scholarly journals Carbonaceous aerosols in China: top-down constraints on primary sources and estimation of secondary contribution

2011 ◽  
Vol 11 (10) ◽  
pp. 28219-28272 ◽  
Author(s):  
T.-M. Fu ◽  
J. J. Cao ◽  
X. Y. Zhang ◽  
S. C. Lee ◽  
Q. Zhang ◽  
...  
Keyword(s):  
Eastern China ◽  
Western China ◽  
Spatiotemporal Variability ◽  
Anthropogenic Source ◽  
Carbonaceous Aerosols ◽  
Top Down ◽  
Bottom Up ◽  
Secondary Sources ◽  
Secondary Formation ◽  
Emission Estimate

Abstract. We simulate elemental carbon (EC) and organic carbon (OC) aerosols in China and compare model results to surface measurements at Chinese rural and background sites, with the goal of deriving "top-down" emission estimates of EC and OC, as well as better quantifying the secondary sources of OC. We include in the model state-of-the-science Chinese "bottom-up" emission inventories for EC (1.92 Tg C yr−1) and OC (3.95 Tg C yr−1), as well as updated secondary OC formation pathways. The average simulated annual mean EC concentration at rural and background site is 1.1 μg C m−3, 56% lower than the observed 2.5 μg C m−3. The average simulated annual mean OC concentration at rural and background sites is 3.4 μg C m−3, 76% lower than the observed 14 μg C m−3. Multiple regression to fit surface monthly mean EC observations at rural and background sites yields best estimate of Chinese EC source of 3.05 ± 0.78 Tg C yr−1. Based on the top-down EC emission estimate and observed seasonal primary OC/EC ratios, we estimate Chinese OC total emissions to be 6.67 ± 1.30 Tg C yr−1. Using these top-down estimates, the simulated average annual mean EC concentration at rural and background sites significantly improved to 1.9 μg C m−3. However, the model still significantly underestimates observed OC in all seasons (simulated average annual mean OC at rural and background sites is 5.4 μg C m−3), with little skill in capturing the spatiotemporal variability. Secondary formation accounts for 21% of Chinese annual mean surface OC in the model, with isoprene being the most important precursor. In summer, as high as 62% of the observed surface OC may be due to secondary formation in eastern China. Our analysis points to three shortcomings in the current bottom-up inventories of Chinese carbonaceous aerosols: (1) the anthropogenic source is severely underestimated, particularly for OC; (2) there is a missing source in western China, likely associated with the use of biofuels or other low-quality fuels for heating; and (3) sources in fall are not well represented, either because the seasonal shifting of emissions and/or secondary formation are poorly captured or because specific fall emission events are missing. More regional measurements with better spatiotemporal coverage are needed to resolve these shortcomings.

scholarly journals Carbonaceous aerosols in China: top-down constraints on primary sources and estimation of secondary contribution

2012 ◽  
Vol 12 (5) ◽  
pp. 2725-2746 ◽  
Author(s):  
T.-M. Fu ◽  
J. J. Cao ◽  
X. Y. Zhang ◽  
S. C. Lee ◽  
Q. Zhang ◽  
...  
Keyword(s):  
Eastern China ◽  
Western China ◽  
Spatiotemporal Variability ◽  
Anthropogenic Source ◽  
Carbonaceous Aerosols ◽  
Top Down ◽  
Bottom Up ◽  
Secondary Sources ◽  
Secondary Formation ◽  
Emission Estimate

