Grantee Research Project Results
2012 Progress Report: Constraining ammonia emissions and PM2.5 control efficiencies with a new combination of satellite data, surface observations and adjoint modeling techniques
EPA Grant Number: R834559Title: Constraining ammonia emissions and PM2.5 control efficiencies with a new combination of satellite data, surface observations and adjoint modeling techniques
Investigators: Henze, Daven K
Institution: University of Colorado at Boulder
EPA Project Officer: Chung, Serena
Project Period: May 1, 2010 through April 30, 2013 (Extended to April 30, 2014)
Project Period Covered by this Report: May 1, 2012 through April 30,2013
Project Amount: $249,942
RFA: Novel Approaches to Improving Air Pollution Emissions Information (2009) RFA Text | Recipients Lists
Research Category: Air Quality and Air Toxics , Air
Objective:
The project goal is to reduce existing uncertainties in current estimates of NH3 emissions in order to better characterize and control distributions of ne particulate matter (PM2.5) and reactive nitrogen. The specific research objectives are to:
- quantify the magnitude and variability, both geographical and seasonal, of US NH3 emissions at a high spatial resolution.
- provide detailed estimates of PM2.5 control eciencies and how they will evolve owing to regulations that alter key balances among inorganic particulate species.
Progress Summary:
Top down constraints on NH3 emissions for April, July and October have been derived for North America, using observations from the years 2006-2009 and model simulations for the year 2008 run at 2 degree x 2.5 degree resolution are reported in Zhu et al. (2013). Overall, emissions appear to be underestimated in many regions, by up to a factor of three or more, although adjustments vary strongly by location and season. Possible explanations for the large adjustments are explored, such as the impacts of the diurnal variability of livestock sources making it appear that NH3 concentrations are underestimated, when in fact the timing of the emissions was contributing to a perceived underestimation by the satellite (Zhu et al., 2013; Joeng et al., submitted). We continue to address the impacts of diurnal variability and bidirectional exchange on the top-down emissions constraints. An active soil NH3 pool has been implemented in GEOS-Chem to see if late summer emissions may in fact be a result of evaded fertilizer earlier in the year, rather than fresh livestock emissions. Further, model resolution and instrument sampling limits are being explored, with future work using nested model simulations at the 0.5 degree x 0.666 degree resolution.
Building on the source attribution study of Paulot et al. (2012), additional top-down constraints on NH3 sources are derived using the GEOS-Chem adjoint model and wet deposition measurements (Paulot et al., submitted). These emission constraints are also explained with a new bottom-up NH3 inventory (MASAGE NH3). This approach nds that emissions in current inventories may be too high in parts of the eastern United States, but are likely underestimated in many midwestern regions during spring and fall. The overall results agree well with the satellite constraints in spring and fall, but there is still signicant discrepancy in July.
Changing our estimates of NH3 sources impacts model estimates of ammonium nitrate formation, and also the amount by which NH3 governs PM levels relative to other precursors such as SO2 and NOx. Despite high NH3 concentrations in some seasons, and constraints on these levels developed through satellite observations from TES (Shephard et al., 2011) and IASI (Kharol et al., 2013) or deposition (Paulot et al., submitted), PM2.5 concentrations in Asia appear to be most persistently influenced year round by NOx sources. In the U.S., ongoing work focuses on the impacts of the diurnal variability of NH3 on PM2.5 via ammonium nitrate aerosol. We have also examined the impacts of changing NH3 and NOx emissions on reactive nitrogen deposition following RCP emissions scenarios (Paulot et al., 2013).
Future Activities:
The remaining eorts will focus on non-attainment modeling and evaluation of emissions control eciencies. For this purpose the nested GEOS-Chem adjoint model will be used for sensitivity analysis over the US. We will consider both present day and future emissions scenarios. In addition, will also complete a study using deposition observations as an alternative means of constraining the NH3 inverse model.Journal Articles on this Report : 7 Displayed | Download in RIS Format
Other project views: | All 49 publications | 10 publications in selected types | All 10 journal articles |
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Kharol SK, Martin RV, Philip S, Vogel S, Henze DK, Chen D, Wang Y, Zhang Q, Heald CL. Persistent sensitivity of Asian aerosol to emissions of nitrogen oxides. Geophysical Research Letters 2013;40(5):1021-1026. |
R834559 (2012) R834559 (Final) |
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Paulot F, Jacob DJ, Henze DK. Sources and processes contributing to nitrogen deposition: an adjoint model analysis applied to biodiversity hotspots worldwide. Environmental Science & Technology 2013;47(7):3226-3233. |
R834559 (2011) R834559 (2012) R834559 (Final) |
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Paulot F, Jacob DJ, Pinder RW, Bash JO, Travis K, Henze DK. Ammonia emissions in the United States, European Union, and China derived by high-resolution inversion of ammonium wet deposition data: interpretation with a new agricultural emissions inventory (MASAGE_NH3). Journal of Geophysical Research–Atmospheres 2014;119(7):4343-4364. |
R834559 (2012) R834559 (Final) |
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Pinder RW, Walker JT, Bash JO, Cady-Pereira KE, Henze DK, Luo M, Osterman GB, Shephard MW. Quantifying spatial and seasonal variability in atmospheric ammonia with in situ and space-based observations. Geophysical Research Letters 2011;38(4):L04802 (5 pp.). |
R834559 (2010) R834559 (2011) R834559 (2012) R834559 (Final) |
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Shephard MW, Cady-Pereira KE, Luo M, Henze DK, Pinder RW, Walker JT, Rinsland CP, Bash JO, Zhu L, Payne VH, Clarisse L. TES ammonia retrieval strategy and global observations of the spatial and seasonal variabiity of ammonia. Atmospheric Chemistry and Physics 2011;11(20):10743-10763. |
R834559 (2010) R834559 (2011) R834559 (2012) R834559 (Final) |
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Wells KC, Millet DB, Cady-Pereira KE, Shephard MW, Henze DK, Bousserez N, Apel EC, de Gouw J, Warneke C, Singh HB. Quantifying global terrestrial methanol emissions using observations from the TES satellite sensor. Atmospheric Chemistry and Physics 2014;14(5):2555-2570. |
R834559 (2012) R834559 (Final) |
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Zhu L, Henze DK, Cady-Pereira KE, Shephard MW, Luo M, Pinder RW, Bash JO, Jeong G-R. Constraining U.S. ammonia emissions using TES remote sensing observations and the GEOS-Chem adjoint model. Journal of Geophysical Research–Atmospheres 2013;118(8):3355-3368. |
R834559 (2011) R834559 (2012) R834559 (Final) |
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Supplemental Keywords:
ammonia, emissions, inverse modeling, adjoint sensitivity, environmental policy, air quality regulations, ne particulate matter, aerosols, remote sensing, data assimilation, 4D-Var, public health, eutrophication;Progress and Final Reports:
Original AbstractThe perspectives, information and conclusions conveyed in research project abstracts, progress reports, final reports, journal abstracts and journal publications convey the viewpoints of the principal investigator and may not represent the views and policies of ORD and EPA. Conclusions drawn by the principal investigators have not been reviewed by the Agency.