Journal of Atmospheric Chemistry

Current research reports and chronological list of recent articles.


The international scientific Journal of Atmospheric Chemistry is devoted to the study of the chemistry of the atmosphere, with particular emphasis on the region below about 100 km. The strongly interdisciplinary nature of atmospheric chemistry means that it embraces a great variety of sciences.

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Journal of Atmospheric Chemistry - Abstracts



Photochemical activation of chlorine by iron-oxide aerosol

Abstract

The photochemical activation of chlorine by dissolved iron in artificial sea-salt aerosol droplets and by highly dispersed iron oxide (Fe2O3) aerosol particles (mainly hematite, specific surface ~150 m2 g−1) exposed to gaseous HCl, was investigated in humidified air in a Teflon simulation chamber. Employing the radical-clock technique, we quantified the production of gaseous atomic chlorine (Cl) from the irradiated aerosol. When the salt aerosol contained Fe2O3 at pH 6, no significant Cl production was observed, even if the dissolution of iron was forced by “weathering” (repeatedly freezing and thawing for five times). Adjusting the pH in the stock suspension to 2.6, 2.2, and 1.9 and equilibrating for one week resulted in a quantifiable amount of dissolved iron (0.03, 0.2, and 0.6 mmol L−1, respectively) and in gaseous Cl production rates of ~1.6, 6, and 8 × 1021 atoms cm−2 h−1, respectively. In a further series of experiments, the pure Fe2O3 aerosol was exposed to various levels of gaseous hydrogen chloride (HCl). The resulting Cl production rates ranged from 8 × 1020 Cl atoms cm−2 h−1 (at ~4 ppb HCl) to 5 × 1022 Cl atoms cm−2 h−1 (at ~350 ppb HCl) and confirmed the uptake and conversion of HCl to atomic Cl (at HCl to Cl conversion yields of 2–5 %, depending on the relative humidity). The Fe2O3 experiments indicate that iron-induced Cl formation may be important for highly soluble combustion-aerosol particles in marine environments in the presence of gaseous HCl.


Datum: 14.04.2016


Seasonal variation of bromocarbons at Hateruma Island, Japan: implications for global sources

Abstract

High-frequency measurements of dibromomethane (CH2Br2) and bromoform (CHBr3) at Hateruma Island, in the subtropical East China Sea, were performed using automated preconcentration gas chromatography/mass spectrometry. Their baseline concentrations, found in air masses from the Pacific Ocean, were 0.65 and 0.26 ppt, respectively, in summer and 1.08 and 0.87 ppt, respectively, in winter. Air masses transported from Southeast Asia were rich in bromocarbons, suggesting strong emissions in this area. The passage of cold fronts from the Asian continent was associated with sharp increases in observed concentrations of bromocarbons derived from coastal regions of the continent. Comparison of the relationships between [CH2Br2]/[CHBr3] and [CHBr3] in the Hateruma Island data with those in monthly mean data from 14 globally distributed U.S. National Oceanic and Atmospheric Administration ground stations suggested that these gases are produced primarily from a common process on a global scale.


Datum: 13.04.2016


Ambient volatile organic compounds in the atmosphere of industrial central India

Abstract

Volatile organic compounds (VOCs) are an important group of compounds because of their role in atmospheric chemistry and the risk they pose to human health and ecosystem. Therefore, the interest in determining VOCs in the atmosphere has increased over the last few decades to understand their emission, distribution, and sources. Considering the expanding urbanization and increasing use of fuels, very limited data of VOCs in India is available. This paper describes the chemical analysis of 12 light VOCs in 144 ambient air samples collected from three different sites near Raipur, India during a period of April, 2006-March, 2007 in order to understand their temporal and spatial distributions. This data has provided some important insights into the VOC profile, for the first time, of an industrial area in India. The annual average concentrations of all 12 VOCs in our study ranged from 43.2 to 160.4 μg m−3 (mean: 95.6 ± 31.0). The annual average concentration of individual VOCs in Raipur region ranged from 3.4 μg m−3 for xylenes to 18.3 μg m−3 for n-butane. n-Butane, i-butane, and propane were the three most abundant pollutants among all of the VOCs measured. The observed concentrations of these compounds in Raipur region were comparable to other Asian cities with some exceptions. The levels of total VOCs showed seasonal variations with a statistically significant winter maximum and lower values during summer and monsoon ranging from 55.9 ± 9.9 μg/m3 in August to 144.5 ± 15.5 μg/m3 in January. Sources of these VOCs have been described using species ratios and correlation studies.