Abstract. We simulated elemental carbon (EC) and organic carbon (OC) aerosols in China and compared model results to surface measurements at Chinese rural and background sites, with the goal of deriving "top-down" emission estimates of EC and OC, as well as better quantifying the secondary sources of OC. We included in the model state-of-the-science Chinese "bottom-up" emission inventories for EC (1.92 TgC yr−1) and OC (3.95 TgC yr−1), as well as updated secondary OC formation pathways. The average simulated annual mean EC concentration at rural and background sites was 1.1 μgC m−3, 56% lower than the observed 2.5 μgC m−3. The average simulated annual mean OC concentration at rural and background sites was 3.4 μgC m−3, 76% lower than the observed 14 μgC m−3. Multiple regression to fit surface monthly mean EC observations at rural and background sites yielded the best estimate of Chinese EC source of 3.05 ± 0.78 TgC yr−1. Based on the top-down EC emission estimate and observed seasonal primary OC/EC ratios, we estimated Chinese OC emissions to be 6.67 ± 1.30 TgC yr−1. Using these top-down estimates, the simulated average annual mean EC concentration at rural and background sites was significantly improved to 1.9 μgC m−3. However, the model still significantly underestimated observed OC in all seasons (simulated average annual mean OC at rural and background sites was 5.4 μgC m−3), with little skill in capturing the spatiotemporal variability. Secondary formation accounts for 21% of Chinese annual mean surface OC in the model, with isoprene being the most important precursor. In summer, as high as 62% of the observed surface OC may be due to secondary formation in eastern China. Our analysis points to four shortcomings in the current bottom-up inventories of Chinese carbonaceous aerosols: (1) the anthropogenic source is underestimated on a national scale, particularly for OC; (2) the spatiotemporal distributions of emissions are misrepresented; (3) there is a missing source in western China, likely associated with the use of biofuels or other low-quality fuels for heating; and (4) sources in fall are not well represented, either because the seasonal shifting of emissions and/or secondary formation are poorly captured or because specific fall emission events are missing. In addition, secondary production of OC in China is severely underestimated. More regional measurements with better spatiotemporal coverage are needed to resolve these shortcomings.

scholarly journals Exploiting satellite measurements to reduce uncertainties in UK bottom-up NO<sub>x</sub> emission estimates

2021 ◽  
Author(s):  
Richard J. Pope ◽  
Rebecca Kelly ◽  
Eloise A. Marais ◽  
Ailish M. Graham ◽  
Chris Wilson ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Spatiotemporal Variability ◽  
Nox Emissions ◽  
Ozone Monitoring Instrument ◽  
Top Down ◽  
Bottom Up ◽  
Emissions Inventory ◽  
Monitoring Instrument ◽  
Hazardous Pollutants ◽  
The Uk

Abstract. Nitrogen oxides (NOx, NO+NO2) are potent air pollutants which directly impact on human health and which aid the formation of other hazardous pollutants such as ozone (O3) and particulate matter. In this study, we use satellite tropospheric column nitrogen dioxide (TCNO2) data to evaluate the spatiotemporal variability and magnitude of the United Kingdom (UK) bottom-up National Atmospheric Emissions Inventory (NAEI) NOx emissions. Although emissions and TCNO2 represent different quantities, for UK city sources we find a spatial correlation of ~0.5 between the NAEI NOx emissions and TCNO2 from the high-spatial-resolution TROPOspheric Monitoring Instrument (TROPOMI), suggesting a good spatial distribution of emission sources in the inventory. Between 2005 and 2015, the NAEI total UK NOx emissions and long-term TCNO2 record from the Ozone Monitoring Instrument (OMI), averaged over England, show decreasing trends of 4.4 % and 2.2 %, respectively. Top-down NOx emissions were derived in this study by applying a simple mass balance approach to TROPOMI observed downwind NO2 plumes from city sources. Overall, these top-down estimates were consistent with the NAEI, but for larger cities such as London and Manchester the inventory is significantly (> 25 %) less than the top-down emissions. This NAEI NOx emission underestimate is supported by comparing simulations from the GEOS-Chem atmospheric chemistry model, driven by the NAEI emissions, with satellite and surface NO2 observations over the UK. This yields substantial model negative biases, providing further evidence to demonstrate that the NAEI may be underestimating NOx emissions in London and Manchester.

scholarly journals Estimation of fossil-fuel CO<sub>2</sub> emissions using satellite measurements of "proxy" species

2016 ◽  
Vol 16 (21) ◽  
pp. 13509-13540 ◽  
Author(s):  
Igor B. Konovalov ◽  
Evgeny V. Berezin ◽  
Philippe Ciais ◽  
Grégoire Broquet ◽  
Ruslan V. Zhuravlev ◽  
...  
Keyword(s):  
Co2 Emissions ◽  
Co2 Emission ◽  
Emission Inventory ◽  
Fossil Fuel ◽  
Inventory Data ◽  
Satellite Measurements ◽  
Top Down ◽  
Bottom Up ◽  
Study Region ◽  
Emission Estimate

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.

scholarly journals Observationally-constrained carbonaceous aerosol source estimates for the Pearl River Delta area of China

