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 Evaluating the impact of storage-and-release on aircraft-based mass-balance methodology using a regional air-quality model

2021 ◽  
Vol 21 (20) ◽  
pp. 15461-15491
Author(s):  
Sepehr Fathi ◽  
Mark Gordon ◽  
Paul A. Makar ◽  
Ayodeji Akingunola ◽  
Andrea Darlington ◽  
...  
Keyword(s):  
Air Quality ◽  
Mass Balance ◽  
Emission Rate ◽  
Meteorological Conditions ◽  
Emission Rates ◽  
Top Down ◽  
Retrieval Accuracy ◽  
Balance Approach ◽  
The Impact ◽  
Mass Balance Approach

Abstract. We investigate the potential for aircraft-based top-down emission rate retrieval over- and under-estimation using a regional chemical transport model, the Global Environmental Multiscale-Modeling Air-Quality and CHemistry (GEM-MACH). In our investigations we consider the application of the mass-balance approach in the Top-down Emission Rate Retrieval Algorithm (TERRA). Aircraft-based mass-balance retrieval methodologies such as TERRA require relatively constant meteorological conditions and source emission rates to reliably estimate emission rates from aircraft observations. Avoiding cases where meteorology and emission rates change significantly is one means of reducing emissions retrieval uncertainty, and quantitative metrics that may be used for retrieval accuracy estimation are therefore desirable. Using these metrics has the potential to greatly improve emission rate retrieval accuracy. Here, we investigate the impact of meteorological variability on mass-balance emission rate retrieval accuracy by using model-simulated fields as a proxy for real-world chemical and meteorological fields, in which virtual aircraft sampling of the GEM-MACH output was used for top-down mass balance estimates. We also explore the impact of upwind emissions from nearby sources on the accuracy of the retrieved emission rates. This approach allows the state of the atmosphere used for top-down estimates to be characterized in time and 3D space; the input meteorology and emissions are “known”, and thus potential means for improving emission rate retrievals and determining the factors affecting retrieval accuracy may be investigated. We found that emissions retrieval accuracy is correlated with three key quantitative criteria, evaluated a priori from forecasts and/or from observations during the sampling period: (1) changes to the atmospheric stability (described as the change in gradient Richardson number), (2) variations in the direction of transport, as a result of plume vertical motion and in the presence of vertical wind shear, and (3) the combined effect of the upwind-to-downwind concentration ratio and the upwind-to-downwind concentration standard deviations. We show here that cases where these criteria indicate high temporal variability and/or high upwind emissions can result in “storage-and-release” events within the sampled region (control volume), which decrease emission rate retrieval accuracy. Storage-and-release events may contribute the bulk of mass-balance emission rate retrieval under- and over-estimates, ranging in the tests carried out here from −25 % to 24 % of the known (input) emissions, with a median of −2 %. Our analysis also includes two cases with unsuitable meteorological conditions and/or significant upwind emissions to demonstrate conditions which may result in severe storage, which in turn cause emission rate under-estimates by the mass-balance approach. We also introduce a sampling strategy whereby the emission rate retrieval under- and over-estimates associated with storage-and-release are greatly reduced (to −14 % to +5 %, respectively, relative to the magnitude of the known emissions). We recommend repeat flights over a given facility and/or time-consecutive upwind and downwind (remote) vertical profiling of relevant fields (e.g., tracer concentrations) in order to measure and account for the factors associated with storage-and-release events, estimate the temporal trends in the evolution of the system during the flight/sampling time, and partially correct for the effects of meteorological variability and upwind emissions.

scholarly journals Evaluating the Impact of Storage-and-Release on Aircraft-based Mass-Balance Methodology Using a Regional Air Quality Model

