Evaluation of interactive and prescribed agricultural ammonia emissions for simulating atmospheric composition in CAM-chem

Vira, Julius; Hess, Peter; Ossohou, Money; Galy-Lacaux, Corinne

doi:10.5194/acp-22-1883-2022

Evaluation of interactive and prescribed agricultural ammonia emissions for simulating atmospheric composition in CAM-chem

Journal Article · Wed Feb 09 00:00:00 EST 2022 · Atmospheric Chemistry and Physics (Online)

DOI:https://doi.org/10.5194/acp-22-1883-2022· OSTI ID:1844277

; Hess, Peter; Ossohou, Money; Galy-Lacaux, Corinne

Abstract. Ammonia (NH3) plays a central role in the chemistry of inorganic secondary aerosols in the atmosphere. The largest emission sector for NH3 is agriculture, where NH3 is volatilized from livestock wastes and fertilized soils. Although the NH3 volatilization from soils is driven by the soil temperature and moisture, many atmospheric chemistry models prescribe the emission using yearly emission inventories and climatological seasonal variations. Here we evaluate an alternative approach where the NH3 emissions from agriculture are simulated interactively using the process model FANv2 (Flow of Agricultural Nitrogen, version 2) coupled to the Community Atmospheric Model with Chemistry (CAM-chem). We run a set of 6-year global simulations using the NH3 emission from FANv2 and three global emission inventories (EDGAR, CEDS and HTAP) and evaluate the model performance using a global set of multi-component (atmospheric NH3 and NH4+, and NH4+ wet deposition) in situ observations. Over East Asia, Europe and North America, the simulations with different emissions perform similarly when compared with the observed geographical patterns. The seasonal distributions of NH3 emissions differ between the inventories, and the comparison to observations suggests that both FANv2 and the inventories would benefit from more realistic timing of fertilizer applications. The largest differences between the simulations occur over data-scarce regions. In Africa, the emissions simulated by FANv2 are 200 %–300 % higher than in the inventories, and the available in situ observations from western and central Africa, as well as NH3 retrievals from the Infrared Atmospheric Sounding Interferometer (IASI) instrument, are consistent with the higher NH3 emissions as simulated by FANv2. Overall, in simulating ammonia and ammonium concentrations over regions with detailed regional emission inventories, the inventories based on these details (HTAP, CEDS) capture the atmospheric concentrations and their seasonal variability the best. However these inventories cannot capture the impact of meteorological variability on the emissions, nor can these inventories couple the emissions to the biogeochemical cycles and their changes with climate drivers. Finally, we show with sensitivity experiments that the simulated time-averaged nitrate concentration in air is sensitive to the temporal resolution of the NH3 emissions. Over the CASTNET monitoring network covering the US, resolving the NH3 emissions hourly instead monthly reduced the positive model bias from approximately 80 % to 60 % of the observed yearly mean nitrate concentration. This suggests that some of the commonly reported overestimation of aerosol nitrate over the US may be related to unresolved temporal variability in the NH3 emissions.

View Journal Article

Research Organization:: Cornell University, Ithaca, NY (United States)

Sponsoring Organization:: National Science Foundation; Strategic Research Council at the Academy of Finland; USDOE Office of Science (SC); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: SC0016361

OSTI ID:: 1844277

Alternate ID(s):: OSTI ID: 1981289

Journal Information:: Atmospheric Chemistry and Physics (Online), Journal Name: Atmospheric Chemistry and Physics (Online) Journal Issue: 3 Vol. 22; ISSN 1680-7324

Publisher:: Copernicus GmbHCopyright Statement

Country of Publication:: Germany

Language:: English

References (64)

