeast Asia/India are decreased by 46% relative to a priori; but over North equatorial Africa they are increased by 50%. A posteriori estimates of soil emissions (8.9 TgN year(-1)) are 68% larger than a priori (5.3 TgN year(-1)). The a posteriori inventory displays the largest soil emissions over tropical savanna/woodland ecosystems (Africa), as well as over agricultural regions in the western U.S. (Great Plains), southern Europe (Spain, Greece, Turkey), and Asia (North China Plain and North India), consistent with field measurements. Emissions over these regions are highest during summer at mid-latitudes and during the rainy season in the Tropics. We estimate that 2.5-4.5 TgN year(-1) are emitted from N-fertilized soils, at the upper end of previous estimates. Soil and biomass burning emissions account for 22% and 14% of global surface NOx emissions, respectively. We infer a significant role for soil NOx emissions at northern mid-latitudes during summer, where they account for nearly half that of the fuel combustion source, a doubling relative to the a priori. The contribution of soil emissions to background ozone is thus likely to be underestimated by the current generation of chemical transport models.
55022379
Satellite observations indicate substantial spatiotemporal variability in biomass burning NO x emission factors for South America
Abstract. Biomass burning is an important contributor to global total emissions of NOx (NO+NO2). Generally bottom-up fire emissions models calculate NOx emissions by multiplying fuel consumption estimates with static biome-specific emission factors, defined in units of grams of NO per kilogram of dry matter consumed. Emission factors are a significant source of uncertainty in bottom-up fire emissions modeling because relatively few observations are available to characterize the large spatial and temporal variability of burning conditions. In this paper we use NO2 tropospheric column observations from the Ozone Monitoring Instrument (OMI) from the year 2005 over South America to calculate monthly NOx emission factors for four fire types: deforestation, savanna/grassland, woodland, and agricultural waste burning. In general, the spatial patterns in NOx emission factors calculated in this work are consistent with emission factors derived from in situ measurements from the region but are more variable than published biome-specific global average emission factors widely used in bottom-up fire emissions inventories such as the Global Fire Emissions Database (GFED). Satellite-based NOx emission factors also indicate substantial temporal variability in burning conditions. Overall, we found that deforestation fires have the lowest NOx emission factors, on average 30% lower than the emission factors used in GFED v3. Agricultural fire NOx emission factors were the highest, on average a factor of 1.8 higher than GFED v3 values. For savanna, woodland, and deforestation fires, early dry season NOx emission factors were a factor of ~1.5–2 higher than late dry season emission factors. A minimum in the NOx emission factor seasonal cycle for deforestation fires occurred in August, the time period of severe drought in South America in 2005, supporting the hypothesis that prolonged dry spells may lead to an increase in the contribution of smoldering combustion from large-diameter fuels, offsetting the higher combustion efficiency of dryer fine fuels. We evaluated the OMI-derived NOx emission factors with SCIAMACHY NO2 tropospheric column observations and found improved model performance in regions dominated by fire emissions.
16005258
High-resolution mapping of vehicle emissions in China in 2008
Abstract. This study is the first in a series of papers that aim to develop high-resolution emission databases for different anthropogenic sources in China. Here we focus on on-road transportation. Because of the increasing impact of on-road transportation on regional air quality, developing an accurate and high-resolution vehicle emission inventory is important for both the research community and air quality management. This work proposes a new inventory methodology to improve the spatial and temporal accuracy and resolution of vehicle emissions in China. We calculate, for the first time, the monthly vehicle emissions for 2008 in 2364 counties (an administrative unit one level lower than city) by developing a set of approaches to estimate vehicle stock and monthly emission factors at county-level, and technology distribution at provincial level. We then introduce allocation weights for the vehicle kilometers traveled to assign the county-level emissions onto 0.05° × 0.05° grids based on the China Digital Road-network Map (CDRM). The new methodology overcomes the common shortcomings of previous inventory methods, including neglecting the geographical differences between key parameters and using surrogates that are weakly related to vehicle activities to allocate vehicle emissions. The new method has great advantages over previous methods in depicting the spatial distribution characteristics of vehicle activities and emissions. This work provides a better understanding of the spatial representation of vehicle emissions in China and can benefit both air quality modeling and management with improved spatial accuracy.
98843401
High-resolution historical emission inventories of crop residue burning in fields in China for the period 1990–2013
High-resolution historical emission inventories of crop residue burning in fields in China were developed for the period 1990–2013. More accurate time-varying statistical data and locally observed emission factors were utilized to estimate crop residue open burning emissions at provincial level. Then pollutants emissions were allocated to a high spatial resolution of 10 km × 10 km and a high temporal resolution of 1 day based on the Moderate Resolution Imaging Spectroradiometer (MODIS) Fire Product (MOD/MYD14A1). Results show that China’s CO emissions have increased by 5.67 times at an annual average rate of 24% from 1.06 Tg in 1990 to 7.06 Tg in 2013; the emissions of CO2, CH4, NMVOCs, N2O, NOx, NH3, SO2, PM2.5, OC, and BC have increased by 595%, 500%, 608%, 584%, 600%, 600%, 543%, 571%, 775%, and 500%, respectively, over the past 24 years. Spatially, the regions with high emissions had been notable expanding over the years, especially in the central eastern districts, the Northeastern of China, and the Sichuan Basin. Strong temporal pattern were observed with the highest emissions in June, followed by March to May and October. This work provides a better understanding of the spatiotemporal representation of agricultural fire emissions in China and can benefit both air quality modeling and management with improved accuracy.
54498837
MIX: a mosaic Asian anthropogenic emission inventory under the international collaboration framework of the MICS-Asia and HTAP
Abstract. The MIX inventory is developed for the years 2008 and 2010 to support the Model Inter-Comparison Study for Asia (MICS-Asia) and the Task Force on Hemispheric Transport of Air Pollution (TF HTAP) by a mosaic of up-to-date regional emission inventories. Emissions are estimated for all major anthropogenic sources in 29 countries and regions in Asia. We conducted detailed comparisons of different regional emission inventories and incorporated the best available ones for each region into the mosaic inventory at a uniform spatial and temporal resolution. Emissions are aggregated to five anthropogenic sectors: power, industry, residential, transportation, and agriculture. We estimate the total Asian emissions of 10 species in 2010 as follows: 51.3 Tg SO2, 52.1 Tg NOx, 336.6 Tg CO, 67.0 Tg NMVOC (non-methane volatile organic compounds), 28.8 Tg NH3, 31.7 Tg PM10, 22.7 Tg PM2.5, 3.5 Tg BC, 8.3 Tg OC, and 17.3 Pg CO2. Emissions from China and India dominate the emissions of Asia for most of the species. We also estimated Asian emissions in 2006 using the same methodology of MIX. The relative change rates of Asian emissions for the period of 2006–2010 are estimated as follows: −8.1 % for SO2, +19.2 % for NOx, +3.9 % for CO, +15.5 % for NMVOC, +1.7 % for NH3, −3.4 % for PM10, −1.6 % for PM2.5, +5.5 % for BC, +1.8 % for OC, and +19.9 % for CO2. Model-ready speciated NMVOC emissions for SAPRC-99 and CB05 mechanisms were developed following a profile-assignment approach. Monthly gridded emissions at a spatial resolution of 0.25°  ×  0.25° are developed and can be accessed from http://www.meicmodel.org/dataset-mix .
