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Title: 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 (PM 2.5) 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 PM 2.5, 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 PM 2.5 epidemiology studies that exclude ALW are biased. This workmore » provides a plausible explanation to resolve multi-decade discrepancies regarding ambient sulfate and health impacts in some epidemiological and toxicological studies« less

Authors:
 [1]; ORCiD logo [1];  [2]; ORCiD logo [3]
  1. Univ. of California, Irvine, CA (United States)
  2. Univ. of Maryland Baltimore County (UMBC), Baltimore, MD (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE; National Aeronautic and Space Administration (NASA); National Science Foundation (NSF)
OSTI Identifier:
1632702
Grant/Contract Number:  
AC02-06CH11357; 80NSSC19K0987; 1719252; 1719245
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Atmosphere (Basel)
Additional Journal Information:
Journal Volume: 11; Journal Issue: 2; Journal ID: ISSN 2073-4433
Publisher:
MDPI
Country of Publication:
United States
Language:
English
Subject:
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. doi: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. doi: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)},
issn = {2073-4433},
number = 2,
volume = 11,
place = {United States},
year = {2020},
month = {2}
}

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