2021 ◽  
Author(s):  
Sepehr Fathi ◽  
Mark David Gordon ◽  
Paul Andrew Makar ◽  
Ayodeji Akingunola ◽  
Andrea Darlington ◽  
...  
Keyword(s):  
Air Quality ◽  
Mass Balance ◽  
Emission Rate ◽  
Meteorological Conditions ◽  
Emission Rates ◽  
Top Down ◽  
Retrieval Accuracy ◽  
Balance Approach ◽  
The Impact ◽  
Mass Balance Approach

Abstract. We investigate the potential for aircraft-based top-down emission rate retrieval over- and under-estimation using a regional chemical transport model, the Global Environmental Multiscale-Modeling Air-Quality and CHemistry (GEM-MACH). In our investigations we consider the application of the mass-balance approach in the Top-down Emission Rate Retrieval Algorithm (TERRA). Aircraft-based mass-balance retrieval methodologies such as TERRA require relatively constant meteorological conditions and source emission rates to reliably estimate emission rates from aircraft observations. Avoiding cases where meteorology and emission rates change significantly is one means of reducing emissions retrieval uncertainty, and quantitative metrics that may be used for retrieval accuracy estimation are therefore desirable. Using these metrics has the potential to greatly improve emission rate retrieval accuracy. Here, we investigate the impact of meteorological variability on mass-balance emission rate retrieval accuracy by using model simulated fields as a proxy for real world chemical and meteorological fields, in which virtual aircraft sampling of the GEM-MACH output was used for top-down mass balance estimates. We also explore the impact of upwind emissions from nearby sources on the accuracy of the retrieved emission rates. This approach allows the state of the atmosphere used for top-down estimates to be characterized in time and 3D space; the input meteorology and emissions are “known”, and thus potential means for improving emission rate retrievals and determining the factors affecting retrieval accuracy may be investigated. We found that emissions retrieval accuracy is correlated with three key quantitative criteria, evaluated a priori from forecasts and/or from observations during the sampling period: (1) changes to the atmospheric stability (described as the change in gradient Richardson number), (2) variations in the direction of transport, as a result of plume vertical motion and in the presence of vertical wind shear, and (3) the combined effect of the upwind to downwind concentration ratio and the upwind to downwind concentration standard deviations. We show here that cases where these criteria indicate high temporal variability and/or high upwind emissions can result in “Storage-and-Release” events within the sampled region (control volume), which decrease emission rate retrieval accuracy. Storage-and-release events may contribute the bulk of mass-balance emission rate retrieval under- and over-estimates, ranging in the tests carried out here from −25 % to 24 % of the known (input) emissions, with a median of −2 %. Our analysis also includes two cases with unsuitable meteorological conditions and/or significant upwind emissions to demonstrate conditions which may result in severe storage, which in turn cause emission rate underestimates by the mass-balance approach. We also introduce a flight strategy whereby the emission rate retrieval under- and over-estimates associated with storage-and-release are greatly reduced (to −14 % to +5 % respectively, relative to the magnitude of the known emissions). We recommend repeat flights over a given facility in order to measure and account for the factors associated with storage-and-release events – to estimate the temporal trends in the evolution of the system during the flight/sampling time, and partially correct for the effects of meteorological variability and upwind emissions. Our analysis allows the increased costs associated with longer flight times to be weighed against quantitatively reduced uncertainty in the emission rate estimates.

scholarly journals Improvement from the satellite-derived NO<sub>x</sub> emissions on air quality modeling and its effect on ozone and secondary inorganic aerosol formation in Yangtze River Delta, China

2020 ◽  
Author(s):  
Yang Yang ◽  
Yu Zhao ◽  
Lei Zhang ◽  
Jie Zhang ◽  
Xin Huang ◽  
...  
Keyword(s):  
Air Quality ◽  
Model Performance ◽  
Yangtze River Delta ◽  
Nox Emissions ◽  
Top Down ◽  
Bottom Up ◽  
Inorganic Aerosols ◽  
Quality Modeling ◽  
Emission Estimation ◽  
Reduced Rate