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) Paulot, F.; Jacob, D. J.; Pinder, R. W. Journal of Geophysical Research: Atmospheres, Vol. 119, Issue 7 https://doi.org/10.1002/2013JD021130	journal	April 2014
Worldwide spatiotemporal atmospheric ammonia (NH ₃ ) columns variability revealed by satellite: NH ₃ SPATIOTEMPORAL VARIABILITY Van Damme, M.; Erisman, J. W.; Clarisse, L. Geophysical Research Letters, Vol. 42, Issue 20 https://doi.org/10.1002/2015GL065496	journal	October 2015
Importance of coarse‐mode nitrate produced via sea salt as atmospheric input to East Asian oceans Itahashi, Syuichi; Hayami, Hiroshi; Uno, Itsushi Geophysical Research Letters, Vol. 43, Issue 10 https://doi.org/10.1002/2016GL068722	journal	May 2016
Nitrogen deposition and plant biodiversity: past, present, and future Payne, Richard J.; Dise, Nancy B.; Field, Christopher D. Frontiers in Ecology and the Environment, Vol. 15, Issue 8 https://doi.org/10.1002/fee.1528	journal	September 2017
CLMcrop yields and water requirements: avoided impacts by choosing RCP 4.5 over 8.5 Levis, Samuel; Badger, Andrew; Drewniak, Beth Climatic Change, Vol. 146, Issue 3-4 https://doi.org/10.1007/s10584-016-1654-9	journal	March 2016
Rainwater Chemistry and Wet Deposition over the Wet Savanna Ecosystem of Lamto (Côte d'Ivoire) Yoboué, V.; Galy-Lacaux, C.; Lacaux, J. P. Journal of Atmospheric Chemistry, Vol. 52, Issue 2 https://doi.org/10.1007/s10874-005-0281-z	journal	October 2005
Rainwater chemistry and bulk atmospheric deposition in a tropical semiarid ecosystem: the Brazilian Caatinga Deusdará, K. R. L.; Forti, M. C.; Borma, L. S. Journal of Atmospheric Chemistry, Vol. 74, Issue 1 https://doi.org/10.1007/s10874-016-9341-9	journal	June 2016
Parameterization of surface resistances to gaseous dry deposition in regional-scale numerical models Wesely, M. L. Atmospheric Environment (1967), Vol. 23, Issue 6 https://doi.org/10.1016/0004-6981(89)90153-4	journal	January 1989
Wet deposition fluxes of atmospheric inorganic reactive nitrogen at an urban and rural site in the Indo-Gangetic Plain Singh, Saumya; Sharma, Anshu; Kumar, Bablu Atmospheric Pollution Research, Vol. 8, Issue 4 https://doi.org/10.1016/j.apr.2016.12.021	journal	July 2017
Observations of fine and coarse particle nitrate at several rural locations in the United States Lee, T.; Yu, X.; Ayres, B. Atmospheric Environment, Vol. 42, Issue 11 https://doi.org/10.1016/j.atmosenv.2007.05.016	journal	April 2008
Bottom-up uncertainty estimates of global ammonia emissions from global agricultural production systems Beusen, A. H. W.; Bouwman, A. F.; Heuberger, P. S. C. Atmospheric Environment, Vol. 42, Issue 24 https://doi.org/10.1016/j.atmosenv.2008.03.044	journal	August 2008
A global assessment of precipitation chemistry and deposition of sulfur, nitrogen, sea salt, base cations, organic acids, acidity and pH, and phosphorus Vet, Robert; Artz, Richard S.; Carou, Silvina Atmospheric Environment, Vol. 93 https://doi.org/10.1016/j.atmosenv.2013.10.060	journal	August 2014
Ammonia emissions in tropical biomass burning regions: Comparison between satellite-derived emissions and bottom-up fire inventories Whitburn, S.; Van Damme, M.; Kaiser, J. W. Atmospheric Environment, Vol. 121 https://doi.org/10.1016/j.atmosenv.2015.03.015	journal	November 2015