Datum: 05.04.2016


A method for the selective measurement of HO 2 and RO 2 radical concentrations using a Nafion-PERCA system

Abstract

An instrument is developed for the measurement of peroxy radical using chemical amplification coupled with NO2-luminol chemiluminescence detection. The chain length of 147 ± 10 (1σ) is determined by an HO2 source that uses the photolysis of water vapor under 184.9 nm in air. A Nafion system equipped with a Nafion tube of ~2.2 mm external diameter and 350 mm length is employed in the PERCA instrument (Nafion-PERCA system). When flowing an air sample containing HO2 through the Nafion system, it is found that - 94.6 % of HO2 is removed. In contrast, only 17.8 % of RO2 radicals (a mixtures of CH3O2 and CH3C(O)O2 with a ratio of 1.1:0.9) are removed. The results indicate the Nafion system has a good selective removing performance of HO2 radical during the PERCA measurement. Therefore, the method could be applied to ambient and laboratory measurements of absolute concentrations of RO2 as well as the sum of HO2 and RO2.


Datum: 01.04.2016


Analysis of chemical characteristics of PM 2.5 in Beijing over a 1-year period

Abstract

Beijing is one of the largest and most densely populated cities in China. PM2.5 (fine particulates with aerodynamic diameters less than 2.5 μm) pollution has been a serious problem in Beijing in recent years. To study the temporal and spatial variations in the chemical components of PM2.5 and to discuss the formation mechanisms of secondary particles, SO2, NO2, PM2.5, and chemical components of PM2.5 were measured at four sites in Beijing, Dingling (DL), Chegongzhuang (CG), Fangshan (FS), and Yufa (YF), over four seasons from 2012 to 2013. Fifteen chemical components, including organic carbon (OC), elemental carbon (EC), K+, NH4 +, NO3 , SO4 2−, Cl, Al, Ca, Fe, Mg, Na, Pb, Si, and Zn, were selected for analysis. Overall, OC, SO4 2−, NO3 , and NH4 + were dominant among 15 components, the annual average concentrations of which were 22.62 ± 21.86, 19.39 ± 21.06, 18.89 ± 19.82, and 13.20 ± 12.80 μg·m−3, respectively. Compared with previous studies, the concentrations of NH4 + were significantly higher in this study. In winter, the average concentrations of OC and EC were, respectively, 3 and 2.5 times higher than in summer, a result of coal combustion during winter. The average OC/EC ratios over the four sites were 4.9, 7.0, 8.1, and 8.4 in spring, summer, autumn, and winter, respectively. The annual average [NO3 ]/[SO4 2−] ratios in DL, CG, FS, and YF were 1.01, 1.25, 1.08, and 1.12, respectively, which were significantly higher than previous studies in Beijing, indicating that the contribution ratio of mobile source increased in recent years in Beijing. Analysis of correlations between temperature and relative humidity and between SOR ([SO4 2−]/([SO4 2−] + [SO2])) and NOR ([NO3 ]/([NO3 ] + [NO2])) indicated that gas-phase oxidation reactions were the major formation mechanism of SO4 2− in spring and summer in urban Beijing, whereas slow gas-phase oxidation reactions and heterogeneous reactions both occurred in autumn and winter. NO3 was mainly formed through year-round heterogeneous reactions in urban Beijing.