2015 ◽  
Vol 15 (22) ◽  
pp. 33583-33629 ◽  
Author(s):  
N. Li ◽  
T.-M. Fu ◽  
J. J. Cao ◽  
J. Y. Zheng ◽  
Q. Y. He ◽  
...  
Keyword(s):  
Pearl River Delta ◽  
River Delta ◽  
Carbonaceous Aerosol ◽  
Pearl River ◽  
Aerosol Formation ◽  
Top Down ◽  
Secondary Sources ◽  
The Pearl River Delta ◽  
Emission Estimate ◽  
The Pearl River

Abstract. We simulated elemental carbon (EC) and organic carbon (OC) aerosols over the Pearl River Delta (PRD) area of China and compared the results to seasonal surface measurements, with the aim of quantifying carbonaceous aerosol sources from a "top-down" perspective. Our regional model was driven by current-best estimates of PRD EC (39.5 Gg C yr−1) and OC (32.8 Gg C yr−1) emissions and included updated secondary organic aerosol formation pathways. The simulated annual mean EC and OC concentrations were 4.0 and 7.7 μg C m−3, respectively, lower than the observed annual mean EC and OC concentrations (4.5 and 13.1 μg C m−3, respectively). We used multiple regression to match the simulated EC against seasonal mean observations. The resulting top-down estimate for EC emission in the PRD area was 52.9 ± 8.0 Gg C yr−1. We estimated the OC emission in the PRD area to be 60.2 ± 10.3 Gg C yr−1, based on the top-down EC emission estimate and the primary OC / EC ratios derived from bottom-up statistics. Using these top-down emission estimates, the simulated average annual mean EC and OC concentrations were improved to 4.4 and 9.5 μg C m−3, respectively, closer to the observations. Secondary sources accounted for 42 % of annual mean surface OC in our top-down simulations, with biogenic VOCs being the most important precursors.

scholarly journals Supplementary material to "Top-down and bottom-up estimates of anthropogenic methyl bromide emissions from eastern China"

2021 ◽  
Author(s):  
Haklim Choi ◽  
Mi-Kyung Park ◽  
Paul J. Fraser ◽  
Hyeri Park ◽  
Sohyeon Geum ◽  
...  
Keyword(s):  
Methyl Bromide ◽  
Eastern China ◽  
Top Down ◽  
Bottom Up ◽  
Supplementary Material

scholarly journals Estimation of fossil-fuel CO<sub>2</sub> emissions using satellite measurements of "proxy" species

2016 ◽  
Author(s):  
Igor B. Konovalov ◽  
Evgeny V. Berezin ◽  
Philippe Ciais ◽  
Grégoire Broquet ◽  
Ruslan B. Zhuravlev ◽  
...  
Keyword(s):  
Co2 Emissions ◽  
Co2 Emission ◽  
Emission Inventory ◽  
Fossil Fuel ◽  
Inventory Data ◽  
Satellite Measurements ◽  
Top Down ◽  
Bottom Up ◽  
Study Region ◽  
Emission Estimate

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.

scholarly journals Airborne formaldehyde and volatile organic compound measurements over the Daesan petrochemical complex on Korea’s northwest coast during the Korea-United States Air Quality study

Elem Sci Anth ◽  
2020 ◽  
Vol 8 (1) ◽  
Author(s):  
Alan Fried ◽  
James Walega ◽  
Petter Weibring ◽  
Dirk Richter ◽  
Isobel J. Simpson ◽  
...  
Keyword(s):  
United States ◽  
Air Quality ◽  
Mass Balance ◽  
Northwest Coast ◽  
Top Down ◽  
Bottom Up ◽  
Petrochemical Complex ◽  
Volatile Organic ◽  
Emission Estimate ◽  
Mass Balance Approach

