Photochemical model assessment of single source NO2 and O3 plumes using field study data

Kirk R Baker; Lukas Valin; Jim Szykman; Laura Judd; Qian Shu; Bill Hutzell; Sergey Napelenok; Ben Murphy; Vickie Connors

doi:10.1016/j.scitotenv.2023.166606

Photochemical model assessment of single source NO₂ and O₃ plumes using field study data

Sci Total Environ. 2023 Dec 10:903:166606. doi: 10.1016/j.scitotenv.2023.166606. Epub 2023 Aug 26.

Authors

Kirk R Baker¹, Lukas Valin², Jim Szykman², Laura Judd³, Qian Shu², Bill Hutzell², Sergey Napelenok², Ben Murphy², Vickie Connors⁴

Affiliations

¹ U.S. Environmental Protection Agency, Research Triangle Park, NC, USA. Electronic address: baker.kirk@epa.gov.
² U.S. Environmental Protection Agency, Research Triangle Park, NC, USA.
³ NASA Langley Research Center, Hampton, VA, USA.
⁴ Virginia Commonwealth University, Richmond, VA, USA.

PMID: 37640074
PMCID: PMC10713090 (available on 2024-12-10)
DOI: 10.1016/j.scitotenv.2023.166606

Abstract

Single source contribution to ambient O₃ and PM_2.5 has been estimated with photochemical grid models to support policy demonstrations for National Ambient Air Quality Standards, regional haze, and permit related programs. Limited field data exists to evaluate model representation of the spatial extent and chemical composition of plumes emitted by specific facilities. New tropospheric column measurements of NO₂ and in-plume chemical measurements downwind of specific facilities allows for photochemical model evaluation of downwind plume extent, grid resolution impacts on plume concentration gradients, and source attribution methods. Here, photochemical models were applied with source sensitivity and source apportionment approaches to differentiate single source impacts on NO₂ and O₃ and compare with field study measurements. Source sensitivity approaches (e.g., brute-force difference method and decoupled direct method (DDM)) captured the spatial extent of NO₂ plumes downwind of three facilities and the transition of near-source O₃ titration to downwind production. Source apportionment approaches showed variability in terms of attributing the spatial extent of NO₂ plumes and downwind O₃ production. Each of the Community Multiscale Air Quality (CMAQ) source apportionment options predicted large O₃ contribution from a large industrial facility in the flight transects nearest the facility when measurements and source sensitivity approaches suggest titration was outpacing production. In general, CMAQ DDM tends to attribute more O₃ to boundary inflow and less to within-domain NO_X and VOC sources compared to CMAQ source apportionment. The photochemical modeling system was able to capture single source plumes using 1 to 12 km grid resolution with best representation of plume extent and magnitude at the finer resolutions. When modeled at 1 to 12 km grid resolution, primary and secondary PM_2.5 impacts were highest at the source location and decrease as distance increases downwind. The use of coarser grid resolution for single source attribution resulted in predicted impacts highest near the source but lower peak source specific concentrations compared to finer grid resolution simulations because impacts were spread out over a larger area.

Keywords: CMAQ; DDM; NO(2) column; O(3); Source apportionment.

Published by Elsevier B.V.

Grants and funding

EPA999999/ImEPA/Intramural EPA/United States