Abstract. We developed a top-down methodology combining the inversed chemistry transport modeling and satellite-derived tropospheric vertical column of NO2, and estimated the NOx emissions of Yangtze River Delta (YRD) region at a horizontal resolution of 9 km for January, April, July and October 2016. The effect of the top-down emission estimation on air quality modeling, and the response of ambient ozone (O3) and secondary inorganic aerosols (SO42−, NO3−, and NH4+, SNA) to the changed precursor emissions were evaluated with the Community Multi-scale Air Quality (CMAQ) system. The top-down estimates of NOx emissions were smaller than those in a national emission inventory, MEIC (i.e., the bottom-up estimates), for all the four months, and the monthly mean was calculated at 260.0 Gg/month, 24 % less than the bottom-up one. The NO2 concentrations simulated with the bottom-up estimate of NOx emissions were clearly higher than the ground observation, indicating the possible overestimation in current emission inventory attributed to its insufficient consideration of recent emission control in the region. The model performance based on top-down estimate was much better, and the biggest change was found for July with the normalized mean bias (NMB) and normalized mean error (NME) reduced from 111 % to −0.4 % and from 111 % to 33 %, respectively. The results demonstrate the improvement of NOx emission estimation with the nonlinear inversed modeling and satellite observation constraint. With the smaller NOx emissions in the top-down estimate than the bottom-up one, the elevated concentrations of ambient O3 were simulated for most YRD and they were closer to observation except for July, implying the VOC (volatile organic compound)-limit regime of O3 formation. With available ground observations of SNA in the YRD, moreover, better model performance of NO3− and NH4+ were achieved for most seasons, implying the effectiveness of precursor emission estimation on the simulation of secondary inorganic aerosols. Through the sensitivity analysis of O3 formation for April 2016, the decreased O3 concentrations were found for most YRD region when only VOCs emissions were reduced or the reduced rate of VOCs emissions was two times of that of NOx, implying the crucial role of VOCs control on O3 pollution abatement. The SNA level for January 2016 was simulated to decline 12 % when 30 % of NH3 emissions were reduced, while the change was much smaller with the same reduced rate for SO2 or NOx. The result suggests that reducing NH3 emissions was the most effective way to alleviate SNA pollution for YRD in winter.

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 Estimating European volatile organic compound emissions using satellite observations of formaldehyde from the Ozone Monitoring Instrument

2010 ◽  
Vol 10 (23) ◽  
pp. 11501-11517 ◽  
Author(s):  
G. Curci ◽  
P. I. Palmer ◽  
T. P. Kurosu ◽  
K. Chance ◽  
G. Visconti
Keyword(s):  
Satellite Observations ◽  
Atmospheric Composition ◽  
Ozone Monitoring Instrument ◽  
Top Down ◽  
Bottom Up ◽  
Voc Emissions ◽  
The Balkans ◽  
Monitoring Instrument ◽  
Volatile Organic ◽  
Ozone Monitoring

Abstract. Emission of non-methane Volatile Organic Compounds (VOCs) to the atmosphere stems from biogenic and human activities, and their estimation is difficult because of the many and not fully understood processes involved. In order to narrow down the uncertainty related to VOC emissions, which negatively reflects on our ability to simulate the atmospheric composition, we exploit satellite observations of formaldehyde (HCHO), an ubiquitous oxidation product of most VOCs, focusing on Europe. HCHO column observations from the Ozone Monitoring Instrument (OMI) reveal a marked seasonal cycle with a summer maximum and winter minimum. In summer, the oxidation of methane and other long-lived VOCs supply a slowly varying background HCHO column, while HCHO variability is dominated by most reactive VOC, primarily biogenic isoprene followed in importance by biogenic terpenes and anthropogenic VOCs. The chemistry-transport model CHIMERE qualitatively reproduces the temporal and spatial features of the observed HCHO column, but display regional biases which are attributed mainly to incorrect biogenic VOC emissions, calculated with the Model of Emissions of Gases and Aerosol from Nature (MEGAN) algorithm. These "bottom-up" or a-priori emissions are corrected through a Bayesian inversion of the OMI HCHO observations. Resulting "top-down" or a-posteriori isoprene emissions are lower than "bottom-up" by 40% over the Balkans and by 20% over Southern Germany, and higher by 20% over Iberian Peninsula, Greece and Italy. We conclude that OMI satellite observations of HCHO can provide a quantitative "top-down" constraint on the European "bottom-up" VOC inventories.

