Articles | Volume 21, issue 24
https://doi.org/10.5194/acp-21-18271-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-21-18271-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
16 Dec 2021
Research article |
| 16 Dec 2021
| 16 Dec 2021
Urban aerosol chemistry at a land–water transition site during summer – Part 2: Aerosol pH and liquid water content
Michael A. Battaglia Jr.
Department of Chemical, Biochemical and Environmental Engineering, University of Maryland, Baltimore County, Baltimore, MD, USA
current affiliation: School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA, USA
Nicholas Balasus
Department of Chemical, Biochemical and Environmental Engineering, University of Maryland, Baltimore County, Baltimore, MD, USA
Katherine Ball
Department of Chemical, Biochemical and Environmental Engineering, University of Maryland, Baltimore County, Baltimore, MD, USA
Vanessa Caicedo
Joint Center for Earth Systems Technology, University of Maryland, Baltimore County, Baltimore, MD, USA
Ruben Delgado
Joint Center for Earth Systems Technology, University of Maryland, Baltimore County, Baltimore, MD, USA
Annmarie G. Carlton
Department of Chemistry, University of California, Irvine, CA, USA
Christopher J. Hennigan
CORRESPONDING AUTHOR
Department of Chemical, Biochemical and Environmental Engineering, University of Maryland, Baltimore County, Baltimore, MD, USA
Related authors
Nicholas Balasus, Michael A. Battaglia Jr., Katherine Ball, Vanessa Caicedo, Ruben Delgado, Annmarie G. Carlton, and Christopher J. Hennigan
Atmos. Chem. Phys., 21, 13051–13065, https://doi.org/10.5194/acp-21-13051-2021, https://doi.org/10.5194/acp-21-13051-2021, 2021
Short summary
Short summary
Measurements of aerosol and gas composition were carried out at a land–water transition site near Baltimore, MD. Gas-phase ammonia concentrations were highly elevated compared to measurements at a nearby inland site. Our analysis reveals that NH2 was from both industrial and agricultural sources. This had a pronounced effect on aerosol chemical composition at the site, most notably contributing to episodic spikes of aerosol nitrate.
Vikram Pratap, Christopher J. Hennigan, Bastian Stieger, Andreas Tilgner, Laurent Poulain, Dominik van Pinxteren, Gerald Spindler, and Hartmut Herrmann
Atmos. Chem. Phys., 25, 8871–8889, https://doi.org/10.5194/acp-25-8871-2025, https://doi.org/10.5194/acp-25-8871-2025, 2025
Short summary
Short summary
In this work, we characterize trends in aerosol pH and its controlling factors during the period 2010–2019 at the Melpitz research station in eastern Germany. We find strong trends in aerosol pH and major inorganic species in response to changing emissions. We conduct a detailed thermodynamic analysis of the aerosol system and discuss implications for controlling particulate matter in the region.
Daniel L. Goldberg, M. Omar Nawaz, Congmeng Lyu, Jian He, Annmarie G. Carlton, Shobha Kondragunta, and Susan C. Anenberg
EGUsphere, https://doi.org/10.5194/egusphere-2025-1350, https://doi.org/10.5194/egusphere-2025-1350, 2025
Short summary
Short summary
This research investigates how air quality, specifically NO2 concentrations, is different under clear and cloudy skies. We find that in situ surface NO2 is, on average, +36 % larger during cloudy days versus clear sky days, with a wide distribution based on geographic region and roadway proximity: largest in the Northeast U.S. and smallest in the Southwest U.S. and near major roadways. This has implications for satellite data applications, which only use measurements in the absence of clouds.
Christopher J. Hennigan, Michael McKee, Vikram Pratap, Bryanna Boegner, Jasper Reno, Lucia Garcia, Madison McLaren, and Sara M. Lance
Atmos. Chem. Phys., 23, 14437–14449, https://doi.org/10.5194/acp-23-14437-2023, https://doi.org/10.5194/acp-23-14437-2023, 2023
Short summary
Short summary
This study characterized the optical properties of light-absorbing organic compounds, called brown carbon (BrC), in atmospheric cloud water samples. In all samples, light absorption by BrC increased linearly with increasing pH. There was variability in the sensitivity of the absorption–pH relationship, depending on the degree of influence from fire emissions. Overall, these results show that the climate forcing of BrC is quite strongly affected by its pH-dependent absorption.