Datum: 01.04.2016


Competing impact of anthropogenic emissions and meteorology on the distribution of trace gases over Indian region

Abstract

The spatial distribution of trace gases exhibit large spatial heterogeneity over the Indian region with an elevated pollution loading over densely populated Gangetic Plains (IGP). The contending role and importance of anthropogenic emissions and meteorology in deciding the trace gases level and distribution over Indian region, however, is poorly investigated. In this paper, we use an online regional chemistry transport model (WRF/Chem) to simulate the spatial distribution of trace gases over Indian region during one representative month of only three meteorological seasons namely winter, spring/summer and monsoon. The base simulation, using anthropogenic emissions from SEAC4RS inventory, is used to simulate the general meteorological conditions and the realistic spatial distribution of trace gases. A sensitivity simulation is conducted after removing the spatial heterogeneity in the anthropogenic emissions, i.e., with spatially uniform emissions to decouple the role of anthropogenic emissions and meteorology and their role in controlling the distribution of trace gases over India. The concentration levels of Ozone, CO, SO2 and NO2 were found to be lower over IGP when the emissions are uniform over India. A comparison of the base run with the sensitivity run highlights that meteorology plays a dominant role in controlling the spatial distribution of relatively longer-lived species like CO and secondary species like Ozone while short-lived species like NOX and SO2 are predominantly controlled by the spatial variability in anthropogenic emissions over the Indian region.


Datum: 01.03.2016


Ozone and secondary organic aerosol formation from Ethylene-NO x -NaCl irradiations under different relative humidity conditions

Abstract

The formation of ozone and secondary organic aerosol (SOA) from ethylene-NO x -NaCl(aerosol) irradiations was studied under various relative humidity (RH) conditions in an indoor smog chamber. In the absence of NaCl seed aerosols, SOA was hardly formed and peak O3 concentrations decreased linearly with increasing RH in ethylene irradiations. For the irradiations with NaCl seed aerosols, when RH <48 % (efflorescence relative humidity of NaCl), NaCl existed as solid phase and had little effect on peak O3 concentrations. The infrared spectra from sampled particles showed that SOA was rarely formed on solid NaCl particles. However, when NaCl was in the aqueous phase as RH ≥ 48 %, the peak O3 concentration was sharply reduced by over 20 % as compared to experiments without NaCl aerosol, and the absorption of NaNO3 in aerosols was coincidently increased with RH. Model results indicated that the heterogeneous reaction of N2O5 with aqueous NaCl aerosols was the main cause for the sharp decrease of O3. Besides, the absorptions from C-H, C = O, ONO2 and COO groups all greatly increased with RH. Our results show that SOA from ethylene-NOx irradiations was mainly formed through aqueous reactions. The yields of SOA from ethylene were measured to be 1.5 and 2.3 % at RH of 65 and 84 %, respectively.


Datum: 01.03.2016


Biogenic volatile compound emissions from a temperate forest, China: model simulation

Abstract

Emissions of biogenic volatile organic compounds (BVOC) were measured using a relaxed eddy accumulation (REA) technique on an above-canopy tower in a temperate forest (Changbai Mountain, Jilin province, China) during the 2010 and 2011 summer seasons. Solar global radiation and photosynthetically active radiation (PAR) were also measured. Based on PAR energy dynamic balance, an empirical BVOC emission and PAR transfer model was developed that includes the processes of BVOC emissions and PAR transfer above the canopy level, including PAR absorption and consumption, and scattering by gases, liquids, and particles (GLPs). Simulated emissions of isoprene and monoterpenes were in agreement with observations. The averages of the relative estimator biases for the flux were 39.3 % for isoprene, and 27.1 % for monoterpenes in the 2010 and 2011 growing seasons, with NMSE (normalized mean square error) values of 0.133 and 0.101, respectively. The observed and simulated mean diurnal variations of isoprene and monoterpenes in the 2010 and 2011 growing seasons were evaluated for the validation of the empirical model. Under observed atmospheric conditions, the sensitivity analysis showed that emissions of isoprene and monoterpenes were more sensitive to changes in PAR than to water vapor content or to the magnitude of the scattering factor. The emissions of isoprene and monoterpenes in the 2010 and 2011 growing seasons (from June to September) were estimated using this empirical model along with hourly observational data, with mean hourly emissions of 1.71 and 1.55 mg m−2 h−1 for isoprene, and 0.48 and 0.47 mg m−2 h−1 for monoterpenes in 2010 and 2011, respectively. As formaldehyde (HCHO) is considered as the main oxidation product of isoprene and monoterpenes, it is necessary to investigate the link between HCHO and BVOC emissions. GOME-2 HCHO vertical column densities (VCDs) can be used to estimate BVOC emission fluxes in the Changbai Mountain temperate forest.


