Preprints
https://doi.org/10.5194/acp-2021-495
https://doi.org/10.5194/acp-2021-495

  14 Jun 2021

14 Jun 2021

Review status: a revised version of this preprint is currently under review for the journal ACP.

Changes in PM2.5 concentrations and their sources in the US from 1990 to 2010

Ksakousti Skyllakou1, Pablo Garcia Rivera2, Brian Dinkelacker2, Eleni Karnezi2,3, Ioannis Kioutsioukis4, Carlos Hernandez5, Peter J. Adams5, and Spyros N. Pandis1,6 Ksakousti Skyllakou et al.
  • 1Institute of Chemical Engineering Sciences (FORTH/ICE-HT), 26504, Patras, Greece
  • 2Department of Chemical Engineering, Carnegie Mellon University, Pittsburgh, PA 15213, USA
  • 3Barcelona Supercomputing Center, 08034, Barcelona, Spain
  • 4Department of Physics, University of Patras, 26500, Patras, Greece
  • 5Department of Civil and Environmental Engineering, Carnegie Mellon University, Pittsburgh, PA 15213, USA
  • 6Department of Chemical Engineering, University of Patras, 26500, Patras, Greece

Abstract. Significant reductions of emissions of SO2, NOx, volatile organic compounds (VOCs) and primary particulate matter (PM) took place in the US from 1990 to 2010. We evaluate here our understanding of the links between these emissions changes and corresponding changes in concentrations and health outcomes using a chemical transport model, the Particulate Matter Comprehensive Air Quality Model with Extensions (PMCAMx) with the Particle Source Apportionment Algorithm (PSAT). Results for 1990, 2001 and 2010 are presented. The reductions in SO2 emissions (64 %, mainly from electric generating units) during these 20 years have dominated the reductions in PM2.5 leading to a 45 % reduction in sulfate levels. The predicted sulfate reductions are in excellent agreement with the available measurements. Also, the reductions in elemental carbon (EC) emissions (mainly from transportation) have led to a 30 % reduction of EC concentrations. The most important source of organic aerosol (OA) through the years according to PMCAMx is biomass burning, followed by biogenic secondary organic aerosol (SOA). OA from on-road transport has been reduced by more than a factor of three. On the other hand, changes in biomass burning OA and biogenic SOA have been modest. In 1990, about half of the US population was exposed to annual-average PM2.5 concentrations above 20 μg m−3, but by 2010 this fraction had dropped to practically zero. The predicted changes in concentrations are evaluated against the observed changes for 1990, 2001, and 2010, in order to understand if the model represents reasonably well the corresponding processes caused by the changes in emissions.

Ksakousti Skyllakou et al.

Status: final response (author comments only)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on acp-2021-495', Anonymous Referee #1, 02 Jul 2021
    • AC1: 'Response to Referee #1', Spyros Pandis, 02 Sep 2021
  • RC2: 'Comment on acp-2021-495', Anonymous Referee #2, 07 Jul 2021
    • AC2: 'Response to Referee #2', Spyros Pandis, 02 Sep 2021

Ksakousti Skyllakou et al.

Ksakousti Skyllakou et al.

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Short summary
Significant reductions of pollutant emissions took place in the US from 1990 to 2010. The reductions in sulfur dioxide emissions from electric generating units have dominated the reductions in fine particle mass. The reductions in transportation emissions from have led to a 30 % reduction of elemental concentrations and of organic particulate matter by a factor of three. On the other hand, changes in biomass burning and biogenic secondary organic aerosol have been modest.
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