Trends and seasonal variability of atmospheric NO2 and HNO3 concentrations across three major African biomes inferred from long-term series of ground-based and satellite measurements Ossohou, M.; Galy-Lacaux, C.; Yoboué, V. Atmospheric Environment, Vol. 207 https://doi.org/10.1016/j.atmosenv.2019.03.027	journal	June 2019
Atmospheric organic and inorganic nitrogen inputs to coastal urban and montane Atlantic Forest sites in southeastern Brazil de Souza, Patricia A.; Ponette-González, Alexandra G.; de Mello, William Z. Atmospheric Research, Vol. 160 https://doi.org/10.1016/j.atmosres.2015.03.011	journal	June 2015
Intense Warming Will Significantly Increase Cropland Ammonia Volatilization Threatening Food Security and Ecosystem Health Shen, Huizhong; Chen, Yilin; Hu, Yongtao One Earth, Vol. 3, Issue 1 https://doi.org/10.1016/j.oneear.2020.06.015	journal	July 2020
Response of Inorganic PM to Precursor Concentrations Ansari, Asif S.; Pandis, Spyros N. Environmental Science & Technology, Vol. 32, Issue 18 https://doi.org/10.1021/es971130j	journal	September 1998
Sulfur chemistry in the National Center for Atmospheric Research Community Climate Model: Description, evaluation, features, and sensitivity to aqueous chemistry Barth, M. C.; Rasch, P. J.; Kiehl, J. T. Journal of Geophysical Research: Atmospheres, Vol. 105, Issue D1 https://doi.org/10.1029/1999JD900773	journal	January 2000
Gas/aerosol partitioning: 1. A computationally efficient model Metzger, Swen Journal of Geophysical Research, Vol. 107, Issue D16 https://doi.org/10.1029/2001JD001102	journal	January 2002
A dynamical ammonia emission parameterization for use in air pollution models Gyldenkærne, Steen Journal of Geophysical Research, Vol. 110, Issue D7 https://doi.org/10.1029/2004JD005459	journal	January 2005
Nitrogen and sulfur deposition on regional and global scales: A multimodel evaluation: MULTIMODEL GLOBAL DEPOSITION Dentener, F.; Drevet, J.; Lamarque, J. F. Global Biogeochemical Cycles, Vol. 20, Issue 4 https://doi.org/10.1029/2005GB002672	journal	October 2006
Global modeling of nitrate and ammonium: Interaction of aerosols and tropospheric chemistry Feng, Yan; Penner, Joyce E. Journal of Geophysical Research, Vol. 112, Issue D1 https://doi.org/10.1029/2005JD006404	journal	January 2007
Simulating Agriculture in the Community Land Model Version 5 Lombardozzi, Danica L.; Lu, Yaqiong; Lawrence, Peter J. Journal of Geophysical Research: Biogeosciences, Vol. 125, Issue 8 https://doi.org/10.1029/2019JG005529	journal	August 2020
A global high-resolution emission inventory for ammonia Bouwman, A. F.; Lee, D. S.; Asman, W. A. H. Global Biogeochemical Cycles, Vol. 11, Issue 4 https://doi.org/10.1029/97GB02266	journal	December 1997
Industrial and agricultural ammonia point sources exposed Van Damme, Martin; Clarisse, Lieven; Whitburn, Simon Nature, Vol. 564, Issue 7734 https://doi.org/10.1038/s41586-018-0747-1	journal	December 2018
Rural versus urban gaseous inorganic reactive nitrogen in the Indo-Gangetic plains (IGP) of India Singh, Saumya; Kulshrestha, U. C. Environmental Research Letters, Vol. 9, Issue 12 https://doi.org/10.1088/1748-9326/9/12/125004	journal	December 2014
Towards a climate-dependent paradigm of ammonia emission and deposition Sutton, Mark A.; Reis, Stefan; Riddick, Stuart N. Philosophical Transactions of the Royal Society B: Biological Sciences, Vol. 368, Issue 1621 https://doi.org/10.1098/rstb.2013.0166	journal	July 2013
