scholarly journals Multiannual changes of CO<sub>2</sub> emissions in China: indirect estimates derived from satellite measurements of tropospheric NO<sub>2</sub> columns

2013 ◽  
Vol 13 (18) ◽  
pp. 9415-9438 ◽  
Author(s):  
E. V. Berezin ◽  
I. B. Konovalov ◽  
P. Ciais ◽  
A. Richter ◽  
S. Tao ◽  
...  

Abstract. Multiannual satellite measurements of tropospheric NO2 columns are used for evaluation of CO2 emission changes in China in the period from 1996 to 2008. Indirect top-down annual estimates of CO2 emissions are derived from the satellite NO2 column measurements by means of a simple inverse modeling procedure involving simulations performed with the CHIMERE mesoscale chemistry–transport model and the CO2-to-NOx emission ratios from the Emission Database for Global Atmospheric Research (EDGAR) global anthropogenic emission inventory and Regional Emission Inventory in Asia (REAS). Exponential trends in the normalized time series of annual emissions are evaluated separately for the periods from 1996 to 2001 and from 2001 to 2008. The results indicate that the both periods manifest strong positive trends in the CO2 emissions, and that the trend in the second period was significantly larger than the trend in the first period. Specifically, the trends in the first and second periods are best estimated to be in the range from 3.7 to 8.3 and from 11.0 to 13.2% per year, respectively, taking into account statistical uncertainties and differences between the CO2-to-NOx emission ratios from the EDGAR and REAS inventories. Comparison of our indirect top-down estimates of the CO2 emission changes with the corresponding bottom-up estimates provided by the EDGAR (version 4.2) and Global Carbon Project (GCP) glomal emission inventories reveals that while acceleration of the CO2 emission growth in the considered period is a common feature of both kinds of estimates, nonlinearity in the CO2 emission changes may be strongly exaggerated in the global emission inventories. Specifically, the atmospheric NO2 observations do not confirm the existence of a sharp bend in the emission inventory data time series in the period from 2000 to 2002. A significant quantitative difference is revealed between the bottom-up and indirect top-down estimates of the CO2 emission trend in the period from 1996 to 2001 (specifically, the trend was not positive according to the global emission inventories, but is strongly positive in our estimates). These results confirm the findings of earlier studies that indicated probable large uncertainties in the energy production and other activity data for China from international energy statistics used as the input information in the global emission inventories. For the period from 2001 to 2008, some quantitative differences between the different kinds of estimates are found to be in the range of possible systematic uncertainties associated with our estimation method. In general, satellite measurements of tropospheric NO2 are shown to be a useful source of information on CO2 sources collocated with sources of nitrogen oxides; the corresponding potential of these measurements should be exploited further in future studies.

2013 ◽  
Vol 13 (1) ◽  
pp. 255-309 ◽  
Author(s):  
E. V. Berezin ◽  
I. B. Konovalov ◽  
P. Ciais ◽  
A. Richter ◽  
S. Tao ◽  
...  