19778473
Comparison of emissions inventories of anthropogenic air pollutants and greenhouse gases in China
Abstract. Anthropogenic air pollutant emissions have been increasing rapidly in China, leading to worsening air quality. Modelers use emissions inventories to represent the temporal and spatial distribution of these emissions needed to estimate their impacts on regional and global air quality. However, large uncertainties exist in emissions estimates. Thus, assessing differences in these inventories is essential for the better understanding of air pollution over China. We compare five different emissions inventories estimating emissions of carbon dioxide (CO2), carbon monoxide (CO), nitrogen oxides (NOx), sulfur dioxide (SO2), and particulate matter with an aerodynamic diameter of 10 µm or less (PM10) from China. The emissions inventories analyzed in this paper include the Regional Emission inventory in ASia v2.1 (REAS), the Multi-resolution Emission Inventory for China (MEIC), the Emission Database for Global Atmospheric Research v4.2 (EDGAR), the inventory by Yu Zhao (ZHAO), and the Greenhouse Gas and Air Pollution Interactions and Synergies (GAINS). We focus on the period between 2000 and 2008, during which Chinese economic activities more than doubled. In addition to national totals, we also analyzed emissions from four source sectors (industry, transport, power, and residential) and within seven regions in China (East, North, Northeast, Central, Southwest, Northwest, and South) and found that large disagreements exist among the five inventories at disaggregated levels. These disagreements lead to differences of 67 µg m−3, 15 ppbv, and 470 ppbv for monthly mean PM10, O3, and CO, respectively, in modeled regional concentrations in China. We also find that all the inventory emissions estimates create a volatile organic compound (VOC)-limited environment and MEIC emissions lead to much lower O3 mixing ratio in East and Central China compared to the simulations using REAS and EDGAR estimates, due to their low VOC emissions. Our results illustrate that a better understanding of Chinese emissions at more disaggregated levels is essential for finding effective mitigation measures for reducing national and regional air pollution in China.
14101319
Inverse modelling of the spatial distribution of NO x emissions on a continental scale using satellite data
The recent important developments in satellite measurements of the composition of the lower atmosphere open the challenging perspective to use such measurements as independent information on sources and sinks of atmo- spheric pollutants. This study explores the possibility to im- prove estimates of gridded NOx emissions used in a conti- nental scale chemistry transport model (CTM), CHIMERE, by employing measurements performed by the GOME and SCIAMACHY instruments. We set-up an original inverse modelling scheme that not only enables a computationally efficient optimisation of the spatial distribution of seasonally averaged NOx emissions (during summertime), but also al- lows estimating uncertainties in input data and a priori emis- sions. The key features of our method are (i) replacement of the CTM by a set of empirical models describing the rela- tionships between tropospheric NO2 columns and NOx emis- sions with sufficient accuracy, (ii) combination of satellite data for tropospheric NO2 columns with ground based mea- surements of near surface NO2 concentrations, and (iii) eval- uation of uncertainties in a posteriori emissions by means of a special Bayesian Monte-Carlo experiment which is based on random sampling of errors of both NO2 columns and emis- sion rates. We have estimated the uncertainty in a priori emissions based on the EMEP emission inventory to be about 1.9 (in terms of geometric standard deviation) and found the uncertainty in a posteriori emissions obtained from our in- verse modelling scheme to be significantly lower (about 1.4). It is found also that a priori NOx emission estimates are prob- able to be persistently biased in many regions of Western Eu- rope, and that the use of a posteriori emissions in the CTM improves the agreement between the modelled and measured data.
55824802
An operational system for the assimilation of the satellite information on wild-land fires for the needs of air quality modelling and forecasting
This paper investigates a potential of two remotely sensed wild-land fire characteristics: 4-μm Brightness Temperature Anomaly (TA) and Fire Radiative Power (FRP) for the needs of operational chemical transport modelling and short-term forecasting of atmospheric composition and air quality. The treatments of the TA and FRP data are presented and a methodology for evaluating the emission fluxes of primary aerosols (PM 2.5 and total PM) is described. The method does not include the complicated analysis of vegetation state, fuel load, burning efficiency and related factors, which are uncertain but inevitably involved in approaches based on burnt-area scars or similar products. The core of the current methodology is based on the empirical emission factors that are used to convert the observed temperature anomalies and fire radiative powers into emission fluxes. These factors have been derived from the analysis of several fire episodes in Europe (28.4–5.5.2006, 15.8–25.8.2006 and in August 2008). These episodes were characterised by: (i) well-identified FRP and TA values, and (ii) available ground-based observations of aerosol concentrations, and optical thickness for the regions where the contribution of the fire smoke to the concentrations of PM 2.5 was dominant, in comparison with those of other pollution sources. The emission factors were determined separately for the forested and grassland areas; in case of mixed-type land use, an intermediate scaling was assumed. Despite significant differences between the TA and FRP methodologies, an accurate non-linear fitting was found between the predictions of these approaches. The agreement was comparatively weak only for small fires, for which the accuracy of both products is expected to be low. The applications of the Fire Assimilation System (FAS) in combination with the dispersion model SILAM showed that both the TA and FRP products are suitable for the evaluation of the emission fluxes from wild-land fires. The fire-originated concentrations of aerosols (PM 2.5 , PM 10 , sulphates and nitrates) and AOD, as predicted by the SILAM model were mainly within a factor of 2–3 compared with the observations. The main challenges of the FAS improvement include refining of the emission factors globally, determination of the types of fires (smouldering vs flaming), evaluation of the injection heights of the plumes, and predicting the temporal evolution of fires.
