Heterogeneous reactions on model polar stratospheric cloud surfaces: reaction of dinitrogen pentoxide on ice and nitric acid trihydrate

1990 ◽  
Vol 94 (8) ◽  
pp. 3255-3260 ◽  
Author(s):  
Michael A. Quinlan ◽  
Christa M. Reihs ◽  
David M. Golden ◽  
Margaret A. Tolbert
Keyword(s):  
Nitric Acid ◽  
Heterogeneous Reactions ◽  
Dinitrogen Pentoxide ◽  
Polar Stratospheric Cloud

scholarly journals Nitrate formation from heterogeneous uptake of dinitrogen pentoxide during a severe winter haze in southern China

2018 ◽  
Author(s):  
Hui Yun ◽  
Weihao Wang ◽  
Tao Wang ◽  
Men Xia ◽  
Chuan Yu ◽  
...  
Keyword(s):  
Nitric Acid ◽  
Time Resolution ◽  
Southern China ◽  
Fine Particulate Matter ◽  
Measurement Data ◽  
Heterogeneous Reactions ◽  
Chemical Mechanism ◽  
Rural Site ◽  
Phase Reaction ◽  
Dinitrogen Pentoxide

Abstract. Nitrate (NO3−) has become a major component of fine particulate matter (PM2.5) during hazy days in China. However, the role of the heterogeneous reactions of dinitrogen pentoxide (N2O5) in nitrate formation is not well constrained. In January 2017, a severe haze event occurred in the Pearl River Delta (PRD) of southern China during which high levels of PM2.5 (~ 400 μg m−3) and O3 (~ 160 ppbv) were observed at a semi-rural site (Heshan) in the western PRD. Nitrate concentrations were up to 108 μg m−3 (1 h time resolution), and the contribution of nitrate to PM2.5 reached nearly 40 %. Concurrent increases in NO3− and ClNO2 (with a maximum value of 8.3 ppbv in 1 min time resolution) were observed in the first several hours after sunset, indicating an intense N2O5 heterogeneous uptake on aerosols. The formation potential of NO3− via N2O5 heterogeneous reactions was estimated to be 39.7 to 77.3 μg m−3 in the early hours (3 to 6 h) after sunset based on the measurement data, which could completely explain the measured increase in the NO3− concentration during the same time period. Daytime production of nitric acid from the gas-phase reaction of OH + NO2 was calculated with a chemical box model built using the Master Chemical Mechanism (MCM v3.3.1) and constrained by the measurement data. The integrated nocturnal nitrate formed via N2O5 chemistry was comparable to or even higher than the nitric acid formed during the daytime. This study confirms that N2O5 heterogeneous chemistry was a significant source of aerosol nitrate during hazy days in southern China.

scholarly journals Nitrate formation from heterogeneous uptake of dinitrogen pentoxide during a severe winter haze in southern China

2018 ◽  
Vol 18 (23) ◽  
pp. 17515-17527 ◽  
Author(s):  
Hui Yun ◽  
Weihao Wang ◽  
Tao Wang ◽  
Men Xia ◽  
Chuan Yu ◽  
...  
Keyword(s):  
Nitric Acid ◽  
Time Resolution ◽  
Southern China ◽  
Fine Particulate Matter ◽  
Measurement Data ◽  
Heterogeneous Reactions ◽  
Chemical Mechanism ◽  
Rural Site ◽  
Phase Reaction ◽  
Dinitrogen Pentoxide

Abstract. Nitrate (NO3-) has become a major component of fine particulate matter (PM2.5) during hazy days in China. However, the role of the heterogeneous reactions of dinitrogen pentoxide (N2O5) in nitrate formation is not well constrained. In January 2017, a severe haze event occurred in the Pearl River Delta (PRD) of southern China during which high levels of PM2.5 (∼400 µg m−3) and O3 (∼160 ppbv) were observed at a semi-rural site (Heshan) in the western PRD. Nitrate concentrations reached 108 µg m−3 (1 h time resolution), and the contribution of nitrate to PM2.5 was nearly 40 %. Concurrent increases in NO3- and ClNO2 (with a maximum value of 8.3 ppbv at a 1 min time resolution) were observed in the first several hours after sunset, indicating an intense N2O5 heterogeneous uptake by aerosols. The formation potential of NO3- via N2O5 heterogeneous reactions was estimated to be between 29.0 and 77.3 µg m−3 in the early hours (2 to 6 h) after sunset based on the measurement data, which could completely explain the measured increase in the NO3- concentration during the same time period. Daytime production of nitric acid from the gas-phase reaction of OH+NO2 was calculated with a chemical box model built using the Master Chemical Mechanism (MCM v3.3.1) and constrained by the measurement data. The integrated nocturnal nitrate formed via N2O5 chemistry was comparable to or even higher than the nitric acid formed during the day. This study confirms that N2O5 heterogeneous chemistry was a significant source of aerosol nitrate during hazy days in southern China.

scholarly journals Polar processing in a split vortex: early winter Arctic ozone loss in 2012/13

2015 ◽  
Vol 15 (4) ◽  
pp. 4973-5029 ◽  
Author(s):  
G. L. Manney ◽  
Z. D. Lawrence ◽  
M. L. Santee ◽  
N. J. Livesey ◽  
A. Lambert ◽  
...  
Keyword(s):  
Nitric Acid ◽  
Lower Stratosphere ◽  
Polar Vortex ◽  
The Arctic ◽  
Early Winter ◽  
Sudden Stratospheric Warming ◽  
Ozone Loss ◽  
Chlorine Monoxide ◽  
Polar Stratospheric Cloud ◽  
Vortex Split