Christine Wiedinmyer, Yosuke Kimura, Elena C. McDonald-Buller, Louisa K. Emmons, Rebecca R. Buchholz, Wenfu Tang, Keenan Seto, Maxwell B. Joseph, Kelley C. Barsanti, Annmarie G. Carlton, and Robert Yokelson
Geosci. Model Dev., 16, 3873–3891, https://doi.org/10.5194/gmd-16-3873-2023, https://doi.org/10.5194/gmd-16-3873-2023, 2023
Short summary
Short summary
The Fire INventory from NCAR (FINN) provides daily global estimates of emissions from open fires based on satellite detections of hot spots. This version has been updated to apply MODIS and VIIRS satellite fire detection and better represents both large and small fires. FINNv2.5 generates more emissions than FINNv1 and is in general agreement with other fire emissions inventories. The new estimates are consistent with satellite observations, but uncertainties remain regionally and by pollutant.
Claudia Bernier, Yuxuan Wang, Guillaume Gronoff, Timothy Berkoff, K. Emma Knowland, John T. Sullivan, Ruben Delgado, Vanessa Caicedo, and Brian Carroll
Atmos. Chem. Phys., 22, 15313–15331, https://doi.org/10.5194/acp-22-15313-2022, https://doi.org/10.5194/acp-22-15313-2022, 2022
Short summary
Short summary
Coastal regions are susceptible to variable and high ozone which is difficult to simulate. We developed a method to characterize large datasets of multi-dimensional measurements from lidar instruments taken in coastal regions. Using the clustered ozone groups, we evaluated model performance in simulating the coastal ozone variability vertically and diurnally. The approach allowed us to pinpoint areas where the models succeed in simulating coastal ozone and areas where there are still gaps.
Nicholas Balasus, Michael A. Battaglia Jr., Katherine Ball, Vanessa Caicedo, Ruben Delgado, Annmarie G. Carlton, and Christopher J. Hennigan
Atmos. Chem. Phys., 21, 13051–13065, https://doi.org/10.5194/acp-21-13051-2021, https://doi.org/10.5194/acp-21-13051-2021, 2021
Short summary
Short summary
Measurements of aerosol and gas composition were carried out at a land–water transition site near Baltimore, MD. Gas-phase ammonia concentrations were highly elevated compared to measurements at a nearby inland site. Our analysis reveals that NH2 was from both industrial and agricultural sources. This had a pronounced effect on aerosol chemical composition at the site, most notably contributing to episodic spikes of aerosol nitrate.
Jianfeng Li, Yuhang Wang, Ruixiong Zhang, Charles Smeltzer, Andrew Weinheimer, Jay Herman, K. Folkert Boersma, Edward A. Celarier, Russell W. Long, James J. Szykman, Ruben Delgado, Anne M. Thompson, Travis N. Knepp, Lok N. Lamsal, Scott J. Janz, Matthew G. Kowalewski, Xiong Liu, and Caroline R. Nowlan
Atmos. Chem. Phys., 21, 11133–11160, https://doi.org/10.5194/acp-21-11133-2021, https://doi.org/10.5194/acp-21-11133-2021, 2021
Short summary
Short summary
Comprehensive evaluations of simulated diurnal cycles of NO2 and NOy concentrations, vertical profiles, and tropospheric vertical column densities at two different resolutions with various measurements during the DISCOVER-AQ 2011 campaign show potential distribution biases of NOx emissions in the National Emissions Inventory 2011 at both 36 and 4 km resolutions, providing another possible explanation for the overestimation of model results.
