Corrigendum to: Atmospheric variation of nitrous acid at different sites in Europe

2007 ◽  
Vol 4 (5) ◽  
pp. 364 ◽  
Author(s):  
Karin Acker ◽  
Detlev Möller
Keyword(s):  
Hydroxyl Radical ◽  
Nitrous Acid ◽  
Field Experiments ◽  
Early Morning ◽  
Mixing Ratio ◽  
Gas Phase Reactions ◽  
Sources And Sinks ◽  
Mixing Ratios ◽  
Secondary Pollutants ◽  
Rural Sites

Environmental context. Nitrous acid (HNO2) is an important source of the hydroxyl radical (OH.), the most important daytime oxidising species that contributes to the formation of ozone as well as of other secondary pollutants in the troposphere. Understanding the sources and sinks of HNO2 is of crucial interest for accurately modelling the chemical composition of the troposphere and predicting future trace gas concentrations. Abstract. Nitrous acid and several other atmospheric components and variables were continuously measured during complex field experiments at seven different suburban and rural sites in Europe. HNO2 is mainly formed by heterogeneous processes and is often accumulated in the nighttime boundary layer. Our results confirm that the photolysis of HNO2 is an important source of the hydroxyl radical, not only in the early morning hours but also throughout the entire day, and is often comparable with the contribution of ozone and formaldehyde photolysis. At all research sites unexpectedly high HNO2 mixing ratios were observed during the daytime (up to several hundred ppt, or pmol mol-1). Moreover, surprisingly, the HNO2 mixing ratio at the three mountain sites often showed a broad maximum or several distinct peaks at midday and lower mixing ratios during the night. Assuming a quickly established photo-equilibrium between the known significant gas phase reactions, only a few ppt HNO2 should be present around noon. The ratio of known sources to sinks indicates a missing daytime HNO2 source of 160-2600 ppt h-1 to make up the balance. Based on these values and on production mechanisms proposed in the literature we hypothesise that the daytime mixing ratio levels may only be explained by a fast electron transfer onto adsorbed NO2.

Atmospheric variation of nitrous acid at different sites in Europe

2007 ◽  
Vol 4 (4) ◽  
pp. 242 ◽  
Author(s):  
Karin Acker ◽  
Detlev Möller
Keyword(s):  
Hydroxyl Radical ◽  
Nitrous Acid ◽  
Field Experiments ◽  
Early Morning ◽  
Mixing Ratio ◽  
Gas Phase Reactions ◽  
Sources And Sinks ◽  
Mixing Ratios ◽  
Secondary Pollutants ◽  
Rural Sites

Environmental context. Nitrous acid (HNO2) is an important source of the hydroxyl radical (OH•), the most important daytime oxidising species that contributes to the formation of ozone as well as of other secondary pollutants in the troposphere. Understanding the sources and sinks of HNO2 is of crucial interest for accurately modelling the chemical composition of the troposphere and predicting future trace gas concentrations. Abstract. Nitrous acid and several other atmospheric components and variables were continuously measured during complex field experiments at seven different suburban and rural sites in Europe. HNO2 is mainly formed by heterogeneous processes and is often accumulated in the nighttime boundary layer. Our results confirm that the photolysis of HNO2 is an important source of the hydroxyl radical, not only in the early morning hours but also throughout the entire day, and is often comparable with the contribution of ozone and formaldehyde photolysis. At all research sites unexpectedly high HNO2 mixing ratios were observed during the daytime (up to several hundred ppt, or pmol mol–1). Moreover, surprisingly, the HNO2 mixing ratio at the three mountain sites often showed a broad maximum or several distinct peaks at midday and lower mixing ratios during the night. Assuming a quickly established photo-equilibrium between the known significant gas phase reactions, only a few ppt HNO2 should be present around noon. The ratio of known sources to sinks indicates a missing daytime HNO2 source of 160–2600 ppt h–1 to make up the balance. Based on these values and on production mechanisms proposed in the literature we hypothesise that the daytime mixing ratio levels may only be explained by a fast electron transfer onto adsorbed NO2.

scholarly journals Assessment of Tropospheric Concentrations of NO2 from the TROPOMI/Sentinel-5 Precursor for the Estimation of Long-Term Exposure to Surface NO2 over South Korea

