Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 115, Issue 6, Pages 1186-1191Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1714715115
Keywords
NMVOC; eddy covariance; urban emissions; air pollution; mass spectrometry
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Funding
- EC Seventh Framework Program (Marie Curie Reintegration Program, ALP-AIR) [334084]
- Austrian National Science Fund [P26931, P30600]
- Austrian Science Fund (FWF) [P30600, P26931] Funding Source: Austrian Science Fund (FWF)
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Atmospheric chemistry is fueled by a large annual influx of non-methane volatile organic compounds (NMVOC). These compounds influence ozone formation, lead to secondary organic aerosol production, and play a significant role for the oxidizing capacity of the atmosphere. The anthropogenic NMVOC budget is considerably uncertain due to the diversity of urban emission sources. Here, we present comprehensive observations of urban NMVOC eddy covariance fluxes using a newly designed proton-transfer-reaction quadrupole interface time-of-flight mass spectrometer. We found emission fluxes of a surprisingly large pool of oxygenated NMVOCs (OVOCs) with an appreciable fraction of higher oxidized OVOCs that cannot be explained by known fast photochemical turnaround or current primary emission estimates. Measured OVOC/NMVOC bulk flux ratios are two to four times higher than inferred from aggregated anthropogenic emission inventories. Extrapolating these results would double the global anthropogenic NMVOC flux. In view of globally accelerating urbanization, our study highlights the need to reevaluate the influence of anthropogenic NMVOC on atmospheric chemistry, human health, and the climate system.
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