Contributions to local- and regional-scale formaldehyde concentrations

Journal Article · 02 July 2019 · Atmospheric Chemistry and Physics (Online)

DOI: https://doi.org/10.5194/acp-19-8363-2019 · OSTI ID:1566226

Bastien, Lucas A. J.; Brown, Nancy J.; Harley, Robert A.

Reducing ambient formaldehyde concentrations is a complex task because formaldehyde is both a primary and a secondary air pollutant, with significant anthropogenic and biogenic sources of volatile organic compound (VOC) precursor emissions. This work uses adjoint sensitivity analysis in a chemical transport model to identify emission sources and chemical reactions that influence formaldehyde mixing ratios in the San Francisco Bay Area and within three urbanized sub-areas. For each of these receptors, the use of the adjoint technique allows for efficient calculation of the sensitivity of formaldehyde to emissions of NO_x, formaldehyde, and VOC precursors occurring at any location and time. Formaldehyde mixing ratios are found to be generally higher in summer than in winter. The opposite seasonal trend is observed for the sensitivities of these mixing ratios to formaldehyde emissions. In other words, even though formaldehyde is higher in summer, reducing formaldehyde emissions has a greater impact in winter. In winter, 85%–90% of the sensitivity to emissions is attributed to direct formaldehyde emissions. In summer, this contribution is smaller and more variable, ranging from 27% to 75% among the receptor areas investigated in this study. Higher relative contributions of secondary formation versus direct emissions are associated with receptors located farther away from heavily urbanized and emission-rich areas. In particular, the relative contribution of biogenic VOC emissions (15%–43% in summer) is largest for these receptors. Ethene and other alkenes are the most influential anthropogenic precursors to secondary formaldehyde. Isoprene is the most influential biogenic precursor. Sensitivities of formaldehyde to NO_x emissions are generally negative but relatively small in magnitude compared to sensitivities to VOC emissions. The magnitude of anthropogenic emissions of organic compounds other than formaldehyde is found to correlate reasonably well with their influence on population-weighted formaldehyde mixing ratios at the air-basin scale. This correlation does not hold for ambient formaldehyde in smaller urbanized sub-areas. The magnitude of biogenic emissions does not correlate with their influence in either case.

• Sponsoring Organization: USDOE
• Grant/Contract Number: AC02-05CH11231
• OSTI ID: 1566226
• Journal Information: Atmospheric Chemistry and Physics (Online), Journal Name: Atmospheric Chemistry and Physics (Online) Vol. 19 Journal Issue: 13; ISSN 1680-7324
• Publisher: Copernicus Publications, EGUCopyright Statement
• Country of Publication: Germany
• Language: English