Amy E. Christiansen, Annmarie G. Carlton, and Barron H. Henderson
Atmos. Chem. Phys., 20, 11607–11624, https://doi.org/10.5194/acp-20-11607-2020, https://doi.org/10.5194/acp-20-11607-2020, 2020
Short summary
Short summary
We quantify differences in surface-level fine particle mass (PM2.5) chemical composition in relation to satellite-derived cloud flags and find significant differences between clear-sky and cloud days. The work suggests that future analysis in this area is warranted.
Cited articles
Angle, K. J., Crocker, D. R., Simpson, R. M. C., Mayer, K. J., Garofalo, L. A., Moore, A. N., Garcia, S. L. M., Or, V. W., Srinivasan, S., Farhan, M., Sauer, J. S., Lee, C., Pothier, M. A., Farmer, D. K., Martz, T. R., Bertram, T. H., Cappa, C. D., Prather, K. A., and Grassian, V. H.: Acidity across the interface from the ocean surface to sea spray aerosol, P. Natl. Acad. Sci. USA, 118, e2018397118, https://doi.org/10.1073/pnas.2018397118, 2021.
Balasus, N., Battaglia Jr., M. A., Ball, K., Caicedo, V., Delgado, R., Carlton, A. G., and Hennigan, C. J.: Urban aerosol chemistry at a land–water transition site during summer – Part 1: Impact of agricultural and industrial ammonia emissions, Atmos. Chem. Phys., 21, 13051–13065, https://doi.org/10.5194/acp-21-13051-2021, 2021.
Battaglia Jr., M. A., Douglas, S., and Hennigan, C. J.: Effect of the Urban Heat Island on Aerosol pH, Environ. Sci. Technol., 51, 13095–13103, https://doi.org/10.1021/acs.est.7b02786, 2017.
Battaglia Jr., M. A., Weber, R. J., Nenes, A., and Hennigan, C. J.: Effects of water-soluble organic carbon on aerosol pH, Atmos. Chem. Phys., 19, 14607–14620, https://doi.org/10.5194/acp-19-14607-2019, 2019.
Bougiatioti, A., Nikolaou, P., Stavroulas, I., Kouvarakis, G., Weber, R., Nenes, A., Kanakidou, M., and Mihalopoulos, N.: Particle water and pH in the eastern Mediterranean: source variability and implications for nutrient availability, Atmos. Chem. Phys., 16, 4579–4591, https://doi.org/10.5194/acp-16-4579-2016, 2016.
Boyer, H. C., Gorkowski, K., and Sullivan, R. C.:
In Situ pH Measurements of Individual Levitated Microdroplets Using Aerosol Optical Tweezers,
Anal. Chem.,
92, 1089–1096, https://doi.org/10.1021/acs.analchem.9b04152, 2020.
Brimblecombe, P., and Clegg, S. L.:
The Solubility and Behavior of Acid Gases in the Marine Aerosol,
J. Atmos. Chem.,
7, 1–18, https://doi.org/10.1007/bf00048251, 1988.
Carlton, A. M. G., Pye, H. O. T., Baker, K. R., and Hennigan, C. J.: Additional benefits of federal air quality rules: model estimates of controllable biogenic secondary organic aerosol, Environ. Sci. Technol., 52, 9254–9265, https://doi.org/10.1021/acs.est.8b01869, 2018.
Craig, R. L., Peterson, P. K., Nandy, L., Lei, Z., Hossain, M. A., Camarena, S., Dodson, R. A., Cook, R. D., Dutcher, C. S., and Ault, A. P.:
Direct Determination of Aerosol pH: Size-Resolved Measurements of Submicrometer and Supermicrometer Aqueous Particles,
Anal. Chem.,
90, 11232–11239, https://doi.org/10.1021/acs.analchem.8b00586, 2018.
El-Sayed, M. M. H., Amenumey, D., and Hennigan, C. J.:
Drying-Induced Evaporation of Secondary Organic Aerosol during Summer,
Environ. Sci. Technol.,
50, 3626–3633, https://doi.org/10.1021/acs.est.5b06002, 2016.