1604108
Substantial Underestimation of Post-Harvest Burning Emissions in the North China Plain Revealed by Multi-Species Space Observations
The large-scale burning of crop residues in the North China Plain (NCP), one of the most densely populated world regions, was recently recognized to cause severe air pollution and harmful health effects. A reliable quantification of the magnitude of these fires is needed to assess regional air quality. Here, we use an eight-year record (2005–2012) of formaldehyde measurements from space to constrain the emissions of volatile organic compounds (VOCs) in this region. Using inverse modelling, we derive that satellite-based post-harvest burning fluxes are, on average, at least a factor of 2 higher than state-of-the-art bottom-up statistical estimates, although with significant interannual variability. Crop burning is calculated to cause important increases in surface ozone (+7%) and fine aerosol concentrations (+18%) in the North China Plain in June. The impact of crop fires is also found in satellite observations of other species, glyoxal, nitrogen dioxide and methanol, and we show that those measurements validate the magnitude of the top-down fluxes. Our study indicates that the top-down crop burning fluxes of VOCs in June exceed by almost a factor of 2 the combined emissions from other anthropogenic activities in this region, underscoring the need for targeted actions towards changes in agricultural management practices.
30881469
Improved Attribution of Climate Forcing to Emissions
All Together Now Deciding how to change emissions of polluting gases that affect climate through their radiative forcing properties requires that the quantitative impact of these emissions be understood. Most past calculations of this type have considered only the radiative forcing of the specific emission and its atmospheric lifetime. Shindell et al. (p. 716; see the Perspectives by Arneth et al. and by Parrish and Zhu) use sophisticated atmospheric chemical and climate modeling to determine how gas-aerosol interactions affect the radiative properties of the atmosphere, finding significant departures from the standard method for emissions of methane, carbon monoxide, and nitrogen oxides. These findings should help to optimize strategies for mitigating global warming by reducing anthropogenic emissions. Chemical interactions between atmospheric gases and aerosols modify the global warming impacts of emissions. Evaluating multicomponent climate change mitigation strategies requires knowledge of the diverse direct and indirect effects of emissions. Methane, ozone, and aerosols are linked through atmospheric chemistry so that emissions of a single pollutant can affect several species. We calculated atmospheric composition changes, historical radiative forcing, and forcing per unit of emission due to aerosol and tropospheric ozone precursor emissions in a coupled composition-climate model. We found that gas-aerosol interactions substantially alter the relative importance of the various emissions. In particular, methane emissions have a larger impact than that used in current carbon-trading schemes or in the Kyoto Protocol. Thus, assessments of multigas mitigation policies, as well as any separate efforts to mitigate warming from short-lived pollutants, should include gas-aerosol interactions.
24139651
Cleaning up the air: effectiveness of air quality policy for SO 2 and NO x emissions in China
Abstract. Air quality observations by satellite instruments are global and have a regular temporal resolution, which makes them very useful in studying long-term trends in atmospheric species. To monitor air quality trends in China for the period 2005–2015, we derive SO2 columns and NOx emissions on a provincial level with improved accuracy. To put these trends into perspective they are compared with public data on energy consumption and the environmental policies of China. We distinguish the effect of air quality regulations from economic growth by comparing them relatively to fossil fuel consumption. Pollutant levels, per unit of fossil fuel, are used to assess the effectiveness of air quality regulations. We note that the desulfurization regulations enforced in 2005–2006 only had a significant effect in the years 2008–2009, when a much stricter control of the actual use of the installations began. For national NOx emissions a distinct decreasing trend is only visible from 2012 onwards, but the emission peak year differs from province to province. Unlike SO2, emissions of NOx are highly related to traffic. Furthermore, regulations for NOx emissions are partly decided on a provincial level. The last 3 years show a reduction both in SO2 and NOx emissions per fossil fuel unit, since the authorities have implemented several new environmental regulations. Despite an increasing fossil fuel consumption and a growing transport sector, the effects of air quality policy in China are clearly visible. Without the air quality regulations the concentration of SO2 would be about 2.5 times higher and the NO2 concentrations would be at least 25 % higher than they are today in China.
3516416
Asian emissions of CO and NOx : Constraints from aircraft and Chinese station data
[1] Observations of CO and NOy from the Transport and Chemical Evolution over the Pacific (TRACE-P) aircraft mission over the northwest Pacific and from two Chinese ground stations (Hong Kong and Lin An) during spring 2001 are used in conjunction with an optimal estimation inverse model to constrain estimates of Asian emissions of CO and NOx. A priori emissions are based on a detailed bottom-up inventory for the observation period. The inversion analysis requires 43% and 47% increases in Chinese emissions of CO and NOx, respectively, distributed heterogeneously, with the largest adjustments required for central China. A posteriori estimates of emissions from biomass burning in Southeast Asia are much lower than a priori values. Inversion results for NOx emissions are consistent with CO emissions in terms of the sense of the adjustments. Inclusion of the station data in the inversion analysis significantly improves estimates for emissions from central and south China. A large increase in NOx emissions inferred for central China (a factor of 3) is attributed to decomposition of organic wastes associated with the human-animal food chain and extensive applications of chemical fertilizer. An analysis of emission ratios for CO relative to NOx for different sectors indicates that emissions attributed to industry and transportation may be underestimated in the bottom-up inventory for central China, while emissions from the domestic sector may be underestimated for south China. An increase in emission factors could help reconcile results from the inversion analysis with the “bottom-up” approach. Detailed analysis of the surface observations using a posteriori emissions indicates the importance of meteorological phenomena, notably cold fronts in March and small-scale high- and low-pressure systems in April in modulating concentrations of CO, with the latter most evident in the data from Lin An.
1120830
Asian emissions in 2006 for the NASA INTEX-B mission
Abstract. A new inventory of air pollutant emissions in Asia in the year 2006 is developed to support the Intercontinental Chemical Transport Experiment-Phase B (INTEX-B) funded by the National Aeronautics and Space Administration (NASA). Emissions are estimated for all major anthropogenic sources, excluding biomass burning. We estimate total Asian anthropogenic emissions in the year 2006 as follows: 47.1 Tg SO2, 36.7 Tg NOx, 298.2 Tg CO, 54.6 Tg NMVOC, 29.2 Tg PM10, 22.2 Tg PM2.5, 2.97 Tg BC, and 6.57 Tg OC. We emphasize emissions from China because they dominate the Asia pollutant outflow to the Pacific and the increase of emissions from China since 2000 is of great concern. We have implemented a series of improved methodologies to gain a better understanding of emissions from China, including a detailed technology-based approach, a dynamic methodology representing rapid technology renewal, critical examination of energy statistics, and a new scheme of NMVOC speciation for model-ready emissions. We estimate China's anthropogenic emissions in the year 2006 to be as follows: 31.0 Tg SO2, 20.8 Tg NOx, 166.9 Tg CO, 23.2 Tg NMVOC, 18.2 Tg PM10, 13.3 Tg PM2.5, 1.8 Tg BC, and 3.2 Tg OC. We have also estimated 2001 emissions for China using the same methodology and found that all species show an increasing trend during 2001–2006: 36% increase for SO2, 55% for NOx, 18% for CO, 29% for VOC, 13% for PM10, and 14% for PM2.5, BC, and OC. Emissions are gridded at a resolution of 30 min×30 min and can be accessed at our web site ( http://mic.greenresource.cn/intex-b2006 ).