2021 ◽  
Vol 13 (10) ◽  
pp. 1877
Author(s):  
Ukkyo Jeong ◽  
Hyunkee Hong
Keyword(s):  
South Korea ◽  
Spatial Resolution ◽  
Atmospheric Composition ◽  
Mixing Ratio ◽  
Mean Values ◽  
Mixing Ratios ◽  
Tropospheric No2 ◽  
Korean Ministry ◽  
Surface Mixing ◽  
Rural Sites

Since April 2018, the TROPOspheric Monitoring Instrument (TROPOMI) has provided data on tropospheric NO2 column concentrations (CTROPOMI) with unprecedented spatial resolution. This study aims to assess the capability of TROPOMI to acquire high spatial resolution data regarding surface NO2 mixing ratios. In general, the instrument effectively detected major and moderate sources of NO2 over South Korea with a clear weekday–weekend distinction. We compared the CTROPOMI with surface NO2 mixing ratio measurements from an extensive ground-based network over South Korea operated by the Korean Ministry of Environment (SKME; more than 570 sites), for 2019. Spatiotemporally collocated CTROPOMI and SKME showed a moderate correlation (correlation coefficient, r = 0.67), whereas their annual mean values at each site showed a higher correlation (r = 0.84). The CTROPOMI and SKME were well correlated around the Seoul metropolitan area, where significant amounts of NO2 prevailed throughout the year, whereas they showed lower correlation at rural sites. We converted the tropospheric NO2 from TROPOMI to the surface mixing ratio (STROPOMI) using the EAC4 (ECMWF Atmospheric Composition Reanalysis 4) profile shape, for quantitative comparison with the SKME. The estimated STROPOMI generally underestimated the in-situ value obtained, SKME (slope = 0.64), as reported in previous studies.

scholarly journals Development and application of a new mobile LOPAP instrument for the measurement of HONO altitude profiles in the planetary boundary layer

2009 ◽  
Vol 2 (4) ◽  
pp. 2027-2054 ◽  
Author(s):  
R. Häseler ◽  
T. Brauers ◽  
F. Holland ◽  
A. Wahner
Keyword(s):  
Nitrous Acid ◽  
Ground Level ◽  
Concentration Profiles ◽  
Mixing Ratio ◽  
Above Ground Level ◽  
Mixing Ratios ◽  
New Instrument ◽  
Mobile Measurements ◽  
Southwest Germany ◽  
Absorption Technique

Abstract. The LOPAP (long path absorption) technique has been shown to be very sensitive for the detection of nitrous acid (HONO) in the atmosphere. However, current instruments were mainly built for ground based applications. Therefore, we designed a new LOPAP instrument to be more versatile for mobile measurements and to meet the requirements for airborne application. The detection limit of the new instrument is below 1 ppt at a time resolution of 5 to 7 min. As a first test, the instrument was successfully employed during the ZEPTER-1 campaign in July 2007 on board of the Zeppelin NT airship. During 15 flights on six days we measured HONO concentration profiles over southwest Germany, predominantly in the range between 100 m and 650 m above ground level. On average, a mixing ratio of 34 ppt was observed, almost independently of height. Within a econd campaign, ZEPTER-2 in fall 2008, higher HONO mixing ratios were observed in the Lake Constance area.

scholarly journals Modeling nitrous acid and its impact on ozone and hydroxyl radical during the Texas Air Quality Study 2006

2012 ◽  
Vol 12 (2) ◽  
pp. 5851-5880 ◽  
Author(s):  
B. H. Czader ◽  
B. Rappenglück ◽  
P. Percell ◽  
D. W. Byun ◽  
F. Ngan ◽  
...  
Keyword(s):  
Air Quality ◽  
Hydroxyl Radical ◽  
Gas Phase ◽  
Nitrous Acid ◽  
Organic Materials ◽  
Optical Absorption Spectroscopy ◽  
Ozone Formation ◽  
Mixing Ratios ◽  
Quality Study ◽  
Mist Chamber