Datum: 01.03.2016


Carbonaceous aerosols over Pune and Hyderabad (India) and influence of meteorological factors

Abstract

Sampling of particulate matter with aerodynamic diameter cut off at 2.5 μm (PM2.5) has been carried out over a semi urban site of Pune and an urban site of Hyderabad. Analysis of elemental Carbon (EC) and Organic Carbon (OC) present in PM2.5 was carried out using advanced Desert Research Institute’s (DRI) Thermal/Optical Carbon Analyzer operated on IMPROVE_ A (Interagency Monitoring of Protected Visual Environments_ A) protocol. It is found that average concentration of EC and OC both at Pune and Hyderabad was highest during winter season and lowest during monsoon season. Winter high is mainly controlled by inversion, whereas monsoon low is due to rain-out and wash-out process. OC/EC ratio showed higher variation over Pune compared to that over Hyderabad in different seasons, indicating divergent sources of emission of OC and EC at Pune. Formation of Secondary Organic Carbon (SOC) has also been identified as one of the reasons for wide variation in OC/EC ratio value in different seasons over both the sites.


Datum: 01.03.2016


Analysis of bulk precipitation chemistry in Serbia for the period from 1982 to 2010

Abstract

Bulk precipitation samples collected daily through bulk collectors at eight meteorological stations in Serbia were analyzed for their chemical composition. The data covers time series, from 20 to 28 years, in the period between 1982 and 2010. The most abundant ion in the samples was sulfate. Only 0.17 % of all samples were from strong acid rains (pH < 3.5). The relatively high average pH values (5.94–6.26) of the collected precipitation indicate the neutral or alkaline nature of local rainwater. Trends in both the annual amount and the composition of precipitation were tested by the nonparametric Mann–Kendall test and Sen’s slope estimator. Significant increasing trend of precipitation was identified for almost all stations. Rebuilding activities after the bombing of Serbia in 1999 were identified as a possible anthropogenic cause of the sharp increase of some ions (Ca2+) in the first year following the bombing. The origin of air masses arriving at one particular station was examined using two-dimensional backward trajectories. Western sectors (W, SW and NW) accounted for almost half (44.3 %) of all rainy days, while eastern sectors (SE, E and NE) brought only 10.4 % of all rainy days. The distribution, per sector, of volume-weighted concentrations of sulfate, nitrate, ammonium, calcium, potassium, magnesium, chloride and sodium ions, as well as the amount of precipitation and its pH values for one station, was also analyzed. Rainwater from the SE and S sectors was the most polluted.


