On Aerosol Liquid Water and Sulfate Associations: The Potential for Fine Particulate Matter Biases
Abstract
In humid locations of the Eastern U.S., sulfate is a surrogate for aerosol liquid water (ALW), a poorly measured particle constituent. Regional and seasonal variation in ALW–sulfate relationships offers a potential explanation to reconcile epidemiology and toxicology studies regarding particulate sulfur and health endpoints. ALW facilitates transfer of polar species from the gas phase to the particle phase and affects particle pH and metal oxidation state. Though abundant and a potential indicator of adverse health endpoints, ALW is largely removed in most particulate matter measurement techniques, including in routine particulate matter (PM2.5) networks that use federal reference method (FRM) monitors, which are used in epidemiology studies. We find that in 2004, a typical year in the available record, ambient ALW mass is removed during sampling and filter equilibration to standard laboratory conditions at most (94%) sites, up to 85% of the ambient water mass. The removal of ALW can induce the evaporation of other semi-volatile compounds present in PM2.5, such as ammonium nitrate and numerous organics. This produces an artifact in the PM mass measurements that is, importantly, not uniform in space or time. This suggests that PM2.5 epidemiology studies that exclude ALW are biased. This work provides a plausiblemore »
- Authors:
-
[1];
[3]
- Univ. of California, Irvine, CA (United States)
- Univ. of Maryland Baltimore County (UMBC), Baltimore, MD (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE; National Aeronautics and Space Administration (NASA); National Science Foundation (NSF)
- OSTI Identifier:
- 1632702
- Grant/Contract Number:
- AC02-06CH11357; 80NSSC19K0987; 1719252; 1719245
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Atmosphere (Basel)
- Additional Journal Information:
- Journal Name: Atmosphere (Basel); Journal Volume: 11; Journal Issue: 2; Journal ID: ISSN 2073-4433
- Publisher:
- MDPI
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 54 ENVIRONMENTAL SCIENCES; PM2.5; aerosol liquid water; air quality
Citation Formats
Babila, Jonathon E., Carlton, Annmarie G., Hennigan, Christopher J., and Ghate, Virendra P. On Aerosol Liquid Water and Sulfate Associations: The Potential for Fine Particulate Matter Biases. United States: N. p., 2020.
Web. doi:10.3390/atmos11020194.
Babila, Jonathon E., Carlton, Annmarie G., Hennigan, Christopher J., & Ghate, Virendra P. On Aerosol Liquid Water and Sulfate Associations: The Potential for Fine Particulate Matter Biases. United States. https://doi.org/10.3390/atmos11020194
Babila, Jonathon E., Carlton, Annmarie G., Hennigan, Christopher J., and Ghate, Virendra P. Wed .
"On Aerosol Liquid Water and Sulfate Associations: The Potential for Fine Particulate Matter Biases". United States. https://doi.org/10.3390/atmos11020194. https://www.osti.gov/servlets/purl/1632702.
@article{osti_1632702,
title = {On Aerosol Liquid Water and Sulfate Associations: The Potential for Fine Particulate Matter Biases},
author = {Babila, Jonathon E. and Carlton, Annmarie G. and Hennigan, Christopher J. and Ghate, Virendra P.},
abstractNote = {In humid locations of the Eastern U.S., sulfate is a surrogate for aerosol liquid water (ALW), a poorly measured particle constituent. Regional and seasonal variation in ALW–sulfate relationships offers a potential explanation to reconcile epidemiology and toxicology studies regarding particulate sulfur and health endpoints. ALW facilitates transfer of polar species from the gas phase to the particle phase and affects particle pH and metal oxidation state. Though abundant and a potential indicator of adverse health endpoints, ALW is largely removed in most particulate matter measurement techniques, including in routine particulate matter (PM2.5) networks that use federal reference method (FRM) monitors, which are used in epidemiology studies. We find that in 2004, a typical year in the available record, ambient ALW mass is removed during sampling and filter equilibration to standard laboratory conditions at most (94%) sites, up to 85% of the ambient water mass. The removal of ALW can induce the evaporation of other semi-volatile compounds present in PM2.5, such as ammonium nitrate and numerous organics. This produces an artifact in the PM mass measurements that is, importantly, not uniform in space or time. This suggests that PM2.5 epidemiology studies that exclude ALW are biased. This work provides a plausible explanation to resolve multi-decade discrepancies regarding ambient sulfate and health impacts in some epidemiological and toxicological studies},
doi = {10.3390/atmos11020194},
journal = {Atmosphere (Basel)},
number = 2,
volume = 11,
place = {United States},
year = {Wed Feb 12 00:00:00 EST 2020},
month = {Wed Feb 12 00:00:00 EST 2020}
}
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Figures / Tables:
Figure 1: Yearly average in 2004 at Interagency Monitoring of PROtected Visual Environments (IMPROVE) monitoring sites of (a) ratio of aerosol liquid water (ALW) mass per measured PM2.5 ‘dry’ mass (b) ambient ALW mass concentrations and (c) equivalent concentration loss upon filter equilibration to standard laboratory conditions. Point color andmore »
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