Snowpack processing of acetaldehyde and acetone in the Arctic atmospheric boundary layer
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- 作者：Guimbaud ; Christophe ; Grannas ; Amanda M. ; Shepson ; Paul B. ; Fuentes ; José ; D. ; Boudries ; Hacene ; et. al.
- 关键词：Acetaldehyde ; Acetone ; Arctic chemistry ; Snowpack ; Polar Sunrise Experiment 2000
- 刊名：Atmospheric Environment
- 出版年：2002
- 出版时间：May - June, 2002
- 年：2002
- 卷：36
- 期：15-16
- 页码：2743-2752
- 全文大小：332 K
文摘
Acetaldehyde (CH3CHO) and acetone (CH3C(O)CH3) concentrations in ambient air, in snowpack air, and bulk snow were determined at Alert, Nunavut, Canada, as a part of the Polar Sunrise Experiment (PSE): ALERT 2000. During the period of continuous sunlight, vertical profiles of ambient and snowpack air exhibited large concentration gradients through the top 
10cm of the snowpack, implying a flux of carbonyl compounds from the surface to the atmosphere. From vertical profile and eddy diffusivity measurements made simultaneously on 22 April, acetaldehyde and acetone fluxes of 4.2(±2.1)×108 and 6.2(±4.2)×108moleculescm−2s−1 were derived, respectively. For this day, the sources and sinks of CH3CHO from gas phase chemistry were estimated. The result showed that the snowpack flux of CH3CHO to the atmosphere was as large as the calculated CH3CHO loss rate from known atmospheric gas phase reactions, and at least 40 times larger (in the surface layer) than the volumetric rate of acetaldehyde produced from the assumed main atmospheric gas phase reaction, i.e. reaction of ethane with hydroxyl radicals. In addition, acetaldehyde bulk snow phase measurements showed that acetaldehyde was produced in or on the snow phase, likely from a photochemical origin. The time series for the observed CH3C(O)CH3, ozone (O3), and propane during PSE 1995, PSE 1998, and ALERT 2000 showed a consistent anti-correlation between acetone and O3 and between acetone and propane. However, our data and model simulations showed that the acetone increase during ozone depletion events cannot be explained by gas phase chemistry involving propane oxidation. These results suggest that the snowpack is a significant source of acetaldehyde and acetone to the Arctic boundary layer.
10cm of the snowpack, implying a flux of carbonyl compounds from the surface to the atmosphere. From vertical profile and eddy diffusivity measurements made simultaneously on 22 April, acetaldehyde and acetone fluxes of 4.2(±2.1)×108 and 6.2(±4.2)×108moleculescm−2s−1 were derived, respectively. For this day, the sources and sinks of CH3CHO from gas phase chemistry were estimated. The result showed that the snowpack flux of CH3CHO to the atmosphere was as large as the calculated CH3CHO loss rate from known atmospheric gas phase reactions, and at least 40 times larger (in the surface layer) than the volumetric rate of acetaldehyde produced from the assumed main atmospheric gas phase reaction, i.e. reaction of ethane with hydroxyl radicals. In addition, acetaldehyde bulk snow phase measurements showed that acetaldehyde was produced in or on the snow phase, likely from a photochemical origin. The time series for the observed CH3C(O)CH3, ozone (O3), and propane during PSE 1995, PSE 1998, and ALERT 2000 showed a consistent anti-correlation between acetone and O3 and between acetone and propane. However, our data and model simulations showed that the acetone increase during ozone depletion events cannot be explained by gas phase chemistry involving propane oxidation. These results suggest that the snowpack is a significant source of acetaldehyde and acetone to the Arctic boundary layer.