Fang, T., Guo, H. Y., Zeng, L. H., Verma, V., Nenes, A., and Weber, R. J.:
Highly Acidic Ambient Particles, Soluble Metals, and Oxidative Potential: A Link between Sulfate and Aerosol Toxicity,
Environ. Sci. Technol.,
51, 2611–2620, https://doi.org/10.1021/acs.est.6b06151, 2017.
Feng, L., Shen, H., Zhu, Y., Gao, H., and Yao, X.:
Insight into Generation and Evolution of Sea-Salt Aerosols from Field Measurements in Diversified Marine and Coastal Atmospheres,
Sci. Rep.,
7, 41260, https://doi.org/10.1038/srep41260, 2017.
Fountoukis, C. and Nenes, A.: ISORROPIA II: a computationally efficient thermodynamic equilibrium model for K+-Ca2+-Mg2+-
Guo, H., Xu, L., Bougiatioti, A., Cerully, K. M., Capps, S. L., Hite Jr., J. R., Carlton, A. G., Lee, S.-H., Bergin, M. H., Ng, N. L., Nenes, A., and Weber, R. J.: Fine-particle water and pH in the southeastern United States, Atmos. Chem. Phys., 15, 5211–5228, https://doi.org/10.5194/acp-15-5211-2015, 2015.
Guo, H., Liu, J., Froyd, K. D., Roberts, J. M., Veres, P. R., Hayes, P. L., Jimenez, J. L., Nenes, A., and Weber, R. J.: Fine particle pH and gas–particle phase partitioning of inorganic species in Pasadena, California, during the 2010 CalNex campaign, Atmos. Chem. Phys., 17, 5703–5719, https://doi.org/10.5194/acp-17-5703-2017, 2017.
Guo, H., Nenes, A., and Weber, R. J.: The underappreciated role of nonvolatile cations in aerosol ammonium-sulfate molar ratios, Atmos. Chem. Phys., 18, 17307–17323, https://doi.org/10.5194/acp-18-17307-2018, 2018.
He, H., Stehr, J. W., Hains, J. C., Krask, D. J., Doddridge, B. G., Vinnikov, K. Y., Canty, T. P., Hosley, K. M., Salawitch, R. J., Worden, H. M., and Dickerson, R. R.: Trends in emissions and concentrations of air pollutants in the lower troposphere in the Baltimore/Washington airshed from 1997 to 2011, Atmos. Chem. Phys., 13, 7859–7874, https://doi.org/10.5194/acp-13-7859-2013, 2013.
Hennigan, C. J., Izumi, J., Sullivan, A. P., Weber, R. J., and Nenes, A.: A critical evaluation of proxy methods used to estimate the acidity of atmospheric particles, Atmos. Chem. Phys., 15, 2775–2790, https://doi.org/10.5194/acp-15-2775-2015, 2015.
Jang, M., Sun, S., Winslow, R., Han, S., and Yu, Z.:
In situ aerosol acidity measurements using a UV–Visible micro-spectrometer and its application to the ambient air,
Aerosol Sci. Tech.,
54, 446–461, https://doi.org/10.1080/02786826.2020.1711510, 2020.
Kakavas, S., Patoulias, D., Zakoura, M., Nenes, A., and Pandis, S. N.: Size-resolved aerosol pH over Europe during summer, Atmos. Chem. Phys., 21, 799–811, https://doi.org/10.5194/acp-21-799-2021, 2021.
Kanakidou, M., Myriokefalitakis, S., Daskalakis, N., Fanourgakis, G., Nenes, A., Baker, A. R., Tsigaridis, K., and Mihalopoulos, N.:
Past, Present, and Future Atmospheric Nitrogen Deposition,
J. Atmos. Sci.,
73, 2039–2047, https://doi.org/10.1175/jas-d-15-0278.1, 2016.
Keene, W. C., Pszenny, A. A. P., Maben, J. R., and Sander, R.:
Variation of marine aerosol acidity with particle size,
Geophys. Res. Lett.,
29, 1101, https://doi.org/10.1029/2001gl013881, 2002.
