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. 2019 Jul 27;124(14):8336-8359.
doi: 10.1029/2019JD030243. Epub 2019 Jul 31.

SO2 Emission Estimates Using OMI SO2 Retrievals for 2005-2017

Zhen Qu  1 , Daven K Henze  1 , Can Li  2   3 , Nicolas Theys  4 , Yi Wang  5 , Jun Wang  5 , Wei Wang  6 , Jihyun Han  7 , Changsub Shim  7 , Russell R Dickerson  8 , Xinrong Ren  8   9
Affiliations

SO2 Emission Estimates Using OMI SO2 Retrievals for 2005-2017

Zhen Qu et al. J Geophys Res Atmos. .

Abstract

SO2 column densities from Ozone Monitoring Instrument provide important information on emission trends and missing sources, but there are discrepancies between different retrieval products. We employ three Ozone Monitoring Instrument SO2 retrieval products (National Aeronautics and Space Administration (NASA) standard (SP), NASA prototype, and BIRA) to study the magnitude and trend of SO2 emissions. SO2 column densities from these retrievals are most consistent when viewing angles and solar zenith angles are small, suggesting more robust emission estimates in summer and at low latitudes. We then apply a hybrid 4D-Var/mass balance emission inversion to derive monthly SO2 emissions from the NASA SP and BIRA products. Compared to HTAPv2 emissions in 2010, both posterior emission estimates are lower in United States, India, and Southeast China, but show different changes of emissions in North China Plain. The discrepancies between monthly NASA and BIRA posterior emissions in 2010 are less than or equal to 17% in China and 34% in India. SO2 emissions increase from 2005 to 2016 by 35% (NASA)-48% (BIRA) in India, but decrease in China by 23% (NASA)-33% (BIRA) since 2008. Compared to in situ measurements, the posterior GEOS-Chem surface SO2 concentrations have reduced NMB in China, the United States, and India but not in South Korea in 2010. BIRA posteriors have better consistency with the annual growth rate of surface SO2 measurement in China and spatial variability of SO2 concentration in China, South Korea, and India, whereas NASA SP posteriors have better seasonality. These evaluations demonstrate the capability to recover SO2 emissions using Ozone Monitoring Instrument observations.

Keywords: 4D‐Var; data assimilation; inverse modeling; mass balance; satellite observation; top‐down SO2 emission.

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Figures

Figure 1
Figure 1
Flight tracks of KORUS‐AQ measurements overlapped on surface SO2 concentration from the GEOS‐Chem simulation (a) at 2° × 2.5° in May 2016, (b) at 0.5° × 0.667° in May 2010, and (c) flight tracks of DISCOVER‐AQ overlapped on surface SO2 concentration from the GEOS‐Chem simulation 0.5° × 0.667° in July 2011.
Figure 2
Figure 2
East Asia SO2 SCDs from (first row) GEOS‐Chem, (second row) OMI, and (third row) the difference between the two for January 2010. GEOS‐Chem SCDs are sampled within half an hour of the OMI overpass time and at grid cells that contain OMI footprints. This comparison in the base year reflects differences in SO2 columns only caused by emissions.
Figure 3
Figure 3
Examples of vertical distribution of SO2 sensitivity (m) in the BIRA and NASA retrievals under (a) clear‐sky conditions (cloud fraction = 0, VZA = 56.61°), (b) cloud fraction between 0 and 0.1 (VZA = 56.62°), and (c) cloud fraction between 0.1 and 0.2 (VZA = 62.08°).
Figure 4
Figure 4
Comparison of GEOS‐Chem SO2 SCDs (DU) for different cloud fractions (CF) for January 2010.
Figure 5
Figure 5
The 4D‐Var updates to SO2 emissions (posterior‐prior) when constrained using the BIRA retrieval products in 2010.
Figure 6
Figure 6
Monthly SO2 emissions in China, South Korea, India, and United States (normalized to annual mean) in 2010 from nested simulations (0.5° × 0.667°). Posterior emissions are from 4D‐Var estimates.
Figure 7
Figure 7
Annual budget of SO2 emissions in (left) China and (right) India from 2005 to 2017. Coarse resolution refers to 2° × 2.5°; fine resolution refers to 0.5° × 0.667°.
Figure 8
Figure 8
Trends of SO2 column concentrations (left) including both positive and negative retrievals in U.S. regions and (right) over the East United States using only positive values or both positive and negative values.
Figure 9
Figure 9
Percent changes relative to 2010 in SO2 concentrations in China from surface measurements (from the 272 sites with data in every year from 2005 to 2012) and co‐located estimates from prior and posterior GEOS‐Chem simulations.
Figure 10
Figure 10
Comparison of GEOS‐Chem SO2 vertical profiles with (left) KORUS‐AQ DC‐8 aircraft measurements from 26 April to 18 June of 2016 and (right) DISCOVER‐AQ aircraft measurements over Virginia and Maryland in the United States from 8 June to 25 August 2011. The horizontal bars show the 25% and 75% quartiles of the measurements averaged at each height, and the year and horizontal resolution of the GEOS‐Chem simulations are indicated in the legends.
Figure A1
Figure A1
Annual mean of the difference between GEOS‐Chem and OMI SO2 SCD (NASA standard product) in 2010. Two cases are tested: (1) AMF = 0.36 applied to both model and OMI VCDs and (2) local AMFs applied to GEOS‐Chem and AMF = 0.36 applied to OMI VCD.
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