Datum: 01.03.2016


Chemical and isotopic interpretation of major ion compositions from precipitation: a one-year temporal monitoring study in Wrocław, SW Poland

Abstract

The chemical compositions (Na+, NH4 +, K+, Mg2+, Ca2+, Cl, NO2 , NO3 , SO4 2−, HCO3 ) of wet precipitation and nitrogen isotope compositions δ15N(NH4 +) were studied from January to December 2010 in Wrocław (SW Poland). Results of a principle component analysis show that 82 % of the data variability can be explained by three main factors: 1) F1 (40 %) observed during vegetative season (electrical conductivity, HCO3 , NO3 , NO2 , NH4 + and SO4 2−), mainly controlling rainwater mineralization; 2) F2 (26 %) observed during vegetative and heating seasons (K+, Ca2+ and Mg2+), probably representing a combination of two processes: anthropogenic dusts and fertilizers application in agricultural fields, and 3) F3 (16 %) reported mainly during heating season (Na+ and Cl) probably indicating the influence of marine aerosols. Variations of δ15N(NH4 +) from −11.5 to 18.5 ‰ identify three main pathways for the formation of NH4 +: 1) equilibrium fractionation between NH3 and NH4 +; 2) kinetic exchange between NH3 and NH4 +; 3) NH4 + exchange between atmospheric salts particles and precipitation. The coupled chemical/statistical analysis and δ15N(NH4 +) approach shows that while fossil fuels burning is the main source of NH4 + in precipitation during the heating season, during the vegetative season NH4 + originates from local sewage irrigation fields in Osobowice or agricultural fertilizers.


Datum: 01.03.2016


Optical properties and chemical apportionment of summertime PM 2.5 in the suburb of Nanjing

Abstract

A field measurement of aerosol optical properties and chemical composition was carried out from August 25, 2012 to September 6, 2012 in Nanjing, China. A three-wavelength Photo-Acoustic Soot Spectrometer (PASS-3) was used to measure aerosol scattering and absorption coefficient (B sca and B abs ) with the wavelength dependent (405, 532, 781 nm). Samples were also collected by a Particle into Liquid Sampler (PILS) with a time resolution of 1 hour and water soluble chemical composition was analyzed by ion chromatography (IC). The hourly average B sca were 239.9 ± 115.3, 185.9 ± 99.3 and 93.8 ± 59.8 Mm−1 while the average B abs were 33.5 ± 21.8, 23.9 ± 15.7 and 16.7 ± 11.7 Mm−1 for 405, 532 and 781 nm. The air mass from Shandong province to Northwest of Nanjing (SN) brought rich chemical composition which can enhance aerosol optical properties. The largest B sca (~389.9, 321.9, 180.5 Mm−1), B abs (~59.7, 43.0, 31.0 Mm−1), ω532 (~0.89) and lowest visibility (~3.2Km), Å sca (405/781) (~1.19) were observed during SN period. The mass concentrations of organic carbon (OC), elemental carbon (EC) and water soluble inorganic ions (NH4 +, K+, NO3 , and SO4 2−) also continued to increase. However, aerosol optical properties and chemical composition kept stable for the episode with the air mass from Oceanic Regions (OR). Ammonium sulfate ((NH4)2SO4), ammonium nitrate (NH4NO3), organic mass (OM), elemental carbon (EC), fine soil (FS) and sea salt (SS) contributed 49.1, 4.0, 31.6, 9.3, 5.9, and 0.1 % to the total extinction coefficient in summer. (NH4)2SO4, OM and EC were dominant chemical components and the total contribution of them reached to 90 % of the dry aerosol extinction. The proportion of (NH4)2SO4 increased whereas OM and EC showed a decrease during SN period. Our study indicated that the summertime aerosol pollution at the northern suburb of Nanjing was mainly attributed to agricultural biomass burning and secondary aerosol formation. The long-range transport plays an important role in the formation of haze episodes in summertime of Nanjing.