Abstract. Nitrous acid (HONO) mixing ratios for the Houston metropolitan area were simulated with the Community Multiscale Air Quality (CMAQ) model for an episode during the Texas Air Quality Study (TexAQS) II in August/September 2006 and compared to in-situ MC/IC (mist-chamber/ion chromatograph) and long path DOAS (Differential Optical Absorption Spectroscopy) measurements at three different altitudes. Several HONO sources were accounted for in simulations, such as gas phase formation, direct emissions, nitrogen dioxide (NO2*) hydrolysis, photo-induced formation from excited NO2* and photo-induced conversion of NO2 into HONO on surfaces covered with organic materials. Compared to the gas-phase HONO formation there was about a tenfold increase in HONO mixing ratios when additional HONO sources were taken into account, which improved the correlation between modeled and measured values. Concentrations of HONO simulated with only gas phase chemistry did not change with altitude, while measured HONO concentrations decrease with height. A trend of decreasing HONO concentration with altitude was well captured with CMAQ predicted concentrations when heterogeneous chemistry and photolytic sources of HONO were taken into account. Heterogeneous HONO production mainly accelerated morning ozone formation, albeit slightly. Also HONO formation from excited NO2 only slightly affected HONO and ozone (O3) concentrations. Photo-induced conversion of NO2 into HONO on surfaces covered with organic materials turned out to be a strong source of daytime HONO. Since HONO immediately photo-dissociates during daytime its ambient mixing ratios were only marginally altered (up to 0.5 ppbv), but significant increase in the hydroxyl radical (OH) and ozone concentration was obtained. In contrast to heterogeneous HONO formation that mainly accelerated morning ozone formation, inclusion of photo-induced surface chemistry influenced ozone throughout the day.

Photo-Induced Heterogeneous Chemistry of Reactive Species on Aerosol Surfaces: Using Photo-Fragmentation Laser Induced Fluorescence for the Measurement of Nitrous Acid Production from Titanium Dioxide Aerosols

2020 ◽  
Author(s):  
Joanna Dyson ◽  
Graham Boustead ◽  
Lauren Fleming ◽  
Mark Blitz ◽  
Daniel Stone ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Nitrous Acid ◽  
Laser Induced Fluorescence ◽  
Heterogeneous Chemistry ◽  
Sources And Sinks ◽  
Atmospheric Species ◽  
Highly Sensitive ◽  
Secondary Pollutants ◽  
Reactive Uptake Coefficient

<p>The hydroxyl radical (OH) is the main oxidant in the troposphere and is vitally important for its role in the removal of greenhouse gases such as methane from the atmosphere. Moreover, the OH radical also has a role in the formation of secondary pollutants such as tropospheric ozone and secondary organic aerosols (SOAs), formed via the oxidation of volatile organic compounds (VOCs). Understanding the sources and sinks of OH within the atmosphere is therefore crucial in order to fully understand the concentration and distribution of trace atmospheric species associated with climate change and poor air quality.</p><p>In polluted environments the dominant source of OH to initiate oxidation is the photolysis of nitrous acid (HONO). Current atmospheric chemistry models underestimate the concentration of HONO indicating a potential missing tropospheric source of HONO. There is a large uncertainty in the production of HONO from the contribution and role of aerosols and heterogeneous chemistry both under light and dark conditions.</p><p>In order to investigate the missing source of HONO from illuminated aerosols and determine its atmospheric relevance, a photo-fragmentation laser induced fluorescence (PF-LIF) instrument coupled to an aerosol flow tube system has been constructed. The PF-LIF instrument provides a highly sensitive measurement of HONO by fragmenting it into OH which is then detected in a low pressure cell by LIF. The aim of this system is to measure the rate of production of HONO from illuminated aerosol surfaces.</p><p>We will present an overview of the PF-LIF instrument and results from experiments investigating the reactive uptake of NO<sub>2</sub> by TiO<sub>2</sub> aerosols to produce HONO. The change in the reactive uptake coefficient as a function of NO<sub>2</sub> concentration and the dependence of HONO production on relative humidity and light intensity will also be discussed.   </p>

scholarly journals Measurement report: Exploring NH<sub>3</sub> behavior in urban and suburban Beijing: comparison and implications