Abstract. A sudden stratospheric warming (SSW) in early January 2013 caused the polar vortex to split. After the lower stratospheric vortex split on 8 January, the two offspring vortices – one over Canada and the other over Siberia – remained intact, well-confined, and largely at latitudes that received sunlight until they reunited at the end of January. As the SSW began, temperatures abruptly rose above chlorine activation thresholds throughout the lower stratosphere. The vortex was very disturbed prior to the SSW, and was exposed to much more sunlight than usual in December 2012 and January 2013. Aura Microwave Limb Sounder (MLS) nitric acid (HNO3) data and observations from CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) indicate extensive polar stratospheric cloud (PSC) activity, with evidence of PSCs containing solid nitric acid trihydrate particles during much of December 2012. Consistent with the sunlight exposure and PSC activity, MLS observations show that chlorine monoxide (ClO) became enhanced early in December. Despite the cessation of PSC activity with the onset of the SSW, enhanced vortex ClO persisted until mid-February, indicating lingering chlorine activation. The smaller Canadian offspring vortex had lower temperatures, lower HNO3, lower hydrogen chloride (HCl), and higher ClO in late January than the Siberian vortex. Chlorine deactivation began later in the Canadian than in the Siberian vortex. HNO3 remained depressed within the vortices after temperatures rose above the PSC existence threshold, and passive transport calculations indicate vortex-averaged denitrification of about 4 ppbv; the resulting low HNO3 values persisted until the vortex dissipated in mid-February. Consistent with the strong chlorine activation and exposure to sunlight, MLS measurements show rapid ozone loss commencing in mid-December and continuing through January. Lagrangian transport estimates suggest ~ 0.7–0.8 ppmv (parts per million by volume) vortex-averaged chemical ozone loss by late January near 500 K (~ 21 km), with substantial loss occurring from ~ 450 to 550 K. The surface area of PSCs in December 2012 was larger than that in any other December observed by CALIPSO. As a result of denitrification, HNO3 abundances in 2012/13 were among the lowest in the MLS record for the Arctic. ClO enhancement was much greater in December 2012 through mid-January 2013 than that at the corresponding time in any other Arctic winter observed by MLS. Furthermore, reformation of HCl appeared to play a greater role in chlorine deactivation than in more typical Arctic winters. Ozone loss in December 2012 and January 2013 was larger than any previously observed in those months. This pattern of exceptional early winter polar processing and ozone loss resulted from the unique combination of dynamical conditions associated with the early January 2013 SSW, namely unusually low temperatures in December 2012 and offspring vortices that remained well-confined and largely in sunlit regions for about a month after the vortex split.

scholarly journals Technical Note: Evaporation of polar stratospheric cloud particles, in situ, in a heated inlet

2005 ◽  
Vol 5 (1) ◽  
pp. 97-106 ◽  
Author(s):  
T. Eidhammer ◽  
T. Deshler
Keyword(s):  
Particle Size ◽  
Nitric Acid ◽  
Size Distribution ◽  
Technical Note ◽  
Ternary Solution ◽  
Slow Evaporation ◽  
Partial Pressures ◽  
Polar Stratospheric Cloud ◽  
Stratospheric Clouds

Abstract. In December 2001 and 2002 in situ aerosol measurements were made from balloon-borne platforms within polar stratospheric clouds (PSC) which contained particles of supercooled ternary solution (STS), nitric acid trihydrate (NAT) and ice. Particle size and number concentrations were measured with two optical particle counters. One of these included an ~80cm inlet heated to K to evaporate the PSC particles and thus to obtain measurements, within PSCs, of the size distribution of the particles upon which the PSCs condensed. These measurements are compared to models, described here, that calculate the evaporation of PSC particles at and for an inlet transition time of about 0.1s. The modeled evaporation for STS agrees well with the measurements. For NAT the modeled evaporation is less than the evaporation measured. The primary uncertainty concerns the phase and morphology of NAT particles as they are brought to temperatures >50K above equilibrium temperatures for NAT at stratospheric partial pressures. The slow evaporation of NAT in heated inlets could be used to identify a small NAT component within a mixed phase PSC dominated by STS.

Scale‐Up Studies of the Electrosynthesis of Dinitrogen Pentoxide in Nitric Acid

1997 ◽  
Vol 144 (6) ◽  
pp. 2032-2044 ◽  
Author(s):  
J. E. Harrar ◽  
R. Quong ◽  
L. P. Rigdon ◽  
R. R. McGuire
Keyword(s):  
Nitric Acid ◽  
Scale Up ◽  
Dinitrogen Pentoxide

Heterogeneous reactions of soot aerosols with nitrogen dioxide and nitric acid: atmospheric chamber and Knudsen cell studies

2002 ◽  
Vol 36 (36-37) ◽  
pp. 5729-5740 ◽  
Author(s):  
A.Preszler Prince ◽  
J.L. Wade ◽  
V.H. Grassian ◽  
P.D. Kleiber ◽  
M.A. Young
Keyword(s):  
Nitric Acid ◽  
Nitrogen Dioxide ◽  
Heterogeneous Reactions ◽  
Knudsen Cell ◽  
Atmospheric Chamber
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