Datum: 27.02.2016


Analysis of photosynthetically active radiation and applied parameterization model for estimating of PAR in the North China Plain

Abstract

As photosynthetically active radiation (PAR) variability and PAR estimating methods play an important role in climate change and ecological process research, PAR variation trends and broadband global solar radiation (R s ) ratios (PAR/R s ) in the North China Plain (NCP) are examined using in situ PAR and R s observed data for 2005 to 2011. The annual average PAR value found in the NCP is 22.9 mol m−2 d−1. The highest and lowest values were recorded at Changwu and Luancheng sites, respectively. The highest PAR/R s value was found in Jiaozhouwan due to large water vapor volumes present in this area. PAR/R s levels have increased in the NCP due to a decrease in fine aerosols and increase in water vapor concentration. From these analysis results, a parameterization model that can be applied to all sky conditions was checked. Empirical estimation model comparisons for obtaining PAR values indicate that model was least accurate when R s was used independently. When the model included R s, the clearness index (K s) and the solar zenith angle, the model estimated PAR values with acceptable accuracy. A parameterization model was constructed by considering K s and attenuation factors of PAR under clear weather conditions (ρ clear). The improved parameterization model more accurately predicts values for local sites and for various observation sites.


Datum: 25.02.2016


Effect of temperature on the methyl chloride production rate in a marine phytoplankton, Phaeodactylum tricornutum

Abstract

Methyl halides such as methyl chloride (CH3Cl) are known to be important carriers of halogen from the ocean to the atmosphere, and the halogens they release into the stratosphere by photolysis catalyze ozone depletion. Marine phytoplankton have been reported as a source of CH3Cl, but the effects of environmental temperature on the CH3Cl production by phytoplankton have not been investigated. In this study, we investigated the effects of temperature on the production of CH3Cl in the culture of a marine diatom, Phaeodactylum tricornutum CCMP 630, incubated at 10, 15, 20, 25, and 30 °C. CH3Cl concentrations in cultured samples were determined using purge and trap gas chromatograph–mass spectrometry. Phytoplankton growth was monitored by measuring the chlorophyll a concentrations. CH3Cl production was observed for several weeks at four different temperatures ranging from 10 to 25 °C. The CH3Cl production from P. tricornutum was increased with increasing temperature from 10 to 25 °C, and the maximum production rate for CH3Cl was 0.21~0.26 μmol (g chlorophyll a)−1 d−1 at 25 °C, which was several times higher than that at 10 °C (~0.03 μmol (g chlorophyll a)−1 d−1). The Arrhenius equation was successfully used to characterize the effects of temperature on the production rates of CH3Cl in the culture of P. tricornutum. Our results suggest that water temperature directly affects CH3Cl production derived from P. tricornutum and that water temperature would be a significant factor for estimating the emissions of CH3Cl from marine environments.


Datum: 23.02.2016


Mass spectrometric study of aged benzene secondary organic aerosol in the presence of dry ammonium sulfate

Abstract

Inorganic seed particles have relatively large surface area, and play an important role in the formation and aging of secondary organic aerosol (SOA). The effects of dry (NH4)2SO4 which is the most commonly found in urban atmosphere on the aged benzene SOA were qualitatively studied utilizing aerosol laser time-of-flight mass spectrometer (ALTOFMS) coupled with Fuzzy C-Means (FCM) clustering algorithm in this study. Experimental results indicated that nitrophenol, oxocarboxylic acid, epoxide products are the predominant components in the aged benzene SOA in the presence of low concentration (about 10 μg m−3) of dry (NH4)2SO4. These aged products are the same as the previously obtained aged benzene SOA without (NH4)2SO4 seed aerosol, indicating that low concentration of dry (NH4)2SO4 acts just as the nucleation or condensation center of the SOA, and do not affect the chemical composition of SOA. However, 1 H-imidazole, 1 H-imidazole-2-carbaldehyde, hydrated 1 H-imidazole-2-carbaldehyde, 2,2′-biimidazole, hydrated N-glyoxal substituted 1 H-imidazole, N-glyoxal substituted hydrated 1 H-imidazole-2- carbaldehyde, hydrated mono glyoxal substituted hydrated 1 H-imidazole-2-carboxaldehyde, mono glyoxal substituted 2,2-biimidazole and hydrated glyoxal dimer substituted imidazole which are formed from ammonium ion reaction with glyoxal are the major particulate products in the aged benzene SOA in the presence of high concentration (about 100 μg m−3) of dry (NH4)2SO4. The retention of water on the dry (NH4)2SO4 particles creates ammonium ion, which can promote the formation of high-molecular-weight (HMW) products through multiphase reactions such as hydration and polymerization of aldehydes form from OH-initiated oxidation of benzene.


