Articles | Volume 17, issue 8
https://doi.org/10.5194/acp-17-5107-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-17-5107-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
19 Apr 2017
Research article |
| 19 Apr 2017
Inconsistency of ammonium–sulfate aerosol ratios with thermodynamic models in the eastern US: a possible role of organic aerosol
Department of Earth and Planetary Sciences, Harvard University,
Cambridge, MA, USA
Daniel J. Jacob
Department of Earth and Planetary Sciences, Harvard University,
Cambridge, MA, USA
John A. Paulson School of Engineering and Applied Sciences, Harvard
University, Cambridge, MA, USA
Patrick S. Kim
Department of Earth and Planetary Sciences, Harvard University,
Cambridge, MA, USA
Eloise A. Marais
John A. Paulson School of Engineering and Applied Sciences, Harvard
University, Cambridge, MA, USA
now at: School of Geography, Earth and Environmental Sciences,
University of Birmingham, Edgbaston, UK
Jay R. Turner
Department of Energy, Environmental and Chemical Engineering,
Washington University, St. Louis, MO, USA
Pedro Campuzano-Jost
Cooperative Institute for Research in Environmental Sciences,
University of Colorado Boulder, Boulder, CO, USA
Department of Chemistry and Biochemistry, University of Colorado
Boulder, Boulder, CO, USA
Jose L. Jimenez
Cooperative Institute for Research in Environmental Sciences,
University of Colorado Boulder, Boulder, CO, USA
Department of Chemistry and Biochemistry, University of Colorado
Boulder, Boulder, CO, USA
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33 citations as recorded by crossref.
- Coupling of organic and inorganic aerosol systems and the effect on gas–particle partitioning in the southeastern US H. Pye et al. 10.5194/acp-18-357-2018
- Theoretical Phase Resolved Ammonia–Ammonium Nitrogen Equilibrium Isotope Exchange Fractionations: Applications for Tracking Atmospheric Ammonia Gas-to-Particle Conversion W. Walters et al. 10.1021/acsearthspacechem.8b00140
- Effects of Phase State and Phase Separation on Dimethylamine Uptake of Ammonium Sulfate and Ammonium Sulfate–Sucrose Mixed Particles W. DeRieux et al. 10.1021/acsearthspacechem.9b00142
- Investigation of global particulate nitrate from the AeroCom phase III experiment H. Bian et al. 10.5194/acp-17-12911-2017
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- Yearly changes of the sulfate-nitrate-ammonium aerosols and the relationship with their precursors from 1999 to 2016 in Beijing Y. Xie 10.1007/s11356-019-07493-w
- Importance of gas-particle partitioning of ammonia in haze formation in the rural agricultural environment J. Xu et al. 10.5194/acp-20-7259-2020
- Seasonal variations in size distribution, water-soluble ions, and carbon content of size-segregated aerosols over New Delhi P. Kumar et al. 10.1007/s11356-017-0954-6
- Current State of Atmospheric Aerosol Thermodynamics and Mass Transfer Modeling: A Review K. Semeniuk & A. Dastoor 10.3390/atmos11020156
- Seasonal study of stable carbon and nitrogen isotopic composition in fine aerosols at a Central European rural background station P. Vodička et al. 10.5194/acp-19-3463-2019
- Aerosol Acidity: Novel Measurements and Implications for Atmospheric Chemistry A. Ault 10.1021/acs.accounts.0c00303
- Effects of NH3 and alkaline metals on the formation of particulate sulfate and nitrate in wintertime Beijing R. Huang et al. 10.1016/j.scitotenv.2020.137190
- Climate impact on ambient PM2.5 elemental concentration in the United States: A trend analysis over the last 30 years W. Requia et al. 10.1016/j.envint.2019.05.082
- Effects of COVID-19 lockdown on PM10 composition and sources in the Rome Area (Italy) by elements' chemical fractionation-based source apportionment L. Massimi et al. 10.1016/j.atmosres.2021.105970
- Aerosol pH Dynamics During Haze Periods in an Urban Environment in China: Use of Detailed, Hourly, Speciated Observations to Study the Role of Ammonia Availability and Secondary Aerosol Formation and Urban Environment G. Shi et al. 10.1029/2018JD029976
- Trends in remote PM2.5 residual mass across the United States: Implications for aerosol mass reconstruction in the IMPROVE network J. Hand et al. 10.1016/j.atmosenv.2019.01.049
- Chemical nature of PM2.5 and PM10 in the coastal urban Xiamen, China: Insights into the impacts of shipping emissions and health risk S. Wu et al. 10.1016/j.atmosenv.2020.117383
- Sources, species and secondary formation of atmospheric aerosols and gaseous precursors in the suburb of Kitakyushu, Japan X. Zhang et al. 10.1016/j.scitotenv.2020.143001
- Southeast Atmosphere Studies: learning from model-observation syntheses J. Mao et al. 10.5194/acp-18-2615-2018
- Hygroscopicity and Compositional Evolution of Atmospheric Aerosols Containing Water-Soluble Carboxylic Acid Salts and Ammonium Sulfate: Influence of Ammonium Depletion N. Wang et al. 10.1021/acs.est.8b07052
- Linked Response of Aerosol Acidity and Ammonia to SO2 and NOx Emissions Reductions in the United States A. Lawal et al. 10.1021/acs.est.8b00711
- The underappreciated role of nonvolatile cations in aerosol ammonium-sulfate molar ratios H. Guo et al. 10.5194/acp-18-17307-2018
- Trends in Chemical Composition of Global and Regional Population-Weighted Fine Particulate Matter Estimated for 25 Years C. Li et al. 10.1021/acs.est.7b02530
- Reactive Uptake of Isoprene Epoxydiols Increases the Viscosity of the Core of Phase-Separated Aerosol Particles N. Olson et al. 10.1021/acsearthspacechem.9b00138
- Concurrent Temporal and Spatial Trends in Sulfate and Organic Mass Concentrations Measured in the IMPROVE Monitoring Program W. Malm et al. 10.1002/2017JD026865
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- Characterization and variability of inorganic aerosols and their gaseous precursors at a suburban site in northern France over one year (2015–2016) R. Roig Rodelas et al. 10.1016/j.atmosenv.2018.11.041
- Direct Determination of Aerosol pH: Size-Resolved Measurements of Submicrometer and Supermicrometer Aqueous Particles R. Craig et al. 10.1021/acs.analchem.8b00586
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- The acidity of atmospheric particles and clouds H. Pye et al. 10.5194/acp-20-4809-2020
- Effects of High Acidity on Phase Transitions of an Organic Aerosol D. Losey et al. 10.1021/acs.jpca.8b00399
- Understanding nitrate formation in a world with less sulfate P. Vasilakos et al. 10.5194/acp-18-12765-2018
3 citations as recorded by crossref.
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- Atmospheric Aerosols: Clouds, Chemistry, and Climate V. McNeill 10.1146/annurev-chembioeng-060816-101538
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Saved (preprint)
Latest update: 09 Jun 2023
Short summary
We identify a fundamental discrepancy between thermodynamic equilibrium theory and observations of inorganic aerosol composition in the eastern US in summer that shows low ammonium sulfate aerosol ratios. In addition, from 2003 to 2013, while SO2 emissions have declined due to US emission controls, aerosols have become more acidic in the southeastern US. To explain these observations, we suggest that the large and increasing source of organic aerosol may be affecting thermodynamic equilibrium.
We identify a fundamental discrepancy between thermodynamic equilibrium theory and observations...
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