Keene, W. C., Pszenny, A. A. P., Maben, J. R., Stevenson, E., and Wall, A.:
Closure evaluation of size-resolved aerosol pH in the New England coastal atmosphere during summer,
J. Geophys. Res.-Atmos.,
109, D23307, https://doi.org/10.1029/2004jd004801, 2004.
Loughner, C. P., Tzortziou, M., Follette-Cook, M., Pickering, K. E., Goldberg, D., Satam, C., Weinheimer, A., Crawford, J. H., Knapp, D. J., Montzka, D. D., Diskin, G. S., and Dickerson, R. R.:
Impact of Bay-Breeze Circulations on Surface Air Quality and Boundary Layer Export,
J. Appl. Meteorol. Clim.,
53, 1697–1713, https://doi.org/10.1175/jamc-d-13-0323.1, 2014.
Loughner, C. P., Tzortziou, M., Shroder, S., and Pickering, K. E.:
Enhanced dry deposition of nitrogen pollution near coastlines: A case study covering the Chesapeake Bay estuary and Atlantic Ocean coastline,
J. Geophys. Res.-Atmos.,
121, 14221–14238, https://doi.org/10.1002/2016jd025571, 2016.
Murphy, J. G., Gregoire, P., Tevlin, A., Wentworth, G., Ellis, R., Markovic, M., and VandenBoer, T.: Observational constraints on particle acidity using measurements and modelling of particles and gases, Faraday Discuss., 200, 379–395, https://doi.org/10.1039/C7FD00086C, 2017.
NASA: Airborne Science Data for Atmospheric Composition, available at: https://www-air.larc.nasa.gov/cgi-bin/ArcView/owlets.2018, last access: 14 December 2021.
Nenes, A., Pandis, S. N., Weber, R. J., and Russell, A.: Aerosol pH and liquid water content determine when particulate matter is sensitive to ammonia and nitrate availability, Atmos. Chem. Phys., 20, 3249–3258, https://doi.org/10.5194/acp-20-3249-2020, 2020.
Nenes, A., Pandis, S. N., Kanakidou, M., Russell, A. G., Song, S., Vasilakos, P., and Weber, R. J.: Aerosol acidity and liquid water content regulate the dry deposition of inorganic reactive nitrogen, Atmos. Chem. Phys., 21, 6023–6033, https://doi.org/10.5194/acp-21-6023-2021, 2021.
Norman, M., Spirig, C., Wolff, V., Trebs, I., Flechard, C., Wisthaler, A., Schnitzhofer, R., Hansel, A., and Neftel, A.: Intercomparison of ammonia measurement techniques at an intensively managed grassland site (Oensingen, Switzerland), Atmos. Chem. Phys., 9, 2635–2645, https://doi.org/10.5194/acp-9-2635-2009, 2009.
O'Dowd, C. D., and De Leeuw, G.:
Marine aerosol production: a review of the current knowledge,
Philos. T. R. Soc. A,
365, 1753–1774, https://doi.org/10.1098/rsta.2007.2043, 2007.
Phillips, S. M., Bellcross, A. D., and Smith, G. D.: Light Absorption by Brown Carbon in the Southeastern United States is pH-dependent, Environ. Sci. Technol., 51, 6782–6790, https://doi.org/10.1021/acs.est.7b01116, 2017.
Pinder, R. W., Adams, P. J., Pandis, S. N., and Gilliland, A. B.:
Temporally resolved ammonia emission inventories: Current estimates, evaluation tools, and measurement needs,
J. Geophys. Res.-Atmos.,
111, D16310, https://doi.org/10.1029/2005jd006603, 2006.
Pritchard, D. W.:
Salinity Distribution and Circulation in the Chesapeake Bay Estuarine System,
J. Mar. Res.,
11, 106–123, 1952.
Pszenny, A. A. P., Moldanová, J., Keene, W. C., Sander, R., Maben, J. R., Martinez, M., Crutzen, P. J., Perner, D., and Prinn, R. G.: Halogen cycling and aerosol pH in the Hawaiian marine boundary layer, Atmos. Chem. Phys., 4, 147–168, https://doi.org/10.5194/acp-4-147-2004, 2004.