Datum: 02.02.2016


Dimethyl sulfide and other biogenic volatile organic compound emissions from branching coral and reef seawater: potential sources of secondary aerosol over the Great Barrier Reef

Abstract

Volatile organic compounds (VOCs) in the headspace of bubble chambers containing branches of live coral in filtered reef seawater were analysed using gas chromatography with mass spectrometry (GC-MS). When the coral released mucus it was a source of dimethyl sulfide (DMS) and isoprene; however, these VOCs were not emitted to the chamber headspace from mucus-free coral. This finding, which suggests that coral is an intermittent source of DMS and isoprene, was supported by the observation of occasional large pulses of atmospheric DMS (DMSa) over Heron Island reef on the southern Great Barrier Reef (GBR), Australia, in the austral winter. The highest DMSa pulse (320 ppt) was three orders of magnitude less than the DMS mixing ratio (460 ppb) measured in the headspace of a dynamically purged bubble chamber containing a mucus-coated branch of Acropora aspera indicating that coral reefs can be strong point sources of DMSa. Static headspace GC-MS analysis of coral fragments identified mainly DMS and seven other minor reduced sulfur compounds including dimethyl disulfide, methyl mercaptan, and carbon disulfide, while coral reef seawater was an indicated source of methylene chloride, acetone, and methyl ethyl ketone. The VOCs emitted by coral and reef seawater are capable of producing new atmospheric particles < 15 nm diameter as observed at Heron Island reef. DMS and isoprene are known to play a role in low-level cloud formation, so aerosol precursors such as these could influence regional climate through a sea surface temperature regulation mechanism hypothesized to operate over the GBR.


Datum: 22.01.2016


Multi-species chemical data assimilation with the Danish Eulerian hemispheric model: system description and verification

Abstract

Satellite retrievals of atmospheric composition provide a wealth of data on a global scale. These complement results from atmospheric chemistry-transport models (CTMs), and can be combined using data assimilation. We present two assimilation schemes coupled to the Danish Eulerian Hemispheric Model (DEHM), a three-dimensional, off-line CTM with full photochemistry: a variant on the ensemble Kalman filter and the three-dimensional variational scheme. The aim of this paper is to describe the two schemes and present an initial assessment of their impacts on model skill. Retrievals of multiple atmospheric trace gases are assimilated, namely: NO2 tropospheric column densities, CH4 total column densities, and partial column concentrations of O3, CO and CH4; these data are retrieved from four satellite sensors. Data for each species are assimilated independently of one another, and other species are only adjusted indirectly via the model’s chemistry and dynamics. Assimilation results are compared with measurements from surface monitoring stations and other satellite retrievals, and preliminary validation results are presented.Reference simulations (without assimilation) grossly underestimate surface CO concentrations, and both assimilation schemes eliminate this large and systematic model bias. The assimilation improves the spatial correlation of modelled CO with surface observations, and improves the spatial correlation between forecasts and retrievals for CO, NO2 and O3. Results for CH4 show a loss of skill due to a mismatch in model bias between two assimilated CH4 data-sets. Finally, we discuss differences in methodology and results between this paper and a recent study on multi-species chemical data assimilation. Joint optimisation of initial conditions and emission rates offers a promising direction for improving modelled boundary-layer concentrations.