Abstract. Multi-annual satellite measurements of tropospheric NO2 columns are used for evaluation of CO2 emission changes in China in the period from 1996 to 2008. Indirect annual top-down estimates of CO2 emissions are derived from the satellite NO2 columns measurements by means of a simple inverse modeling procedure involving simulations performed with the CHIMERE mesoscale chemistry transport model and the CO2 to NOx emission ratios from the Emission Database for Global Atmospheric Research version 4.2 (EDGAR v4.2) global anthropogenic emission inventory. Exponential trends in the normalized time series of annual emission are evaluated separately for the periods from 1996 to 2001 and from 2001 to 2008. The results indicate that the both periods manifest strong positive trends in the CO2 emissions, and that the trend in the second period was significantly larger than the trend in the first period. Specifically, the trends in the first and second periods are estimated to be in the range from 3.7 to 8.0 and from 9.5 to 13.0 percent per year, respectively, taking into account both statistical and probable systematic uncertainties. Comparison of our top-down estimates of the CO2 emission changes with the corresponding bottom-up estimates provided by EDGAR v4.2 and Global Carbon Project (GCP) emission inventories reveals that while acceleration of the CO2 emission growth in the considered period is a common feature of the both kinds of estimates, nonlinearity in the CO2 emission changes may be strongly exaggerated in the emission inventories. Specifically, the atmospheric NO2 observations do not confirm the existence of a sharp bend in the emission inventory data time series in the period from 2000 to 2002. A significant quantitative difference is revealed between the bottom-up and top-down estimates of the CO2 emission trend in the period from 1996 to 2001 (specifically, the trend was not positive according to the emission inventories, but is strongly positive in our estimates). These results confirm the findings of earlier studies which indicated probable large uncertainties in the energy production and other activity data from international energy statistics used as the input information in the emission inventories for China. For the period from 2001 to 2008, the different kinds of estimates agree within the uncertainty range. In general, satellite measurements of tropospheric NO2 are shown to be a useful source of information on CO2 sources colocated with sources of nitrogen oxides; the corresponding potential of these measurements should be exploited further in future studies.


2016 ◽  
Vol 16 (21) ◽  
pp. 13509-13540 ◽  
Author(s):  
Igor B. Konovalov ◽  
Evgeny V. Berezin ◽  
Philippe Ciais ◽  
Grégoire Broquet ◽  
Ruslan V. Zhuravlev ◽  
...  

Abstract. Fossil-fuel (FF) burning releases carbon dioxide (CO2) together with many other chemical species, some of which, such as nitrogen dioxide (NO2) and carbon monoxide (CO), are routinely monitored from space. This study examines the feasibility of estimation of FF CO2 emissions from large industrial regions by using NO2 and CO column retrievals from satellite measurements in combination with simulations by a mesoscale chemistry transport model (CTM). To this end, an inverse modeling method is developed that allows estimating FF CO2 emissions from different sectors of the economy, as well as the total CO2 emissions, in a given region. The key steps of the method are (1) inferring "top-down" estimates of the regional budget of anthropogenic NOx and CO emissions from satellite measurements of proxy species (NO2 and CO in the case considered) without using formal a priori constraints on these budgets, (2) the application of emission factors (the NOx-to-CO2 and CO-to-CO2 emission ratios in each sector) that relate FF CO2 emissions to the proxy species emissions and are evaluated by using data of "bottom-up" emission inventories, and (3) cross-validation and optimal combination of the estimates of CO2 emission budgets derived from measurements of the different proxy species. Uncertainties in the top-down estimates of the NOx and CO emissions are evaluated and systematic differences between the measured and simulated data are taken into account by using original robust techniques validated with synthetic data. To examine the potential of the method, it was applied to the budget of emissions for a western European region including 12 countries by using NO2 and CO column amounts retrieved from, respectively, the OMI and IASI satellite measurements and simulated by the CHIMERE mesoscale CTM, along with the emission conversion factors based on the EDGAR v4.2 emission inventory. The analysis was focused on evaluation of the uncertainty levels for the top-down NOx and CO emission estimates and "hybrid" estimates (that is, those based on both atmospheric measurements of a given proxy species and respective bottom-up emission inventory data) of FF CO2 emissions, as well as on examining consistency between the FF NO2 emission estimates derived from measurements of the different proxy species. It is found that NO2 measurements can provide much stronger constraints to the total annual FF CO2 emissions in the study region than CO measurements, the accuracy of the NO2-measurement-based CO2 emission estimate being mostly limited by the uncertainty in the top-down NOx emission estimate. Nonetheless, CO measurements are also found to be useful as they provide additional constraints to CO2 emissions and enable evaluation of the hybrid FF CO2 emission estimates obtained from NO2 measurements. Our most reliable estimate for the total annual FF CO2 emissions in the study region in 2008 (2.71 ± 0.30 Pg CO2) is found to be about 11 and 5 % lower than the respective estimates based on the EDGAR v.4.2 (3.03 Pg CO2) and CDIAC (2.86 Pg CO2) emission inventories, with the difference between our estimate and the CDIAC inventory data not being statistically significant. In general, the results of this study indicate that the proposed method has the potential to become a useful tool for identification of possible biases and/or inconsistencies in the bottom-up emission inventory data regarding CO2, NOx, and CO emissions from fossil-fuel burning in different regions of the world.