129834277
Korean National Emissions Inventory System and 2007 Air Pollutant Emissions
Korea has experienced dramatic development and has become highly industrialized and urbanized during the past 40 years, which has resulted in rapid economic growth. Due to the industrialization and urbanization, however, air pollutant emission sources have increased substantially. Rapid increases in emission sources have caused Korea to suffer from serious air pollution. An air pollutant emissions inventory is one set of essential data to help policymakers understand the current status of air pollution levels, to establish air pollution control policies and to analyze the impacts of implementation of policies, as well as for air quality studies. To accurately and realistically estimate administrative district level air pollutant emissions of Korea, we developed a Korean Emissions Inventory System named the Clean Air Policy Support System (CAPSS). In CAPSS, emissions sources are classified into four levels. Emission factors for each classification category are collected from various domestic and international research reports, and the CAPSS utilizes various national, regional and local level statistical data, compiled by approximately 150 Korean organizations. In this paper, we introduced for the first time, a Korean national emissions inventory system and release Korea’s official 2007 air pollutant emissions for five regulated air pollutants.
11372641
Quantifying the uncertainties of a bottom-up emission inventory of anthropogenic atmospheric pollutants in China
The uncertainties of a national, bottom-up inven- tory of Chinese emissions of anthropogenic SO2, NOx, and particulate matter (PM) of different size classes and carbona- ceous species are comprehensively quantified, for the first time, using Monte Carlo simulation. The inventory is struc- tured by seven dominant sectors: coal-fired electric power, cement, iron and steel, other industry (boiler combustion), other industry (non-combustion processes), transportation, and residential. For each parameter related to emission fac- tors or activity-level calculations, the uncertainties, repre- sented as probability distributions, are either statistically fit- ted using results of domestic field tests or, when these are lacking, estimated based on foreign or other domestic data. The uncertainties (i.e., 95% confidence intervals around the central estimates) of Chinese emissions of SO2, NOx, total PM, PM10, PM2.5, black carbon (BC), and organic carbon (OC) in 2005 are estimated to be −14%∼13%, −13%∼37%, −11%∼38%, −14%∼45%, −17%∼54%, −25%∼136%, and −40%∼121%, respectively. Variations at activity lev- els (e.g., energy consumption or industrial production) are not the main source of emission uncertainties. Due to nar- row classification of source types, large sample sizes, and relatively high data quality, the coal-fired power sector is es- timated to have the smallest emission uncertainties for all species except BC and OC. Due to poorer source classi- fications and a wider range of estimated emission factors, considerable uncertainties of NOx and PM emissions from cement production and boiler combustion in other indus- tries are found. The probability distributions of emission factors for biomass burning, the largest source of BC and OC, are fitted based on very limited domestic field measure- ments, and special caution should thus be taken interpreting these emission uncertainties. Although Monte Carlo simu- lation yields narrowed estimates of uncertainties compared to previous bottom-up emission studies, the results are not always consistent with those derived from satellite obser- vations. The results thus represent an incremental research advance; while the analysis provides current estimates of uncertainty to researchers investigating Chinese and global atmospheric transport and chemistry, it also identifies spe- cific needs in data collection and analysis to improve on them. Strengthened quantification of emissions of the in- cluded species and other, closely associated ones - notably CO2, generated largely by the same processes and thus sub- ject to many of the same parameter uncertainties - is essential not only for science but for the design of policies to redress critical atmospheric environmental hazards at local, regional, and global scales.
206970715
Reduction in NO(x) emission trends over China: regional and seasonal variations.
We analyzed satellite observations of nitrogen dioxide (NO2) columns by the Ozone Monitoring Instrument (OMI) over China from 2005 to 2010 in order to estimate the top-down anthropogenic nitrogen oxides (NOx) emission trends. Since NOx emissions were affected by the economic slowdown in 2009, we removed one year of abnormal data in the analysis. The estimated average emission trend is 4.01 ± 1.39% yr(-1), which is slower than the trend of 5.8-10.8% yr(-1) reported for previous years. We find large regional, seasonal, and urban-rural variations in emission trends. The average NOx emission trend of 3.47 ± 1.07% yr(-1) in warm season (June-September) is less than the trend of 5.03 ± 1.92% yr(-1) in cool season (October-May). The regional annual emission trends decrease from 4.76 ± 1.61% yr(-1) in North China Plain to 3.11 ± 0.98% yr(-1) in Yangtze River Delta and further down to -4.39 ± 1.81% yr(-1) in Pearl River Delta. The annual emission trends of the four largest megacities, Shanghai, Beijing, Guangzhou, and Shenzhen are -0.76 ± 0.29%, 0.69 ± 0.27%, -4.46 ± 1.22%, and -7.18 ± 2.88% yr(-1), considerably lower than the regional averages or surrounding rural regions. These results appear to suggest that a number of factors, including emission control measures of thermal power plants, increased hydro-power usage, vehicle emission regulations, and closure or migration of high-emission industries, have significantly reduced or even reversed the increasing trend of NOx emissions in more economically developed megacities and southern coastal regions, but their effects are not as significant in other major cities or less economically developed regions.