Global ammonia emissions from synthetic nitrogen fertilizer applications in agricultural systems: Empirical and process‐based estimates and uncertainty Xu, Rongting; Tian, Hanqin; Pan, Shufen Global Change Biology, Vol. 25, Issue 1 https://doi.org/10.1111/gcb.14499	journal	November 2018
Changes in species richness and composition in European acidic grasslands over the past 70 years: the contribution of cumulative atmospheric nitrogen deposition: NITROGEN DEPOSITION AND SPECIES RICHNESS DuprÃ, Cecilia; Stevens, Carly J.; Ranke, Traute Global Change Biology, Vol. 16, Issue 1 https://doi.org/10.1111/j.1365-2486.2009.01982.x	journal	January 2010
MERRA: NASA’s Modern-Era Retrospective Analysis for Research and Applications Rienecker, Michele M.; Suarez, Max J.; Gelaro, Ronald Journal of Climate, Vol. 24, Issue 14 https://doi.org/10.1175/JCLI-D-11-00015.1	journal	July 2011
Interactive Crop Management in the Community Earth System Model (CESM1): Seasonal Influences on Land–Atmosphere Fluxes Levis, Samuel; Bonan, Gordon B.; Kluzek, Erik Journal of Climate, Vol. 25, Issue 14 https://doi.org/10.1175/JCLI-D-11-00446.1	journal	July 2012
Mapping the Global Distribution of Livestock Robinson, Timothy P.; Wint, G. R. William; Conchedda, Giulia PLoS ONE, Vol. 9, Issue 5 https://doi.org/10.1371/journal.pone.0096084	journal	May 2014
Atmospheric nitrogen budget in Sahelian dry savannas Delon, C.; Galy-Lacaux, C.; Boone, A. Atmospheric Chemistry and Physics, Vol. 10, Issue 6 https://doi.org/10.5194/acp-10-2691-2010	journal	January 2010
Long term measurements of sulfur dioxide, nitrogen dioxide, ammonia, nitric acid and ozone in Africa using passive samplers Adon, M.; Galy-Lacaux, C.; Yoboué, V. Atmospheric Chemistry and Physics, Vol. 10, Issue 15 https://doi.org/10.5194/acp-10-7467-2010	journal	January 2010
Atmospheric ammonia and particulate inorganic nitrogen over the United States Heald, C. L.; Collett, J. L.; Lee, T. Atmospheric Chemistry and Physics, Vol. 12, Issue 21 https://doi.org/10.5194/acp-12-10295-2012	journal	January 2012
Simulation of nitrate, sulfate, and ammonium aerosols over the United States Walker, J. M.; Philip, S.; Martin, R. V. Atmospheric Chemistry and Physics, Vol. 12, Issue 22 https://doi.org/10.5194/acp-12-11213-2012	journal	January 2012
Toward a more physical representation of precipitation scavenging in global chemistry models: cloud overlap and ice physics and their impact on tropospheric ozone Neu, J. L.; Prather, M. J. Atmospheric Chemistry and Physics, Vol. 12, Issue 7 https://doi.org/10.5194/acp-12-3289-2012	journal	January 2012
A global model simulation of present and future nitrate aerosols and their direct radiative forcing of climate Hauglustaine, D. A.; Balkanski, Y.; Schulz, M. Atmospheric Chemistry and Physics, Vol. 14, Issue 20 https://doi.org/10.5194/acp-14-11031-2014	journal	January 2014
HTAP_v2.2: a mosaic of regional and global emission grid maps for 2008 and 2010 to study hemispheric transport of air pollution Janssens-Maenhout, G.; Crippa, M.; Guizzardi, D. Atmospheric Chemistry and Physics, Vol. 15, Issue 19 https://doi.org/10.5194/acp-15-11411-2015	journal	January 2015
Global evaluation of ammonia bidirectional exchange and livestock diurnal variation schemes Zhu, L.; Henze, D.; Bash, J. Atmospheric Chemistry and Physics, Vol. 15, Issue 22 https://doi.org/10.5194/acp-15-12823-2015	journal	January 2015