2021 ◽  
Vol 21 (6) ◽  
pp. 4561-4573
Author(s):  
Ziru Lan ◽  
Weili Lin ◽  
Weiwei Pu ◽  
Zhiqiang Ma
Keyword(s):  
Relative Humidity ◽  
Rural Areas ◽  
Urban Site ◽  
Mixing Ratio ◽  
Mixing Ratios ◽  
Different Seasons ◽  
Rural Sites ◽  
Highly Correlated ◽  
Urban And Rural Areas ◽  
Suburban Site

Abstract. Ammonia (NH3) plays an important role in particulate matter formation; hence, its atmospheric level is relevant to human health and climate change. Due to different relative distributions of NH3 sources, concentrations of atmospheric NH3 may behave differently in urban and rural areas. However, few parallel long-term observations of NH3 exist to reveal the different behaviors of NH3 concentrations at urban and rural sites in a same region. In this study, online ammonia analyzers were used to continuously observe atmospheric NH3 concentrations at an urban site and a suburban site in Beijing from 13 January 2018 to 13 January 2019. The observed mixing ratio of NH3 averaged 21±14 ppb (range of 1.6–133 ppb) at the urban site and 22±15 ppb (range of 0.8–199 ppb) at the suburban site. The NH3 mixing ratios at the urban and suburban sites exhibited similar seasonal variations, with high values in summer and spring and low values in autumn and winter. The hourly mean NH3 mixing ratios at the urban site were highly correlated (R=0.849, P<0.01) with those at the suburban site; however, the average diurnal variations in the NH3 mixing ratios at the urban and suburban sites differed significantly, which implies different contributions from NH3 sources and sinks at the urban and suburban sites. In addition to the emission sources, meteorological factors were closely related to the changes in the NH3 concentrations. For the same temperature (relative humidity) at the urban and suburban sites, the NH3 mixing ratios increased with relative humidity (temperature). Relative humidity was the factor with the strongest influence on the NH3 mixing ratio in different seasons at the two sites. The relationships between the NH3 concentrations and temperature (relative humidity) varied from season to season and showed differences between the urban and suburban sites. The reasons for the different relationships need to be investigated in future studies. Higher wind speed mainly from the northwest sector lowered the NH3 mixing ratios at both sites. Similarly to other primary pollutants in Beijing, the NH3 mixing ratios were high when impacted by air masses from the southern sector.

scholarly journals A conceptual framework to quantify the influence of convective boundary layer development on carbon dioxide mixing ratios

2012 ◽  
Vol 12 (6) ◽  
pp. 2969-2985 ◽  
Author(s):  
D. Pino ◽  
J. Vilà-Guerau de Arellano ◽  
W. Peters ◽  
J. Schröter ◽  
C. C. van Heerwaarden ◽  
...  
Keyword(s):  
Carbon Dioxide ◽  
Boundary Layer ◽  
Early Morning ◽  
Mixing Ratio ◽  
Layer Depth ◽  
Free Atmosphere ◽  
Convective Boundary ◽  
Surface Exchange ◽  
Mixing Ratios ◽  
Boundary Layer Dynamics

Abstract. Interpretation of observed diurnal carbon dioxide (CO2) mixing ratios near the surface requires knowledge of the local dynamics of the planetary boundary layer. In this paper, we study the relationship between the boundary layer dynamics and the CO2 budget in convective conditions through a newly derived set of analytical equations. From these equations, we are able to quantify how uncertainties in boundary layer dynamical variables or in the morning CO2 distribution in the mixed-layer or in the free atmosphere (FA) influence the bulk CO2 mixing ratio. We find that the largest uncertainty incurred on the mid-day CO2 mixing ratio comes from the prescribed early morning CO2 mixing ratios in the stable boundary layer, and in the free atmosphere. Errors in these values influence CO2 mixing ratios inversely proportional to the boundary layer depth (h), just like uncertainties in the assumed initial boundary layer depth and surface CO2 flux. The influence of uncertainties in the boundary layer depth itself is one order of magnitude smaller. If we "invert" the problem and calculate CO2 surface exchange from observed or simulated CO2 mixing ratios, the sensitivities to errors in boundary layer dynamics also invert: they become linearly proportional to the boundary layer depth. We demonstrate these relations for a typical well characterized situation at the Cabauw site in The Netherlands, and conclude that knowledge of the temperature and carbon dioxide profiles of the atmosphere in the early morning are of vital importance to correctly interpret observed CO2 mixing ratios during midday.