2016 ◽  
Author(s):  
Igor B. Konovalov ◽  
Evgeny V. Berezin ◽  
Philippe Ciais ◽  
Grégoire Broquet ◽  
Ruslan B. Zhuravlev ◽  
...  

Abstract. Fossil fuel (FF) burning releases carbon dioxide (CO2) together with many other chemical species, some of which, such as, e.g., nitrogen dioxide (NO2) and carbon monoxide (CO), are routinely monitored from space. This study examines the feasibility of estimation of FF CO2 emissions from large industrial regions by using NO2 and CO column retrievals from satellite measurements in combination with simulations by a mesoscale chemistry transport model (CTM). To this end, an inverse modeling method is developed that allows estimating FF CO2 emissions from different sectors of the economy, as well as the total CO2 emissions, in a given region. The key steps of the method are (1) inferring "top-down" estimates of the regional budget of anthropogenic emissions of proxy species (that is, NOx and CO in the case considered) from satellite measurements without using formal a priori constraints on these budgets, (2) application of emission factors (the NOx-to-CO2 and CO-to-CO2 emission ratios in each sector) that relate FF CO2 emissions to the emissions of the proxy species and are evaluated by using data of "bottom-up" emission inventories, (3) cross-validation and optimal combination of the estimates of CO2 emission budgets derived from measurements of the different proxy species. Uncertainties in the top-down estimates of the emissions of the proxy species are evaluated and systematic differences between the measured and simulated data are taken into account by using original robust techniques validated with synthetic data. To examine the potential of the method, it was applied to the budget of emissions for a western European region including 12 countries by using NO2 and CO column amounts retrieved from, respectively, the OMI and IASI satellite measurements and simulated by the CHIMERE mesoscale CTM, along with the emission conversion factors based on the EDGAR v4.2 emission inventory. The analysis was focused on evaluation of the uncertainty levels for the "top-down" NOx and CO emission estimates and "hybrid" estimates (that is, those based on both atmospheric measurements of a given proxy species and respective "bottom-up" emission inventory data) of FF CO2 emissions, as well as on examining consistency between the FF СO2 emission estimates derived from measurements of the different proxy species. It is found that NO2 measurements can provide much stronger constraints to the total annual FF CO2 emissions in the study region than CO measurements, the accuracy of the NO2-measurement-based CO2 emission estimate being mostly limited by the uncertainty in the top-down NOx emission estimate. Nonetheless, CO measurements are also found to be useful as they provide additional constraints to CO2 emissions and enable evaluation of the hybrid FF CO2 emission estimates obtained from NO2 measurements. Our most reliable estimate for the total annual FF CO2 emissions in the study region in 2008 (2.71±0.30 Pg CO2) is found to be about 11 % and 5 % lower than the respective estimates based on the EDGAR v.4.2 (3.03 Pg CO2) and CDIAC (2.86 Pg CO2) emission inventories, with the difference between our estimate and the CDIAC inventory data being not statistically significant. In general, the results of this study indicate that the proposed method has a potential to become a useful tool for identification of possible biases and/or inconsistencies in the bottom-up emission inventory data regarding CO2, NOx and CO emissions from fossil fuel burning in different regions of the world.


2020 ◽  
Author(s):  
Wei He ◽  
Fei Jiang ◽  
Shuzhuang Feng ◽  
Ngoc Tu Nguyen ◽  
Hengmao Wang ◽  
...  