123221960
The ERA-Interim reanalysis: configuration and performance of the data assimilation system
ERA-Interim is the latest global atmospheric reanalysis produced by the European Centre for Medium-Range Weather Forecasts (ECMWF). The ERA-Interim project was conducted in part to prepare for a new atmospheric reanalysis to replace ERA-40, which will extend back to the early part of the twentieth century. This article describes the forecast model, data assimilation method, and input datasets used to produce ERA-Interim, and discusses the performance of the system. Special emphasis is placed on various difficulties encountered in the production of ERA-40, including the representation of the hydrological cycle, the quality of the stratospheric circulation, and the consistency in time of the reanalysed fields. We provide evidence for substantial improvements in each of these aspects. We also identify areas where further work is needed and describe opportunities and objectives for future reanalysis projects at ECMWF. Copyright © 2011 Royal Meteorological Society
94490058
NOx emission estimates during the 2014 Youth Olympic Games in Nanjing (discussion paper)
The Nanjing Government has taken temporary environmental regulations to guarantee good air quality during the Youth Olympic Games (YOG) in 2014. We study the effect of those regulations by applying the emission estimate algorithm DECSO (Daily Emission estimates Constrained by Satellite Observations) to measurements of the Ozone Monitoring Instrument (OMI). We improved DECSO by updating the chemical transport model CHIMERE from v2006 to v2013 and by adding an Observation minus Forecast (OmF) criterion to filter outlying satellite retrievals due to high aerosol concentrations. The comparison of model results with both ground and satellite observations indicates that CHIMERE v2013 is better performing than CHIMERE v2006. After filtering the satellite observations with high aerosol loads that were leading to large OmF values, unrealistic jumps in the emission estimates are removed. Despite the cloudy conditions during the YOG we could still see a decrease of tropospheric NO2 column concentrations of about 32% in the OMI observations as compared to the average NO2 concentrations from 2005 to 2012. The results of the improved DECSO algorithm for NOx emissions show a reduction of at least 25% during the YOG period. This indicates that air quality regulations taken by the local government were successful. The algorithm is also able to detect an emission reduction of 10% during the Chinese Spring Festival. This study demonstrates the capacity of the DECSO algorithm to capture the change of NOx emissions on a monthly scale. We also show that the observed concentrations and the derived emissions show different patterns that provide complimentary information. For example, the Nanjing smog episode in December 2013 led to a strong increase in NO2 concentrations without an increase in NOx emissions. Furthermore, DECSO gives us important information of the non-trivial seasonal relation between NOx emissions and NO2 concentrations on a local scale.
13452777
Constraints on surface NOx emissions by assimilating satellite observations of multiple species
[1] Surface NOx emissions are estimated by a combined assimilation of satellite observations of NO2, CO, O3, and HNO3 with a global chemical transport model. The assimilation of measurements for species other than NO2 provides additional constraints on the NOx emissions by adjusting the concentrations of the species affecting the NOx chemistry and leads to changes in the regional monthly-mean emissions of −58 to +32% and the annual total emissions of −16 to +3%. These large changes highlight that uncertainties in the model chemistry impact the quality of the emission estimates. In the inversion from NO2 observations only, NOx analysis increments occur closer to the surface. Because of the shorter residence time, larger emissions increments are required compared to the multiple species assimilation. Validation against independent observations and comparisons with the recent Regional Emission inventory in Asia version 2.1 emissions shows that the multiple species assimilation improves the chemical consistency including the relation between concentrations and the estimated emissions.
134614795
Global emission inventories in the Emission Database for Global Atmospheric Research (EDGAR) – Manual (I) I. Gridding: EDGAR emissions distribution on global gridmaps
The Emissions Database for Global Atmospheric Research EDGAR, version 4 is managed at a JRC-server and documented with an emipedia website. The final resulting datasets of sector-specific emission inventories for all world countries and the resulting gridmaps have been published for all greenhouse gases and air pollutants and PM10 particulate matter on edgar.jrc.ec.europa.eu. These are accompanied so far with a description online, which is then worked out in more detail in the EDGAR Manual series. A first part of the EDGAR Manual series is this report "Gridding: EDGAR emissions distribution on global gridmaps". The report documents all geospatial surrogates that were collected, mainly from publicly available information sources, which were manipulated to arrive to a full set of consistent proxy data with spatial resolution of 0.1degx0.1deg. The set of a hundred proxy datasets are applied to all EDGARv4 emissions yielding the sector-specific global emission gridmaps for all substances. Except for population and the derived urban and rural population proxy datasets, the proxy do not change over time. The population proxy, taken from CIESIN is an important default for the gridding and changes over time, reflecting the migration of people. More in particular the urban population proxy, derived in-house based on a combination of population and urban settlements, the urbanisation process over the past two decades is taken up. All spatial datasets are two-dimensional, covering the globe, except for aviation. The airline distribution occurs with three distinct layers at different heights, in order to cover a minimum third dimension. The other emissions data are upon request split into two height layers, one at stack height, one at ground level, based on the type of activity. The global coverage and geospatial consistency allow to provide a consistent input to the atmospheric chemistry. In particular multipollutant sources are represented as one single point source. The usefulness of these proxy datasets is reflected by the requests for applying it on other emission inventories, such as the UNEP emissions from IIASA or the EMEP emissions at CEIP.
59407871
Forty years of improvements in European air quality: regional policy-industry interactions with global impacts
The EDGAR (Emissions Database for Global Atmospheric Research) v4.3 global anthropogenic emissions inventory of several gaseous (SO2, NOx, CO, non-methane volatile organic compounds (NMVOCs) and NH3) and particulate (PM10, PM2.5, black and organic carbon (BC and OC)) air pollutants for the period 1970–2010 is used to develop retrospective air pollution emission scenarios to quantify the roles and contributions of changes in fuels consumption, technology, end-of-pipe emission reduction measures and their resulting impact on health and crop yields. This database presents changes in activity data, fuels and air pollution abatement technology for the past 4 decades, using international statistics and following guidelines for bottom-up emission inventory at the Tier 1 and Tier 2 levels with region-specific default values. 

With two further retrospective scenarios we assess (1) the impact of the technology and end-of-pipe (EOP) reduction measures in the European Union (EU) by considering a stagnation of technology with constant emission factors from 1970 and with no further abatement measures and improvement in European emissions standards, but fuel consumption occurring at historical pace, and (2) the impact of increased fuel consumption by considering unchanged energy use with constant fuel consumption since 1970, but technological development and end-of-pipe reductions. Our scenario analysis focuses on the three most important and most regulated sectors (power generation, the manufacturing industry and road transport), which are subject of multi-pollutant EU Air Quality regulations. 

If technology and European EOP reduction measures had stagnated at 1970 levels, EU air quality in 2010 would have suffered from 129 % higher SO2, 71 % higher NOx and 69 % higher PM2.5 emissions, demonstrating the large role of technology in reducing emissions in 2010. However, if fuel consumption had remained constant starting in 1970, the EU would have benefited from current technology and emission control standards, with reductions in NOx by even 13 % more. Such further savings are not observed for SO2 and PM2.5. If the EU consumed the same amount of fuels as in 1970 but with the current technology and emission control standards, then the emissions of SO2 and PM2.5 would be 42 % respectively 10 % higher. This scenario shows the importance for air quality of abandoning heavy residual fuel oil and shifting fuel types (from, e.g., coal to gas) in the EU. 

A reduced-form TM5-FASST (Fast Screening Scenario Tool based on the global chemical Transport Model 5) is applied to calculate regional and global levels of aerosol and ozone concentrations and to assess the impact of air quality improvements on human health and crop yield loss, showing substantial impacts of export of EU technologies and standards to other world regions.