Datum: 22.12.2015


A study on the precipitation in Izmir, Turkey: chemical composition and source apportionment by receptor models

Abstract

The chemistry of rainwater was studied in three sites of a metropolitan city of Turkey to determine the spatial variation, sources affecting composition and the extent of their influence. The acidity of rainwater, Ca, Co, Cr, Zn, Ba, V and Ni showed significant spatial variations. The most of measured species were moderately to extremely enriched compared to the local soil, which is likely arisen from the anthropogenic activities. SO4 2−, K and Ca were found to be predominantly non-sea origin. Two receptor models, Positive Matrix Factorization (PMF) and Chemical Mass Balance (CMB), agreed well on the source contribution estimations of Al, K, Zn, V, Pb and Cr. The PMF and CMB resolved very similar source contribution profiles to the elemental concentrations of Ca, Zn, V, Pb, K and Na, which the majority of those resulted from mineral industries, bell casting+steel industries, fossil fuel burning, biomass burning+sea salt and sea salt, respectively. The PMF resolved the source contributions of long-transported emissions, particularly for Ba, Sr and Mn, which could not be estimated by the CMB.


Datum: 28.11.2015


A new continuous measurement method for gaseous ammonia by counter-current flow tube sampling and indophenol reaction

Abstract

Ammonia (NH3) is the most abundant alkaline gas in the atmosphere and plays a key role in atmospheric chemistry. Reliable and high-time-resolution data for gaseous ammonia are necessary to understand the sources and sinks of ammonia gas in ambient air. In the present study, a sensitive and continuous instrument for measuring gaseous ammonia was developed. Ammonia gas in ambient air was collected in an aqueous solution using a counter-current flow tube (CCFT) sampler. Then, ammonium formed in the aqueous solution was detected by the indophenol method. Based on a CCFT length of 50 cm and air flow rate of 1 L/min, the collection efficiency exceeded 98.5 % at an ammonia mixing ratio of up to 120 ppbv. The detection limit of this method was 0.062 ppbv. Interferences from several gases were investigated, and the results showed that the present method was not affected by NOx, O3, SO2, HONO, methylamine, formaldehyde, hydrogen sulfide or a mixture of these gases. The most important result was that only gaseous ammonia was detected in the present method without any interference from the particulate ammonium in ambient air. Comparisons with data based on the dry denuder method indicated that the present method showed good agreement with the denuder method.


Datum: 21.10.2015


Carbon isotopic ( 14 C and 13 C) characterization of fossil-fuel derived dissolved organic carbon in wet precipitation in Shandong Province, China

Abstract

We present results from a 1-year study of radiocarbon and stable carbon isotope measurement of dissolved organic carbon (DOC) of wet precipitation samples collected in the Shandong province of China. A total of 32 rainfall and 4 snow samples were collected from two coastal cities (Qingdao and Yantai) and one inland site (Taian) during 2014. Concentrations of DOC in the rainwater and snow samples varied widely from 28 to 616 μM. In general, rainwater originating from marine sources had relatively low DOC concentrations compared with continentally generated precipitation. Values of δ13C-DOC and Δ14C-DOC in the snow and rainwater ranged from −19.0 to −29.4 ‰ and −23 to −494 ‰, with corresponding radiocarbon ages of 125 to 5410 years before present. The dominant DOC in the wet precipitation had a relatively old 14C age (average 2841 years) and a depleted 13C value (average −24.4 ‰), indicating the mixing of contemporary organic carbon with 14C-depleted fossil fuel-derived soluble organic carbon in the atmosphere. Using a dual isotopic two-endmember model, we calculate that 7 % to 52 % of DOC in the snow and rainfall originated from fossil fuels. It is estimated that the flux of DOC in continental rainfall of China is 23 × 1012 g C yr−1 and of this, 7.1 × 1012 g C yr−1 could be fossil-fuel OC. On a global scale, the DOC flux in rainfall is estimated to be 357 Tg C yr−1, and 110 Tg C yr−1 could be fossil fuel-derived. Our study demonstrates that wet precipitation is an important removal process for old fossil fuel carbon from the atmosphere. This removal mechanism could play an important role in the carbon cycle, especially for the anthropogenically derived fraction, and it should be taken into consideration in global carbon cycle models.


Datum: 12.10.2015






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