&lt;p&gt;Accurate estimation of anthropogenic CO&lt;sub&gt;2&lt;/sub&gt; emissions (ACE) is of great importance for climate change mitigation, however, it is quite challenging.&amp;#160; Co-emitted gases, e.g. CO and NO&lt;sub&gt;x&lt;/sub&gt;, have been reported to be useful for tracking ACE. Here we estimated ACE of China based on &amp;#8220;proxy&amp;#8221; species (i.e. CO and NO&lt;sub&gt;x&lt;/sub&gt;) inversions with emission ratios of CO&lt;sub&gt;2 &lt;/sub&gt;and the &amp;#8220;proxy&amp;#8221; species and evaluated the estimates using ground CO&lt;sub&gt;2&lt;/sub&gt; measurements of three tower stations in population-dense areas based on the Stochastic Time-Inverted Lagrangian Transport (STILT) modeling driven by the Global Data Assimilation System (GDAS) meteorology. An ensemble of ACE of China were estimated from different combinations of anthropogenic CO or NO&lt;sub&gt;x&lt;/sub&gt; flux estimates and emission ratios, where the CO or NO&lt;sub&gt;x&lt;/sub&gt; fluxes were estimated from in-situ measured concentration data or satellite column concentration data, and the emission ratios were derived from two emission inventory datasets, i.e. multi-resolution emission inventory for China (MEIC) and Peking University global emission inventories (PKU-FUEL). We found all CO&lt;sub&gt;2&lt;/sub&gt; simulations with &amp;#8220;proxy&amp;#8221; based ACE estimates (either using in-situ or satellite data) in one year clearly fitted better to observations than those with inventory datasets did, especially during winter and early spring. Meanwhile, large mismatches between simulations and observations were found for some periods, which indicated the use of CO or NO&lt;sub&gt;x &lt;/sub&gt;to track ACE may be not suitable for a whole year. Our preliminary result demonstrates the potential to use atmospheric &amp;#8220;proxy&amp;#8221; species to track anthropogenic CO&lt;sub&gt;2&lt;/sub&gt; emissions in China.&lt;/p&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;


2020 ◽  
Author(s):  
Erin E. McDuffie ◽  
Steven J. Smith ◽  
Patrick O'Rourke ◽  
Kushal Tibrewal ◽  
Chandra Venkataraman ◽  
...  

Abstract. Global anthropogenic emission inventories remain vital for understanding the fate and transport of atmospheric pollution, as well as the resulting impacts on the environment, human health, and society. Rapid changes in today’s society require that these inventories provide contemporary estimates of multiple atmospheric pollutants with both source sector and fuel-type information to understand and effectively mitigate future impacts. To fill this need, we have updated the open-source Community Emissions Data System (CEDS) (Hoesly et al., 2019) to develop a new global emission inventory, CEDSGBD-MAPS. This inventory includes emissions of seven key atmospheric pollutants (NOx, CO, SO2, NH3, NMVOCs, BC, OC) over the time period from 1970–2017 and reports annual country-total emissions as a function of 11 anthropogenic sectors (agriculture, energy generation, industrial processes, transportation (on-road and non-road), residential, commercial, and other sectors (RCO), waste, solvent use, and international-shipping) and four fuel categories (total coal, solid biofuel, and the sum of liquid fuels and natural gas combustion, plus remaining process-level emissions). The CEDSGBD-MAPS inventory additionally includes global gridded (0.5°×0.5°) emission fluxes with monthly time resolution for each compound, sector, and fuel-type to facilitate their use in earth system models. CEDSGBD-MAPS utilizes updated activity data, updates to the core CEDS default calibration procedure, and modifications to the final procedures for emissions gridding and aggregation to retain sector and fuel-specific information. Relative to the previous CEDS data released for CMIP6 (Hoesly et al., 2018), these updates extend the emission estimates from 2014 to 2017 and improve the overall agreement between CEDS and two widely used global bottom-up emission inventories. The CEDSGBD-MAPS inventory provides the most contemporary global emission estimates to-date for these key atmospheric pollutants and is the first to provide global estimates for these species as a function of multiple fuel-types across multiple source sectors. Dominant sources of global NOx and SO2 emissions in 2017 include the combustion of oil, gas, and coal in the energy and industry sectors, as well as on-road transportation and international shipping for NOx. Dominant sources of global CO emissions in 2017 include on-road transportation and residential biofuel combustion. Dominant global sources of carbonaceous aerosol in 2017 include residential biofuel combustion, on-road transportation (BC only), as well as emissions from waste. Global emissions of NOx, SO2, CO, BC, and OC all peak in 2012 or earlier, with more recent emission reductions driven by large changes in emissions from China, North America, and Europe. In contrast, global emissions of NH3 and NMVOCs continuously increase between 1970 and 2017, with agriculture serving as a major source of global NH3 emissions and solvent use, energy, residential, and the on-road transport sectors as major sources of global NMVOCs. Due to similar development methods and underlying datasets, the CEDSGBD-MAPS emissions are expected to have consistent sources of uncertainty as other bottom-up inventories, including uncertainties in the underlying activity data and sector- and region-specific emission factors. The CEDSGBD-MAPS source code is publicly available online through GitHub: https://github.com/emcduffie/CEDS/tree/CEDS_GBD-MAPS. The CEDSGBD-MAPS emission inventory dataset (both annual country-total and global gridded files) is publicly available and registered under: https://doi.org/10.5281/zenodo.3754964 (McDuffie et al., 2020).