13407067
CHIMERE 2013 : a model for regional atmospheric composition modelling
Abstract. Tropospheric trace gas and aerosol pollutants have adverse effects on health, environment and climate. In order to quantify and mitigate such effects, a wide range of processes leading to the formation and transport of pollutants must be considered, understood and represented in numerical models. Regional scale pollution episodes result from the combination of several factors: high emissions (from anthropogenic or natural sources), stagnant meteorological conditions, kinetics and efficiency of the chemistry and the deposition. All these processes are highly variable in time and space, and their relative contribution to the pollutants budgets can be quantified with chemistry-transport models. The CHIMERE chemistry-transport model is dedicated to regional atmospheric pollution event studies. Since it has now reached a certain level a maturity, the new stable version, CHIMERE 2013, is described to provide a reference model paper. The successive developments of the model are reviewed on the basis of published investigations that are referenced in order to discuss the scientific choices and to provide an overview of the main results.
12516613
The ozone monitoring instrument
The Ozone Monitoring Instrument (OMI) flies on the National Aeronautics and Space Administration's Earth Observing System Aura satellite launched in July 2004. OMI is a ultraviolet/visible (UV/VIS) nadir solar backscatter spectrometer, which provides nearly global coverage in one day with a spatial resolution of 13 km/spl times/24 km. Trace gases measured include O/sub 3/, NO/sub 2/, SO/sub 2/, HCHO, BrO, and OClO. In addition, OMI will measure aerosol characteristics, cloud top heights, and UV irradiance at the surface. OMI's unique capabilities for measuring important trace gases with a small footprint and daily global coverage will be a major contribution to our understanding of stratospheric and tropospheric chemistry and climate change. OMI's high spatial resolution is unprecedented and will enable detection of air pollution on urban scale resolution. In this paper, the instrument and its performance will be discussed.
55844491
SCIAMACHY: Mission Objectives and Measurement Modes
Abstract SCIAMACHY (Scanning Imaging Absorption Spectrometer for Atmospheric Chartography) is a spectrometer designed to measure sunlight transmitted, reflected, and scattered by the earth’s atmosphere or surface in the ultraviolet, visible, and near-infrared wavelength region (240–2380 nm) at moderate spectral resolution (0.2–1.5 nm, λ/Δλ ≈ 1000–10 000). SCIAMACHY will measure the earthshine radiance in limb and nadir viewing geometries and solar or lunar light transmitted through the atmosphere observed in occultation. The extraterrestrial solar irradiance and lunar radiance will be determined from observations of the sun and the moon above the atmosphere. The absorption, reflection, and scattering behavior of the atmosphere and the earth’s surface is determined from comparison of earthshine radiance and solar irradiance. Inversion of the ratio of earthshine radiance and solar irradiance yields information about the amounts and distribution of important atmospheric constituents and the spectral reflecta...
9167215
CHASER: A global chemical model of the troposphere 1. Model description
[1] We present a new global three-dimensional chemical model for the troposphere, named chemical atmospheric general circulation model (AGCM) for study of atmospheric environment and radiative forcing (CHASER). This model, developed in the framework of the Center for Climate System Research/National Institute for Environment Studies (CCSR/NIES) AGCM, is aimed to study tropospheric photochemistry and its influences on climate. The chemical component of the model simulates the O3-HOx-NOx-CH4-CO photochemical system and oxidation of nonmethane hydrocarbons through 88 chemical and 25 photolytic reactions with 47 chemical species in its present configuration. The model includes emission sources, dry and wet deposition, as well as chemical transformations. Meteorological processes such as transport due to advection, convection, and other subgrid-scale mixing are simulated “on-line” by the dynamical component of the CCSR/NIES AGCM. A detailed evaluation of the model results is presented in a companion paper [Sudo et al., 2002]. An evaluation of the transport scheme adopted in the model suggests that the model is capable of simulating transport associated with convection and boundary layer mixing as well as large-scale advection. The model capability to simulate dry and wet deposition was also evaluated by conducting a simulation of atmospheric lead. The simulated lead distributions are consistent with those observed at the surface, showing the validity of the deposition parameterization adopted in the model.
62683101
MIROC-ESM 2010: model description and basic results of CMIP5-20c3m experiments
Abstract. An earth system model (MIROC-ESM 2010) is fully described in terms of each model component and their interactions. Results for the CMIP5 (Coupled Model Intercomparison Project phase 5) historical simulation are presented to demonstrate the model's performance from several perspectives: atmosphere, ocean, sea-ice, land-surface, ocean and terrestrial biogeochemistry, and atmospheric chemistry and aerosols. An atmospheric chemistry coupled version of MIROC-ESM (MIROC-ESM-CHEM 2010) reasonably reproduces transient variations in surface air temperatures for the period 1850–2005, as well as the present-day climatology for the zonal-mean zonal winds and temperatures from the surface to the mesosphere. The historical evolution and global distribution of column ozone and the amount of tropospheric aerosols are reasonably simulated in the model based on the Representative Concentration Pathways' (RCP) historical emissions of these precursors. The simulated distributions of the terrestrial and marine biogeochemistry parameters agree with recent observations, which is encouraging to use the model for future global change projections.
12526885
Validation of urban NO 2 concentrations and their diurnal and seasonal variations observed from the SCIAMACHY and OMI sensors using in situ surface measurements in Israeli cities
We compare a full-year (2006) record of surface air NO2 concentrations measured in Israeli cities to coin- ciding retrievals of tropospheric NO2 columns from satellite sensors (SCIAMACHY aboard ENVISAT and OMI aboard Aura). This provides a large statistical data set for valida- tion of NO2 satellite measurements in urban air, where vali- dation is difficult yet crucial for using these measurements to infer NOx emissions by inverse modeling. Assuming that NO2 is well-mixed throughout the boundary layer (BL), and using observed average seasonal boundary layer heights, near-surface NO2 concentrations are converted into BL NO2 columns. The agreement between OMI and (13:45) BL NO2 columns (slope=0.93, n=542), and the comparable results at 10:00 h for SCIAMACHY, allow a validation of the seasonal, weekly, and diurnal cycles in satellite-derived NO2. OMI and BL NO2 columns show consistent seasonal cycles (win- ter NO2 1.6-2.7◊ higher than summer). BL and coinciding OMI columns both show a strong weekly cycle with 45-50% smaller NO2 columns on Saturday relative to the weekday mean, reflecting the reduced weekend activity, and validating the weekly cycle observed from space. The diurnal differ- ence between SCIAMACHY (10:00) and OMI (13:45) NO 2 is maximum in summer when SCIAMACHY is up to 40% higher than OMI, and minimum in winter when OMI slightly exceeds SCIAMACHY. A similar seasonal variation in the diurnal difference is found in the source region of Cairo. The surface measurements in Israel cities confirm this sea- sonal variation in the diurnal cycle. Using simulations from a global 3-D chemical transport model (GEOS-Chem), we show that this seasonal cycle can be explained by a much stronger photochemical loss of NO2 in summer than in win- ter.