The U.S. National Aeronautics and Space Administration in partnership with Korea’s National Institute of Environmental Research embarked on the Korea-United States Air Quality (KORUS-AQ) study to address air quality issues over the Korean peninsula. Underestimation of volatile organic compound (VOC) emissions from various large facilities on South Korea’s northwest coast may contribute to this problem, and this study focuses on quantifying top-down emissions of formaldehyde (CH2O) and VOCs from the largest of these facilities, the Daesan petrochemical complex, and comparisons with the latest emission inventories. To accomplish this and additional goals discussed herein, this study employed a number of measurements acquired during KORUS-AQ onboard the NASA DC-8 aircraft during three Daesan overflights on June 2, 3, and 5, 2016, in conjunction with a mass balance approach. The measurements included fast airborne measurements of CH2O and ethane from an infrared spectrometer, additional fast measurements from other instruments, and a suite of 33 VOC measurements acquired by the whole air sampler. The mass balance approach resulted in consistent top-down yearly Daesan VOC emission flux estimates, which averaged (61 ± 14) × 103 MT/year for the 33 VOC compounds, a factor of 2.9 ± 0.6 (±1.0) higher than the bottom-up inventory value. The top-down Daesan emission estimate for CH2O and its four primary precursors averaged a factor of 4.3 ± 1.5 (± 1.9) times higher than the bottom-up inventory value. The uncertainty values in parentheses reflect upper limits for total uncertainty estimates. The resulting averaged top-down Daesan emission estimate for sulfur dioxide (SO2) yielded a ratio of 0.81–1.0 times the bottom-up SO2 inventory, and this provides an important cross-check on the accuracy of our mass balance analysis.

scholarly journals Top-down estimates of anthropogenic VOC emissions in South Korea using formaldehyde vertical column densities from aircraft during the KORUS-AQ campaign

Elem Sci Anth ◽  
2021 ◽  
Vol 9 (1) ◽  
Author(s):  
Hyeong-Ahn Kwon ◽  
Rokjin J. Park ◽  
Yujin J. Oak ◽  
Caroline R. Nowlan ◽  
Scott J. Janz ◽  
...  
Keyword(s):  
South Korea ◽  
Transport Model ◽  
Anthropogenic Source ◽  
Chemical Transport Model ◽  
Top Down ◽  
Vertical Column ◽  
Bottom Up ◽  
Mixing Ratios ◽  
Source Regions ◽  
Volatile Organic

Nonmethane volatile organic compounds (NMVOCs) result in ozone and aerosol production that adversely affects the environment and human health. For modeling purposes, anthropogenic NMVOC emissions have been typically compiled using the “bottom-up” approach. To minimize uncertainties of the bottom-up emission inventory, “top-down” NMVOC emissions can be estimated using formaldehyde (HCHO) observations. In this study, HCHO vertical column densities (VCDs) obtained from the Geostationary Trace gas and Aerosol Sensor Optimization spectrometer during the Korea–United States Air Quality campaign were used to constrain anthropogenic volatile organic compound (AVOC) emissions in South Korea. Estimated top-down AVOC emissions differed from those of the up-to-date bottom-up inventory over major anthropogenic source regions by factors of 1.0 ± 0.4 to 6.9 ± 3.9. Our evaluation using a 3D chemical transport model indicates that simulated HCHO mixing ratios using the top-down estimates were in better agreement with observations onboard the DC-8 aircraft during the campaign relative to those with the bottom-up emission, showing a decrease in model bias from –25% to –13%. The top-down analysis used in this study, however, has some limitations related to the use of HCHO yields, background HCHO columns, and AVOC speciation in the bottom-up inventory, resulting in uncertainties in the AVOC emission estimates. Our attempt to constrain diurnal variations of the AVOC emissions using the aircraft HCHO VCDs was compromised by infrequent aircraft observations over the same source regions. These limitations can be overcome with geostationary satellite observations by providing hourly HCHO VCDs.

scholarly journals Conflicting estimates of natural geologic methane emissions

Elem Sci Anth ◽  
2021 ◽  
Vol 9 (1) ◽  
Author(s):  
B. F. Thornton ◽  
G. Etiope ◽  
S. Schwietzke ◽  
A. V. Milkov ◽  
R. W. Klusman ◽  
...  
Keyword(s):  
Fossil Fuel ◽  
Ice Cores ◽  
Methane Emissions ◽  
Ch4 Emission ◽  
Top Down ◽  
Bottom Up ◽  
Ch4 Emissions ◽  
Emission Estimate

Global bottom-up and top-down estimates of natural, geologic methane (CH4) emissions (average approximately 45 Tg yr–1) have recently been questioned by near-zero (approximately 1.6 Tg yr–1) estimates based on measurements of 14CH4 trapped in ice cores, which imply that current fossil fuel industries’ CH4 emissions are underestimated by 25%–40%. As we show here, such a global near-zero geologic CH4 emission estimate is incompatible with multiple independent, bottom-up emission estimates from individual natural geologic seepage areas, each of which is of the order of 0.1–3 Tg yr–1. Further research is urgently needed to resolve the conundrum before rejecting either method or associated emission estimates in global CH4 accounting.

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