2013 ◽  
Vol 13 (23) ◽  
pp. 11819-11838 ◽  
Author(s):  
R. Hossaini ◽  
H. Mantle ◽  
M. P. Chipperfield ◽  
S. A. Montzka ◽  
P. Hamer ◽  
...  

Abstract. Emissions of halogenated very short-lived substances (VSLS) are poorly constrained. However, their inclusion in global models is required to simulate a realistic inorganic bromine (Bry) loading in both the troposphere, where bromine chemistry perturbs global oxidising capacity, and in the stratosphere, where it is a major sink for ozone (O3). We have performed simulations using a 3-D chemical transport model (CTM) including three top-down and a single bottom-up derived emission inventory of the major brominated VSLS bromoform (CHBr3) and dibromomethane (CH2Br2). We perform the first concerted evaluation of these inventories, comparing both the magnitude and spatial distribution of emissions. For a quantitative evaluation of each inventory, model output is compared with independent long-term observations at National Oceanic and Atmospheric Administration (NOAA) ground-based stations and with aircraft observations made during the NSF (National Science Foundation) HIAPER Pole-to-Pole Observations (HIPPO) project. For CHBr3, the mean absolute deviation between model and surface observation ranges from 0.22 (38%) to 0.78 (115%) parts per trillion (ppt) in the tropics, depending on emission inventory. For CH2Br2, the range is 0.17 (24%) to 1.25 (167%) ppt. We also use aircraft observations made during the 2011 Stratospheric Ozone: Halogen Impacts in a Varying Atmosphere (SHIVA) campaign, in the tropical western Pacific. Here, the performance of the various inventories also varies significantly, but overall the CTM is able to reproduce observed CHBr3 well in the free troposphere using an inventory based on observed sea-to-air fluxes. Finally, we identify the range of uncertainty associated with these VSLS emission inventories on stratospheric bromine loading due to VSLS (BryVSLS). Our simulations show BryVSLS ranges from ~4.0 to 8.0 ppt depending on the inventory. We report an optimised estimate at the lower end of this range (~4 ppt) based on combining the CHBr3 and CH2Br2 inventories which give best agreement with the compilation of observations in the tropics.