Sensitivity of nitrate aerosols to ammonia emissions and to nitrate chemistry: implications for present and future nitrate optical depth Paulot, F.; Ginoux, P.; Cooke, W. F. Atmospheric Chemistry and Physics, Vol. 16, Issue 3 https://doi.org/10.5194/acp-16-1459-2016	journal	January 2016
Satellite evidence of substantial rain-induced soil emissions of ammonia across the Sahel Hickman, Jonathan E.; Dammers, Enrico; Galy-Lacaux, Corinne Atmospheric Chemistry and Physics, Vol. 18, Issue 22 https://doi.org/10.5194/acp-18-16713-2018	journal	January 2018
The underappreciated role of nonvolatile cations in aerosol ammonium-sulfate molar ratios Guo, Hongyu; Nenes, Athanasios; Weber, Rodney J. Atmospheric Chemistry and Physics, Vol. 18, Issue 23 https://doi.org/10.5194/acp-18-17307-2018	journal	January 2018
Agricultural ammonia emissions in China: reconciling bottom-up and top-down estimates Zhang, Lin; Chen, Youfan; Zhao, Yuanhong Atmospheric Chemistry and Physics, Vol. 18, Issue 1 https://doi.org/10.5194/acp-18-339-2018	journal	January 2018
High-resolution hybrid inversion of IASI ammonia columns to constrain US ammonia emissions using the CMAQ adjoint model Chen, Yilin; Shen, Huizhong; Kaiser, Jennifer Atmospheric Chemistry and Physics, Vol. 21, Issue 3 https://doi.org/10.5194/acp-21-2067-2021	journal	January 2021
Aerosol acidity and liquid water content regulate the dry deposition of inorganic reactive nitrogen Nenes, Athanasios; Pandis, Spyros N.; Kanakidou, Maria Atmospheric Chemistry and Physics, Vol. 21, Issue 8 https://doi.org/10.5194/acp-21-6023-2021	journal	January 2021
Dry and wet deposition of inorganic nitrogen compounds to a tropical pasture site (Rondônia, Brazil) Trebs, I.; Lara, L. L.; Zeri, L. M. M. Atmospheric Chemistry and Physics, Vol. 6, Issue 2 https://doi.org/10.5194/acp-6-447-2006	journal	January 2006
Nitrate aerosols today and in 2030: a global simulation including aerosols and tropospheric ozone Bauer, S. E.; Koch, D.; Unger, N. Atmospheric Chemistry and Physics, Vol. 7, Issue 19 https://doi.org/10.5194/acp-7-5043-2007	journal	January 2007
Long term precipitation chemistry and wet deposition in a remote dry savanna site in Africa (Niger) Galy-Lacaux, C.; Laouali, D.; Descroix, L. Atmospheric Chemistry and Physics, Vol. 9, Issue 5 https://doi.org/10.5194/acp-9-1579-2009	journal	January 2009
Version 2 of the IASI NH₃ neural network retrieval algorithm: near-real-time and reanalysed datasets Van Damme, Martin; Whitburn, Simon; Clarisse, Lieven Atmospheric Measurement Techniques, Vol. 10, Issue 12 https://doi.org/10.5194/amt-10-4905-2017	journal	January 2017
Atmospheric ammonia retrieval from the TANSO-FTS/GOSAT thermal infrared sounder Someya, Yu; Imasu, Ryoichi; Shiomi, Kei Atmospheric Measurement Techniques, Vol. 13, Issue 1 https://doi.org/10.5194/amt-13-309-2020	journal	January 2020
Evaluation of a regional air-quality model with bidirectional NH ₃ exchange coupled to an agroecosystem model Bash, J. O.; Cooter, E. J.; Dennis, R. L. Biogeosciences, Vol. 10, Issue 3 https://doi.org/10.5194/bg-10-1635-2013	journal	January 2013
Modelling the effect of soil moisture and organic matter degradation on biogenic NO emissions from soils in Sahel rangeland (Mali) Delon, C.; Mougin, E.; Serça, D. Biogeosciences, Vol. 12, Issue 11 https://doi.org/10.5194/bg-12-3253-2015	journal	January 2015
Modelling land–atmosphere daily exchanges of NO, NH₃, and CO₂ in a semi-arid grazed ecosystem in Senegal Delon, Claire; Galy-Lacaux, Corinne; Serça, Dominique Biogeosciences, Vol. 16, Issue 9 https://doi.org/10.5194/bg-16-2049-2019	journal	January 2019