scholarly journals Simultaneous HONO measurements in and above a forest canopy: influence of turbulent exchange on mixing ratio differences

2010 ◽  
Vol 10 (9) ◽  
pp. 21109-21145 ◽  
Author(s):  
M. Sörgel ◽  
I. Trebs ◽  
A. Serafimovich ◽  
A. Moravek ◽  
A. Held ◽  
...  
Keyword(s):  
Forest Floor ◽  
Forest Canopy ◽  
Early Morning ◽  
Turbulent Exchange ◽  
Mixing Ratio ◽  
Mixing Ratios ◽  
Late Night ◽  
Diel Cycles ◽  
Ground Source ◽  
Photolysis Frequencies

Abstract. We have combined chemical and micrometeorological measurements to investigate the formation and distribution of HONO throughout a forest canopy. HONO was measured simultaneously at two heights, close to the forest floor and just above canopy. The turbulent exchange between the forest and the atmosphere above was studied using vertical profiles of eddy covariance measurements. HONO mixing ratios at both heights showed typical diel cycles with low daytime values (~80 ppt) and high nighttime values (up to 500 ppt), but were influenced by various sources and sinks leading to mixing ratio differences (above canopy minus below) of up to +240 ppt at nighttime. In the late afternoon and early night mixing ratios increased at higher rates near the forest floor, indicating a possible ground source. Due to the simultaneous decoupling of the forest from the air layer above the canopy, mixing ratio differences reached about −170 ppt. From the late night until the early morning mixing ratios above the forest were typically higher than close to the forest floor. For some cases, this could be attributed to advection above the forest, which only partly penetrated the canopy. Measured photolysis frequencies above and below the forest canopy differed by a factor of 10–25 resulting in HONO lifetimes of about 10 min above and 100–250 min below the canopy at noontime. However, these differences of the main daytime HONO sink were not evident in the mixing ratio differences, which were close to zero during the morning hours. Effective turbulent exchange due to a complete coupling of the forest to the air layer above the canopy in the morning has offset the differences caused by the daytime photolytic sink and added to the interplay between different HONO production and loss processes.

scholarly journals Impacts of an unknown daytime nitrous acid source on its daytime concentration and budget, as well as those of hydroxyl, hydroperoxyl, and organic peroxy radicals, in the coastal regions of China

2015 ◽  
Vol 15 (1) ◽  
pp. 807-851 ◽  
Author(s):  
Y. Tang ◽  
J. An ◽  
F. Wang ◽  
Y. Li ◽  
Y. Qu ◽  
...  
Keyword(s):  
Production Rate ◽  
Rural Areas ◽  
Nitrous Acid ◽  
Loss Rate ◽  
Field Experiments ◽  
Peroxy Radicals ◽  
Coastal Regions ◽  
Mixing Ratios ◽  
Inorganic Aerosols ◽  
Urban And Rural Areas