2020 ◽  
Author(s):  
Yun fat Lam ◽  
Shimul Roy ◽  
Ka Wing Chui

&lt;p&gt;In ASEAN (Southeast Asia) countries, anthropogenic emissions have increased significantly over the last two decades from a variety of sources, including power and heating, industries, road-transportation, residential, and agricultural activities. In this study, we analyzed different emission inventories (i.e., MICS-Asia, REAS, EDGAR) to provide the integrated emissions for ASEAN during the period 2000-2010. The study found that anthropogenic emission contribution from ASEAN countries to the total Asian emission was notable during that period. For instance, from the MIX-Asian EI, our analysis shows that the average contribution was the highest from the transportation sector (34%), followed by residential (29%), power (24%), and industrial sector (14%), respectively in 2010. However, similar to the sector-specific emission contribution in 2000 in ASEAN countries, residential sector was the most significant contributor for CO (53%), PM10 (48%), PM2.5 (63%), BC (76%), OC (79%) in 2010, although it is in decreasing trend compared to other sectors. On the contrary, emission contribution of SO2 was the highest from the industrial sector (47%), followed by power (36%), while NOx and NMVOC were contributed mainly by transportation sector (55% and 45%, respectively). Spatially, the emission intensities of SO2, CO, NOx, NMVOC, PM10, PM2.5, BC, OC, and CO2 were high in the major urban cities of Thailand, Vietnam, Malaysia, Philippines, and Indonesia except CH4, N2O, and NH3, which were high in the rural areas of ASEAN countries.&lt;/p&gt;


2016 ◽  
Author(s):  
Thérèse Salameh ◽  
Agnès Borbon ◽  
Charbel Afif ◽  
Stéphane Sauvage ◽  
Thierry Leonardis ◽  
...  

Abstract. The relative importance of Eastern Mediterranean emissions is suspected to be largely underestimated compared to other regions worldwide. Here we use detailed speciated measurements of VOCs (volatile organic compounds) to evaluate the spatial heterogeneity of VOC urban emission composition and the consistency of regional and global emission inventories downscaled to Lebanon (EMEP, ACCMIP, and MACCity). The assessment was conducted through the comparison of the emission ratios extracted from the emission inventories to the ones obtained from the hourly observations collected at a sub-urban site in Beirut, Lebanon during summertime and wintertime ECOCEM campaigns. The observed ERs were calculated by two independent methods. ER values from both methods agree very well (difference up to 10 %) and are comparable to the ones of the road transport sector from near-field measurements for more than 80 % of the species. There is no significant seasonality in ER for more than 90 % of the species unlike the seasonality usually observed in other cities worldwide. Regardless of the season, ERs agree within a factor of 2 between Beirut and other representative worldwide cities except for the unburned fuel fraction and ethane. ERs of aromatics (benzene excepted) are higher in Beirut compared to northern post-industrialized countries and even the Middle Eastern city Mecca. The comparison of the observed ER relative to CO and to acetylene as well as the ratios of every NMVOC to each of the other NMVOCs (NMVOCi) to the ones extracted from ACCMIP and MACCity global emission inventories suggests that the overall speciation of anthropogenic sources for major hydrocarbons that act as ozone and SOA precursors in ACCMIP is reasonably represented. The comparison of the specific road transport ER relative to acetylene derived from near-field measurements to ER from ACCMIP and EMEP emission inventories for road transport sector showed that ER from the road transport sector are usually consistent within a factor of 2 with the regional emission inventory EMEP while xylenes and toluene are underestimated over a factor of 2 by ACCMIP. The observed heterogeneity of anthropogenic VOC emission composition between Middle Eastern cities can be significant for reactive VOC but is not depicted by global emission inventories. This suggests that systematic and detailed measurements are needed in the Eastern Mediterranean Basin in order to better constrain emission inventory.