158045449
Recent reduction in NO x emissions over China: synthesis of satellite observations and emission inventories
Tropospheric nitrogen dioxide (NO2) column densities detected from space are widely used to infer trends in terrestrial nitrogen oxide (NO x ) emissions. We study changes in NO2 column densities using the Ozone Monitoring Instrument (OMI) over China from 2005 to 2015 and compare them with the bottom-up inventory to examine NO x emission trends and their driving forces. From OMI measurements we detect the peak of NO2 column densities at a national level in the year 2011, with average NO2 column densities deceasing by 32% from 2011 to 2015 and corresponding to a simultaneous decline of 21% in bottom-up emission estimates. A significant variation in the peak year of NO2 column densities over regions is observed. Because of the reasonable agreement between the peak year of NO2 columns and the start of deployment of denitration devices, we conclude that power plants are the primary contributor to the NO2 decline, which is further supported by the emission reduction of 56% from the power sector in the bottom-up emission inventory associated with the penetration of selective catalytic reduction (SCR) increasing from 18% to 86% during 2011–2015. Meanwhile, regulations for vehicles also make a significant contribution to NO x emission reductions, in particular for a few urbanized regions (e.g., Beijing and Shanghai), where they implemented strict regulations for vehicle emissions years before the national schedule for SCR installations and thus reached their NO2 peak 2–3 years ahead of the deployment of denitration devices for power plants.
11702123
Assimilated inversion of NOx emissions over east Asia using OMI NO2 column measurements
[1] Assimilated inversion on a daily basis using OMI tropospheric NO2 columns is developed and applied in a regional chemical transport model (REAM) to constrain fossil fuel (FF) NOx emissions over east Asia in 2007. The iterative nature of the assimilated inversion improves upon the widely used monthly-mean inversion by accounting for the chemical feedbacks of changed NOx emissions and reducing the dependence of the a priori emissions. The assimilated a posteriori emissions from FF combustion over east Asia are 9.5 Tg N/yr comparable to 10.9 Tg N/yr of the a priori. Significant changes in the spatial distribution of FF NOx emissions are found in the assimilated inversion from the a priori or monthly-mean inversion. The assimilated inversion shows that the a priori FF NOx emission inventory tends to overestimate the emissions over the economically developed areas and underestimate over the underdeveloped areas in East China, which may reflect in part FF NOx emission reductions resulting from the urban-centric air quality controls in China.
100761873
Multi-satellite sensor study on precipitation-induced emission pulses of NO x from soils in semi-arid ecosystems
Abstract. We present a top-down approach to infer and quantify rain-induced emission pulses of NOx ( ≡  NO + NO2), stemming from biotic emissions of NO from soils, from satellite-borne measurements of NO2. This is achieved by synchronizing time series at single grid pixels according to the first day of rain after a dry spell of prescribed duration. The full track of the temporal evolution several weeks before and after a rain pulse is retained with daily resolution. These are needed for a sophisticated background correction, which accounts for seasonal variations in the time series and allows for improved quantification of rain-induced soil emissions. The method is applied globally and provides constraints on pulsed soil emissions of NOx in regions where the NOx budget is seasonally dominated by soil emissions. We find strong peaks of enhanced NO2 vertical column densities (VCDs) induced by the first intense precipitation after prolonged droughts in many semi-arid regions of the world, in particular in the Sahel. Detailed investigations show that the rain-induced NO2 pulse detected by the OMI (Ozone Monitoring Instrument), GOME-2 and SCIAMACHY satellite instruments could not be explained by other sources, such as biomass burning or lightning, or by retrieval artefacts (e.g. due to clouds). For the Sahel region, absolute enhancements of the NO2 VCDs on the first day of rain based on OMI measurements 2007–2010 are on average 4 × 1014  molec cm−2 and exceed 1 × 1015  molec cm−2 for individual grid cells. Assuming a NOx lifetime of 4 h, this corresponds to soil NOx emissions in the range of 6 up to 65 ng N m−2 s−1, which is in good agreement with literature values. Apart from the clear first-day peak, NO2 VCDs are moderately enhanced (2 × 1014  molec cm−2) compared to the background over the following 2 weeks, suggesting potential further emissions during that period of about 3.3 ng N m−2 s−1. The pulsed emissions contribute about 21–44 % to total soil NOx emissions over the Sahel.
6400167
Intercomparison of SCIAMACHY and OMI Tropospheric NO2 Columns: Observing the Diurnal Evolution of Chemistry and Emissions from Space
[1] Concurrent (August 2006) measurements of tropospheric NO2 columns from OMI aboard Aura (1330 local overpass time) and SCIAMACHY aboard Envisat (1000 local overpass time) offer an opportunity to examine the consistency between the two instruments under tropospheric background conditions and the effect of different observing times. For scenes with tropospheric NO2 columns <5.0 × 1015 molecules cm−2, SCIAMACHY and OMI agree within 1.0–2.0 × 1015 molecules cm−2, consistent with the detection limits of both instruments. We find evidence for a low bias of 0.2 × 1015 molecules cm−2 in OMI observations over remote oceans. Over the fossil fuel source regions at northern midlatitudes, we find that SCIAMACHY observes up to 40% higher NO2 at 1000 local time (LT) than OMI at 1330 LT. Over biomass burning regions in the tropics, SCIAMACHY observes up to 40% lower NO2 columns than OMI. These differences are present in the spectral fitting of the data (slant column) and are augmented in the fossil fuel regions and dampened in the tropical biomass burning regions by the expected increase in air mass factor as the mixing depth rises from 1000 to 1330 LT. Using a global 3-D chemical transport model (GEOS-Chem), we show that the 1000–1330 LT decrease in tropospheric NO2 column over fossil fuel source regions can be explained by photochemical loss, dampened by the diurnal cycle of anthropogenic emissions that has a broad daytime maximum. The observed 1000–1330 LT NO2 column increase over tropical biomass burning regions points to a sharp midday peak in emissions and is consistent with a diurnal cycle of emissions derived from geostationary satellite fire counts.