Pye, H. O. T., Zuend, A., Fry, J. L., Isaacman-VanWertz, G., Capps, S. L., Appel, K. W., Foroutan, H., Xu, L., Ng, N. L., and Goldstein, A. H.: Coupling of organic and inorganic aerosol systems and the effect on gas–particle partitioning in the southeastern US, Atmos. Chem. Phys., 18, 357–370, https://doi.org/10.5194/acp-18-357-2018, 2018.
Pye, H. O. T., Nenes, A., Alexander, B., Ault, A. P., Barth, M. C., Clegg, S. L., Collett Jr., J. L., Fahey, K. M., Hennigan, C. J., Herrmann, H., Kanakidou, M., Kelly, J. T., Ku, I.-T., McNeill, V. F., Riemer, N., Schaefer, T., Shi, G., Tilgner, A., Walker, J. T., Wang, T., Weber, R., Xing, J., Zaveri, R. A., and Zuend, A.: The acidity of atmospheric particles and clouds, Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, 2020.
Rindelaub, J. D., Craig, R. L., Nandy, L., Bondy, A. L., Dutcher, C. S., Shepson, P. B., and Ault, A. P.:
Direct Measurement of pH in Individual Particles via Raman Microspectroscopy and Variation in Acidity with Relative Humidity,
J. Phys. Chem. A,
120, 911–917, https://doi.org/10.1021/acs.jpca.5b12699, 2016.
Seinfeld, J. H., and Pandis, S. N.: Atmospheric chemistry and physics: from air pollution to climate change, 3rd Edn., John Wiley and Sons, Hoboken, NJ, 2016.
Tao, Y.: Identification of Major Factors Influencing Aerosol pH and the Quantitative Relationship between pH and Ammonia Gas/Particle Partitioning, PhD Thesis, University of Toronto, Toronto, available at: https://hdl.handle.net/1807/103788 (last access: 30 April 2021), 2020.
Tao, Y. and Murphy, J. G.: The sensitivity of PM2.5 acidity to meteorological parameters and chemical composition changes: 10-year records from six Canadian monitoring sites, Atmos. Chem. Phys., 19, 9309–9320, https://doi.org/10.5194/acp-19-9309-2019, 2019.
Valerino, M. J., Johnson, J. J., Izumi, J., Orozco, D., Hoff, R. M., Delgado, R., and Hennigan, C. J.:
Sources and composition of PM2.5 in the Colorado Front Range during the DISCOVER-AQ study,
J. Geophys. Res.-Atmos.,
122, 566–582, https://doi.org/10.1002/2016jd025830, 2017.
Vasilakos, P., Russell, A., Weber, R., and Nenes, A.: Understanding nitrate formation in a world with less sulfate, Atmos. Chem. Phys., 18, 12765–12775, https://doi.org/10.5194/acp-18-12765-2018, 2018.
Weber, R. J., Guo, H., Russell, A. G., and Nenes, A.:
High aerosol acidity despite declining atmospheric sulfate concentrations over the past 15 years,
Nat. Geosci.,
9, 282–285, https://doi.org/10.1038/ngeo2665, 2016.
Zheng, G., Su, H., Wang, S., Andreae, M. O., Pöschl, U., and Cheng, Y.:
Multiphase buffer theory explains contrasts in atmospheric aerosol acidity,
Science,
369, 1374, https://doi.org/10.1126/science.aba3719, 2020.
Short summary
This study characterizes aerosol liquid water content and aerosol pH at a land–water transition site near Baltimore, Maryland. We characterize the effects of unique meteorology associated with the close proximity to the Chesapeake Bay and episodic NH3 events derived from industrial and agricultural sources on aerosol chemistry during the summer. We also examine two events where primary Bay emissions underwent aging in the polluted urban atmosphere.
This study characterizes aerosol liquid water content and aerosol pH at a land–water transition...
Altmetrics
Final-revised paper
Preprint