2014 ◽  
Vol 14 (18) ◽  
pp. 10363-10381 ◽  
Author(s):  
G. C. M. Vinken ◽  
K. F. Boersma ◽  
J. D. Maasakkers ◽  
M. Adon ◽  
R. V. Martin

Abstract. Biogenic NOx emissions from soils are a large natural source with substantial uncertainties in global bottom-up estimates (ranging from 4 to 15 Tg N yr−1). We reduce this range in emission estimates, and present a top-down soil NOx emission inventory for 2005 based on retrieved tropospheric NO2 columns from the Ozone Monitoring Instrument (OMI). We use a state-of-science soil NOx emission inventory (Hudman et al., 2012) as a priori in the GEOS-Chem chemistry transport model to identify 11 regions where tropospheric NO2 columns are dominated by soil NOx emissions. Strong correlations between soil NOx emissions and simulated NO2 columns indicate that spatial patterns in simulated NO2 columns in these regions indeed reflect the underlying soil NOx emissions. Subsequently, we use a mass-balance approach to constrain emissions for these 11 regions on all major continents using OMI observed and GEOS-Chem simulated tropospheric NO2 columns. We find that responses of simulated NO2 columns to changing NOx emissions are suppressed over low NOx regions, and account for these non-linearities in our inversion approach. In general, our approach suggests that emissions need to be increased in most regions. Our OMI top-down soil NOx inventory amounts to 10.0 Tg N for 2005 when only constraining the 11 regions, and 12.9 Tg N when extrapolating the constraints globally. Substantial regional differences exist (ranging from −40% to +90%), and globally our top-down inventory is 4–35% higher than the GEOS-Chem a priori (9.6 Tg N yr−1). We evaluate NO2 concentrations simulated with our new OMI top-down inventory against surface NO2 measurements from monitoring stations in Africa, the USA and Europe. Although this comparison is complicated by several factors, we find an encouraging improved agreement when using the OMI top-down inventory compared to using the a priori inventory. To our knowledge, this study provides, for the first time, specific constraints on soil NOx emissions on all major continents using OMI NO2 columns. Our results rule out the low end of reported soil NOx emission estimates, and suggest that global emissions are most likely around 12.9 ± 3.9 Tg N yr−1.


2014 ◽  
Vol 14 (10) ◽  
pp. 14683-14724
Author(s):  
G. C. M. Vinken ◽  
K. F. Boersma ◽  
J. D. Maasakkers ◽  
M. Adon ◽  
R. V. Martin

Abstract. Biogenic NOx emissions from soils are a large natural source with substantial uncertainties in global bottom-up estimates (ranging from 4 to 27 Tg N yr−1). We reduce this range in emission estimates, and present a top-down soil NOx emission inventory for 2005 based on retrieved tropospheric NO2 columns from the Ozone Monitoring Instrument (OMI). We used a state-of-science soil NOx emission inventory (Hudman et al., 2012) as a priori in the GEOS-Chem chemistry transport model to identify 11 regions where tropospheric NO2 columns are dominated by soil NOx emissions. Strong correlations between soil NOx emissions and simulated NO2 columns indicated that spatial patterns in simulated NO2 columns in these regions indeed reflect the underlying soil NOx emissions. Subsequently, we used a mass-balance approach to constrain emissions for these 11 regions on all major continents using OMI observed and GEOS-Chem simulated tropospheric NO2 columns. We found that responses of simulated NO2 columns to changing NOx emissions were suppressed over low NOx regions, and accounted for these non-linearities in our inversion approach. In general, our approach suggests that emissions need to be increased in most regions. Our OMI top-down soil NOx inventory amounts to 10.0 Tg N for 2005 when only constraining the 11 regions, and 12.9 Tg N when extrapolating the constraints globally. Substantial regional differences exist (ranging from −40% to +90%), and globally our top-down inventory is 4–35% higher than the GEOS-Chem a priori (9.6 Tg N yr−1). We evaluated NO2 concentrations simulated with our new OMI top-down inventory against surface NO2 measurements from monitoring stations in Africa, the USA, and Europe. Although this comparison is complicated by several factors, we find an encouraging improved agreement when using the OMI top-down inventory compared to using the a priori inventory. To our knowledge, this study provides, for the first time, specific constraints on soil NOx emissions on all major continents using OMI NO2 columns. Our results rule out the high end of reported soil NOx emission estimates, and suggest that global emissions are most likely around 10–13 Tg N yr−1.


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