56016811
Key chemical NOx sink uncertainties and how they influence top-down emissions of nitrogen oxides
Triggered by recent developments from laboratory and field studies regarding major NO x sink pathways in the troposphere, this study evaluates the influence of chemical uncertainties in NOx sinks for global NOx distributions calculated by the IMAGESv2 chemistry-transport model, and quantifies their significance for top-down NO x emission estimates. Our study focuses on five key chemical parameters believed to be of primary importance, more specifically, the rate of the reaction of NO2 with OH radicals, the newly identified HNO3-forming channel in the reaction of NO with HO 2, the reactive uptake of N2O5 and HO2 by aerosols, and the regeneration of OH in the oxidation of isoprene. Sensitivity simulations are performed to estimate the impact of each source of uncertainty. The model calculations show that, although the NO2+OH reaction is the largest NO x sink globally accounting for ca. 60 % of the total sink, the reactions contributing the most to the overall uncertainty are the formation of HNO 3 in NO+HO2, leading to NOx column changes exceeding a factor of two over tropical regions, and the uptake of HO 2 by aqueous aerosols, in particular over East and South Asia. Emission inversion experiments are carried out using model settings which either minimise (MINLOSS) or maximise (MAXLOSS) the total NOx sink, both constrained by one year of OMI NO2 column data from the DOMINO v2 KNMI algorithm. The choice of the model setup is found to have a major impact on the top-down flux estimates, with 75 % higher emissions for MAXLOSS compared to the MINLOSS inversion globally. Even larger departures are found for soil NO (factor of 2) and lightning (1.8). The global anthropogenic source is better constrained (factor of 1.57) than the natural sources, except over Sou h Asia where the combined uncertainty primarily associated to the NO+HO 2 reaction in summer and HO2 uptake by aerosol in winter lead to top-down emission differences exceeding a factor of 2. Evaluation of the emission optimisation is performed against independent satellite observations from the SCIAMACHY sensor, with airborne NO2 measurements of the INTEX-A and INTEX-B campaigns, as well as with two new bottom-up inventories of anthropogenic emissions in Asia (REASv2) and China (MEIC). Neither the MINLOSS nor the MAXLOSS setup succeeds in providing the best possible match with all independent datasets. Whereas the minimum sink assumption leads to better agreement with aircraft NO2 profile measurements, consistent with the results of a previous analysis ( Henderson et al. , 2012), the same assumption leads to unrealistic features in the inferred distribution of emissions over China. Clearly, although our study addresses an important issue which was largely overlooked in previous inversion exercises, and demonstrates the strong influence of NOx loss uncertainties on top-down emission fluxes, additional processes need to be considered which could also influence the inferred source. Published by Copernicus Publications on behalf of the European Geosciences Union. 9058 T. Stavrakou et al.: Impact of NOx sink uncertainties on top-down NOx emissions
56295198
Structural uncertainty in air mass factor calculation for NO2 and HCHO satellite retrievals
Air mass factor (AMF) calculation is the largest source of uncertainty in NO2 and HCHO satellite retrievals in situations with enhanced trace gas concentrations in the lower troposphere. Structural uncertainty arises when different retrieval methodologies are applied within the scientific community to the same satellite observations. Here, we address the issue of AMF structural uncertainty via a detailed comparison of AMF calculation methods that are structurally different between seven retrieval groups for measurements from the Ozone Monitoring Instrument (OMI). We estimate the escalation of structural uncertainty in every sub-step of the AMF calculation process. This goes beyond the algorithm uncertainty estimates provided in state-of-the-art retrievals, which address the theoretical propagation of uncertainties for one particular retrieval algorithm only. We find that top-of-atmosphere reflectances simulated by four radiative transfer models (RTMs) (DAK, McArtim, SCIATRAN and VLIDORT) agree within 1.5 %. We find that different retrieval groups agree well in the calculations of altitude resolved AMFs from different RTMs (to within 3 %), and in the tropospheric AMFs (to within 6 %) as long as identical ancillary data (surface albedo, terrain height, cloud parameters and trace gas profile) and cloud and aerosol correction procedures are being used. Structural uncertainty increases sharply when retrieval groups use their preference for ancillary data, cloud and aerosol correction. On average, we estimate the AMF structural uncertainty to be 42 % over polluted regions and 31 % over unpolluted regions, mostly driven by substantial differences in the a priori trace gas profiles, surface albedo and cloud parameters. Sensitivity studies for one particular algorithm indicate that different cloud correction approaches result in substantial AMF differences in polluted conditions (5 to 40 % depending on cloud fraction and cloud pressure, and 11 % on average) even for low cloud fractions (<0.2) and the choice of aerosol correction introduces an average uncertainty of 50 % for situations with high pollution and high aerosol loading. Our work shows that structural uncertainty in AMF calculations is significant and that it is mainly caused by the assumptions and choices made to represent the state of the atmosphere. In order to decide which approach and which ancillary data are best for AMF calculations, we call for well-designed validation exercises focusing on polluted conditions in which AMF structural uncertainty has the highest impact on NO2 and HCHO retrievals.
54703464
Satellite constraint for emissions of nitrogen oxides from anthropogenic , lightning and soil sources over East China on a high-resolution grid
Vertical column densities (VCDs) of tropospheric nitrogen dioxide (NO2) retrieved from space provide valuable information to estimate emissions of nitrogen oxides (NOx) inversely. Accurate emission attribution to individual sources, important both for understanding the global biogeochemical cycling of nitrogen and for emission control, remains difficult. This study presents a regression-based multi-step inversion approach to estimate emissions of NO x from anthropogenic, lightning and soil sources individually for 2006 over East China on a 0.25 ◦ long× 0.25 lat grid, employing the DOMINO product version 2 retrieved from the Ozone Monitoring Instrument. The inversion is done gridbox by gridbox to derive the respective emissions, taking advantage of differences in seasonality between anthropogenic and natural sources. Lightning and soil emissions are combined together for any given gridbox due to their similar seasonality; and their different spatial distributions are used implicitly for source separation to some extent. The nested GEOS-Chem model for East Asia is used to simulate the seasonal variations of different emission sources and impacts on VCDs of NO2 for the inversion purpose. Sensitivity tests are conducted to evaluate key assumptions embedded in the inversion process. The inverse estimate suggests annual budgets of about 7.1 TgN ( ±39 %), 0.21 TgN ( ±61 %), and 0.38 TgN (±65 %) for the a posteriori anthropogenic, lightning and soil emissions, respectively, about 18–23 % higher than the respective a priori values. The enhancements in anthropogenic emissions are largest in cities and areas with extensive use of coal, particularly in the north in winter, as evident on the high-resolution grid. Derived soil emissions are consistent with recent bottom-up estimates. They are less than 6 % of anthropogenic emissions annually, increasing to about 13 % for July. Derived lightning emissions are about 3 % of anthropogenic emissions annually and about 10 % in July. Overall, anthropogenic emissions are found to be the dominant source of NO x over East China with important implications for nitrogen control.