A study of formaldehyde sources in air

Haiwei Shen, University of Rhode Island

Abstract

Formaldehyde (CH2 O) is a central component of photooxidation chemistry. The atmospheric sources of CH2 O involve a complex mixture of biogenic and anthropogenic volatile organic compounds (VOCs). This study explores the geographical and altitudinal variations of CH2 O production from its precursors over the Eastern U.S. and assesses the contributions from biogenic and anthropogenic VOC emissions to atmospheric CH2 O. Measurements of airborne CH2 O and hydrocarbons over North America and model results were used to evaluate CH2 O production from its precursors. Source attribution results from a photochemical box model indicate 95% of the CH2 O arose in various proportions from a mixture of methane, isoprene, methyl hydroperoxide, methanol, and a peroxyacetyl group. Methane on average contributed 32% at altitudes below 2 km to CH2 O production, 43% in 2-6 km, and 52% in 6-12 km. It was the predominant CH 2 O source in 1-12 km. Isoprene served as a major source of CH2 O (range 0-72%, average 17%) over the southeastern U.S. region within 0-1-km layer. Methyl hydroperoxide was one of the predominant contributors over the ocean and averaged from 6 to 33% in all layers. Production from the peroxyacetyl group and methanol were 7-17% and 10-14% on average in the layers in 0-12 km, respectively. A compound specific radiocarbon analysis technique was developed for atmospheric CH2 O to examine its biogenic and anthropogenic carbon fraction. The method used filter collection, a preparative capillary gas chromatography isolation technique, and AMS detection. Ambient samples were collected on the roof of the CACS building at the Bay Campus of the University of RI, Narragansett, RI. The 14 CH2 O data, 48-hour back trajectories, and VOC observations from the RI Department of Environmental Management were used to assess the relative contributions of biogenic and fossil precursors to CH2 O. The results show a large fraction of fossil/industrial carbon in collected CH2 O samples and imply the precursors of CH 2 O were dominated by fossil/industrial sources even during summer when biogenic sources are expected at their highest. It is suggested that pollutants from upwind coastal cities carried by the southwest sea breeze strongly influenced the site during our limited summer sample collection.

Recommended Citation

Haiwei Shen, "A study of formaldehyde sources in air" (2008). ETD Collection for University of Rhode Island. Paper AAI3346857.
http://digitalcommons.uri.edu/dissertations/AAI3346857