Preview of the future application of the environmental geo-satellites data using aircraft platform: Estimation of anthropogenic VOC emissions from formaldehyde columns

2020 ◽  
Author(s):  
Rokjin Park ◽  
Hyeong-Ahn Kwon ◽  
Yujin Oak
Keyword(s):  
Air Quality ◽  
South Korea ◽  
Future Application ◽  
Air Quality Model ◽  
Quality Model ◽  
Top Down ◽  
Vertical Column ◽  
Bottom Up ◽  
Ozone Sensitivity ◽  
Emission Changes

&lt;p&gt;The Geostationary Environment Monitoring Spectrometer (GEMS) will be launched in February 2020 and will provide hourly observations of atmospheric compositions in the daytime. Prior to the GEMS launch, we explore an application of GEMS data as constraints for estimating anthropogenic volatile organic compound (AVOC) emissions in South Korea using formaldehyde (HCHO) vertical column densities observations from the Geostationary Trace gas and Aerosol Sensor Optimization (GeoTASO) onboard the B200 aircraft during the KORUS-AQ campaign. Our top-down estimates of total AVOC emissions are higher by a factor of four over the petrochemical industries compared to the bottom-up emissions. However, the national AVOC emissions from the top-down estimates are by 37% lower than those of the bottom-up emission inventory in South Korea. We also show that hourly column observations of HCHO can improve not only the total magnitude of AVOC emissions but also their diurnal variation, which is poorly constrained and used in air quality models. Our hourly estimates of AVOC emissions may, thus, improve air quality model simulations in which the simulated ozone sensitivity to AVOC emission changes are also investigated.&lt;/p&gt;

scholarly journals Contributions to OH reactivity from unexplored volatile organic compounds measured by PTR-ToF-MS – a case study in a suburban forest of the Seoul metropolitan area during the Korea–United States Air Quality Study (KORUS-AQ) 2016

2021 ◽  
Vol 21 (8) ◽  
pp. 6331-6345
Author(s):  
Dianne Sanchez ◽  
Roger Seco ◽  
Dasa Gu ◽  
Alex Guenther ◽  
John Mak ◽  
...  
Keyword(s):  
United States ◽  
Air Quality ◽  
Volatile Organic Compounds ◽  
Organic Compounds ◽  
Mass Spectrometer ◽  
Metropolitan Area ◽  
Seoul Metropolitan Area ◽  
Volatile Organic ◽  
Quality Study ◽  
Tof Ms

Abstract. We report OH reactivity observations by a chemical ionization mass spectrometer–comparative reactivity method (CIMS-CRM) instrument in a suburban forest of the Seoul metropolitan area (SMA) during the Korea–United States Air Quality Study (KORUS-AQ 2016) from mid-May to mid-June of 2016. A comprehensive observational suite was deployed to quantify reactive trace gases inside of the forest canopy including a high-resolution proton transfer reaction time-of-flight mass spectrometer (PTR-ToF-MS). An average OH reactivity of 30.7±5.1 s−1 was observed, while the OH reactivity calculated from CO, NO+NO2 (NOx), ozone (O3), sulfur dioxide (SO2), and 14 volatile organic compounds (VOCs) was 11.8±1.0 s−1. An analysis of 346 peaks from the PTR-ToF-MS accounted for an additional 6.0±2.2 s−1 of the total measured OH reactivity, leaving 42.0 % missing OH reactivity. A series of analyses indicate that the missing OH reactivity most likely comes from VOC oxidation products of both biogenic and anthropogenic origin.

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