Abundance and distribution of gaseous ammonia and particulate ammonium at Delhi, India Singh, S.; Kulshrestha, U. C. Biogeosciences, Vol. 9, Issue 12 https://doi.org/10.5194/bg-9-5023-2012	journal	January 2012
Gridded emissions of air pollutants for the period 1970–2012 within EDGAR v4.3.2 Crippa, Monica; Guizzardi, Diego; Muntean, Marilena Earth System Science Data, Vol. 10, Issue 4 https://doi.org/10.5194/essd-10-1987-2018	journal	January 2018
Historical (1750–2014) anthropogenic emissions of reactive gases and aerosols from the Community Emissions Data System (CEDS) Hoesly, Rachel M.; Smith, Steven J.; Feng, Leyang Geoscientific Model Development, Vol. 11, Issue 1 https://doi.org/10.5194/gmd-11-369-2018	journal	January 2018
Revised treatment of wet scavenging processes dramatically improves GEOS-Chem 12.0.0 simulations of surface nitric acid, nitrate, and ammonium over the United States Luo, Gan; Yu, Fangqun; Schwab, James Geoscientific Model Development, Vol. 12, Issue 8 https://doi.org/10.5194/gmd-12-3439-2019	journal	January 2019
An improved mechanistic model for ammonia volatilization in Earth system models: Flow of Agricultural Nitrogen version 2 (FANv2) Vira, Julius; Hess, Peter; Melkonian, Jeff Geoscientific Model Development, Vol. 13, Issue 9 https://doi.org/10.5194/gmd-13-4459-2020	journal	January 2020
Harmonization of global land use change and management for the period 850–2100 (LUH2) for CMIP6 Hurtt, George C.; Chini, Louise; Sahajpal, Ritvik Geoscientific Model Development, Vol. 13, Issue 11 https://doi.org/10.5194/gmd-13-5425-2020	journal	January 2020
Description and evaluation of the Model for Ozone and Related chemical Tracers, version 4 (MOZART-4) Emmons, L. K.; Walters, S.; Hess, P. G. Geoscientific Model Development, Vol. 3, Issue 1 https://doi.org/10.5194/gmd-3-43-2010	journal	January 2010
CAM-chem: description and evaluation of interactive atmospheric chemistry in the Community Earth System Model Lamarque, J. -F.; Emmons, L. K.; Hess, P. G. Geoscientific Model Development, Vol. 5, Issue 2 https://doi.org/10.5194/gmd-5-369-2012	journal	January 2012
Description and evaluation of tropospheric chemistry and aerosols in the Community Earth System Model (CESM1.2) Tilmes, S.; Lamarque, J. -F.; Emmons, L. K. Geoscientific Model Development, Vol. 8, Issue 5 https://doi.org/10.5194/gmd-8-1395-2015	journal	January 2015
The Land Use Model Intercomparison Project (LUMIP) contribution to CMIP6: rationale and experimental design Lawrence, David M.; Hurtt, George C.; Arneth, Almut Geoscientific Model Development, Vol. 9, Issue 9 https://doi.org/10.5194/gmd-9-2973-2016	journal	January 2016

Similar Records

Agricultural Impacts on Nitrogen Cycling: Climate and Air Pollution (Final Technical Report)

Technical Report · Sun Mar 07 23:00:00 EST 2021 · OSTI ID:1725771

An improved mechanistic model for ammonia volatilization in Earth system models: Flow of Agricultural Nitrogen version 2 (FANv2)

Journal Article · Wed Sep 23 20:00:00 EDT 2020 · Geoscientific Model Development (Online) · OSTI ID:1664612

Related Subjects

54 ENVIRONMENTAL SCIENCES
58 GEOSCIENCES

Evaluation of interactive and prescribed agricultural ammonia emissions for simulating atmospheric composition in CAM-chem

Citation Formats

References (64)

Similar Records

Related Subjects