Abstract. Many field experiments have found high nitrous acid (HONO) mixing ratios in both urban and rural areas during daytime, but these high daytime HONO mixing ratios cannot be explained well by gas-phase production, suggesting that an unknown daytime HONO source (Punknown) could exist. The formula Punknown &amp;approx; 19.60 × NO2 × J(NO2) was obtained using observed data from 13 field experiments across the globe. The additional HONO sources (i.e. the Punknown, HONO emissions, and nighttime hydrolysis conversion of nitrogen dioxide (NO2) on aerosols) were coupled into the WRF-Chem model (Weather Research and Forecasting model coupled with Chemistry) to assess the Punknown impacts on the concentrations and budgets of HONO and peroxy (hydroxyl, hydroperoxyl, and organic peroxy) radicals (ROx) (= OH + HO2 + RO2) in the coastal regions of China. Results indicated that the additional HONO sources produced a significant improvement in HONO and OH simulations, particularly in the daytime. Elevated daytime-mean Punknown values were found in the coastal regions of China, with a maximum of 2.5 ppb h−1 in the Beijing–Tianjin–Hebei region. The Punknown produced a 60–250% increase of OH, HO2 and RO2 near the ground in the major cities of the coastal regions of China, and a 5–48% increase of OH, HO2 and RO2 in the daytime meridional-mean mixing ratios within 1000 m above the ground. When the additional HONO sources were included, the photolysis of HONO was dominated in the OH production rate in Beijing, Shanghai and Guangzhou before 10:00 LST with a maximum of 10.01 [7.26 due to the Punknown] ppb h−1 in Beijing, whereas the reaction of HO2 + NO (nitric oxide) was dominated after 10:00 LST with a maximum of 9.38 [7.23] ppb h−1 in Beijing. The whole ROx cycle was accelerated by the additional HONO sources, especially the Punknown. The OH production rate was enhanced by 0.67 [0.64] to 4.32 [3.86] ppb h−1 via the reaction of HO2 + NO, and by 0.85 [0.69] to 4.11 [3.61] ppb h−1 via the photolysis of HONO, and the OH loss rate was enhanced by 0.58 [0.55] to 2.03 [1.92] ppb h−1 via the reaction of OH + NO2 and by 0.31 [0.28] to 1.78 [1.64] ppb h−1 via the reaction of OH + CO (carbon monoxide) in Beijing, Shanghai and Guangzhou. Similarly, the additional HONO sources produced an increase of 0.31 [0.28] to 1.78 [1.64] ppb h−1 via the reaction of OH + CO and 0.10 [0.09] to 0.63 [0.59] ppb h−1 via the reaction of CH3O2 (methylperoxy radical) + NO in the HO2 production rate, and 0.67 [0.61] to 4.32 [4.27] ppb h−1 via the reaction of HO2 + NO in the HO2 loss rate in Beijing, Shanghai and Guangzhou. The above results suggest that the Punknown considerably enhanced the ROx concentrations and accelerated ROx cycles in the coastal regions of China, and could produce significant increases in concentrations of inorganic aerosols and secondary organic aerosols and further aggravate haze events in these regions.

scholarly journals Large mixing ratios of atmospheric nitrous acid (HONO) at Concordia (East Antarctic Plateau) in summer: a strong source from surface snow?

2014 ◽  
Vol 14 (18) ◽  
pp. 9963-9976 ◽  
Author(s):  
M. Legrand ◽  
S. Preunkert ◽  
M. Frey ◽  
Th. Bartels-Rausch ◽  
A. Kukui ◽  
...  
Keyword(s):  
Nitrous Acid ◽  
Austral Summer ◽  
Vertical Gradient ◽  
No Oxidation ◽  
Local Source ◽  
Mixing Ratio ◽  
Model Calculations ◽  
Antarctic Plateau ◽  
Mixing Ratios ◽  
Surface Snow

Abstract. During the austral summer 2011/2012 atmospheric nitrous acid (HONO) was investigated for the second time at the Concordia site (75°06' S, 123°33' E), located on the East Antarctic Plateau, by deploying a long-path absorption photometer (LOPAP). Hourly mixing ratios of HONO measured in December 2011/January 2012 (35 ± 5.0 pptv) were similar to those measured in December 2010/January 2011 (30.4 ± 3.5 pptv). The large value of the HONO mixing ratio at the remote Concordia site suggests a local source of HONO in addition to weak production from oxidation of NO by the OH radical. Laboratory experiments demonstrate that surface snow removed from Concordia can produce gas-phase HONO at mixing ratios half that of the NOx mixing ratio produced in the same experiment at typical temperatures encountered at Concordia in summer. Using these lab data and the emission flux of NOx from snow estimated from the vertical gradient of atmospheric concentrations measured during the campaign, a mean diurnal HONO snow emission ranging between 0.5 and 0.8 × 109 molecules cm−2 s−1 is calculated. Model calculations indicate that, in addition to around 1.2 pptv of HONO produced by the NO oxidation, these HONO snow emissions can only explain 6.5 to 10.5 pptv of HONO in the atmosphere at Concordia. To explain the difference between observed and simulated HONO mixing ratios, tests were done both in the field and at lab to explore the possibility that the presence of HNO4 had biased the measurements of HONO.

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