Relationships between emission sources and air mass characteristics in East Asia during the TRACE-P period

Long-range transport of pollutants influenced by anthropogenic and natural emission sources in East Asia is investigated by using backward trajectory analysis along the NASA TRACE-P flight tracks and a numerical simulation with the three-dimensional chemical transport model (STEM-2k1). Observation-based regional distributions of trace gases are reconstructed using the observations obtained by measurements on board the DC-8 and P3-B aircrafts. Systematic features of the spatial distribution for each species are identified. It is found that the observed concentrations of CO and some NMHCs, and the ratios between these species, are highly associated with the source distribution features and their regional characteristics. Reconstructed fields of the observed and modeled ethane/CO and ethane/propane are found to reproduce well the estimated emission ratios in East Asia. We also investigated the time rate of change of the concentration of species and their ratio along the trajectory. From this analysis the propane/ethane and propane/acetylene ratios are shown to preserve their emission ratios during regional transport. However systematic differences in the propane vs. acetylene/CO relationships are found between the model and observation values. This analysis suggests that further efforts are needed to improve the estimates of biomass burning emissions in SE Asia. The results presented in this paper also suggest ways to further extend the capabilities to derive observation-based inventories.     

High-resolution simulation of volcanic sulfur dioxide dispersion over the Miyake Island

After severe eruptions of the volcano at Miyake Island in August 2000, a large amount of volcanic gas was released into the atmosphere. To simulate flows and dispersion of sulfur dioxide (SO₂) over Miyake Island, a set of numerical models was developed. The multi-nesting method was adopted to reflect a realistic meteorological field and to sufficiently resolve the flow over the island with a diameter of 8 km. The outermost model was the Regional Spectral Model (RSM) of the Japan Meteorological Agency (JMA) with a horizontal grid size of 10 km. Finer atmospheric structure was simulated with the nonhydrostatic model jointly developed by the Meteorological Research Institute and the Numerical Prediction Division of JMA (MRI/NPD-NHM) with grid intervals of 2 km, 400 m and 100 m. Realistic topography of the island was represented in the innermost model. The Lagrangian particle method was applied to the dispersion model, which is driven by the meteorological field of the 100 m grid MRI/NPD-NHM. The random walk procedure was used to represent the turbulent diffusion. The model was verified in four cases. Simulated SO₂ concentrations agreed well with observed concentrations at a monitoring station including temporal variation. Under a large synoptic change, however, accurate prediction became difficult. Further numerical experiments have been done to investigate characteristics of the flow and the distribution of SO₂. Steady inflows, classified according to the surface wind speed and direction, were assumed. Simulated SO₂ distribution on the ground apparently depends on the surface wind. Under relatively weak inflow, there is a large diurnal change in SO₂ distribution, affected by the thermally induced flow. SO₂ gas is widely spread downstream in the nighttime but hardly reaches the coastal area in the daytime. On the other hand, SO₂ gas steadily reached the downstream coast with little diurnal variation under the stronger inflow. Ground temperature, as well as the static stability of the inflow, also influences downstream wind, turbulent diffusivity and SO₂ distribution.     

The Danish eulerian hemispheric model — a three-dimensional air pollution model used for the arctic

A three-dimensional Eulerian hemispheric air pollution model, the Danish Eulerian Hemispheric Model (DEHM), is in development at the National Environmental Research Institute (NERI). The model has been used to study long-range transport of air pollution in the Northern Hemisphere. The present version of the model includes long-range transport of sulphur dioxide (SO₂) and particulate sulphate (SC₄²⁻. The chemistry in the model is described by a simple linear oxidation of SO₂ to SO₄²⁻, and the wet deposition of SO₂ and SO₄⁻ is estimated based on the amount of precipitation, which is calculated from the contents of liquid cloud water (see Christensen, Air Pollution Modelling and its Applicatioons, Vol. X, pp. 119–127, Vol. XI, pp. 249–256, Plenum press, New York; 1995, Ph.D. thesis, National Environmental Research Institute, Denmark). The model has been used to study the air pollution in the Arctic. Results from yr simulation with an analysis of the results is presented: the model results are verified by comparisons, to measurements not only from the Arctic region but also from Europe and Canada. Some examples of episodes in the Arctic including analysis of the meteorological conditions during the episodes are presented. Finally, the model has been used to estimate the contribution from the different source regions on the northern hemisphere to the Arctic sulphur pollution.     

In situ measurement of isoprene in the marine air and surface seawater from the western North Pacific

Isoprene (2-methyl-1,3-butadiene) was measured on board of R/V Mirai for eight air samples and 14 seawater samples collected in the western North Pacific during ACE-Asia campaign (from 18 to 26 May 2001). The measurements were conducted in situ using a cryo-focus/gas chromatography/mass spectrometry (Cryo/GC/MS). Concentrations of isoprene ranged from 7.2 to 110 parts-per-trillion (pptv) in the marine air, and ranged from below 12 to 94 pmol l⁻¹ in the seawater. Based on these results, sea-to-air fluxes of isoprene were calculated to be 184 and 300 nmol m⁻² day⁻¹ for two samples, and the upper limits of the fluxes were also calculated to be from 32 to 300 nmol m⁻² day⁻¹. Atmospheric isoprene concentrations cannot be explained only by the flux from the seawater. Thus, the concentrations of isoprene in the marine air in western North Pacific should be significantly affected by terrestrial vegetational emission and subsequent long-range atmospheric transport of isoprene.     

The growth response of Alternanthera philoxeroides in a simulated post-combustion emission with ultrahigh [CO2] and acidic pollutants

Although post-combustion emissions from power plants are a major source of air pollution, they contain excess CO₂ that could be used to fertilize commercial greenhouses and stimulate plant growth. We addressed the combined effects of ultrahigh [CO₂] and acidic pollutants in flue gas on the growth of Alternanthera philoxeroides. When acidic pollutants were excluded, the biomass yield of A. philoxeroides saturated near 2000 μmol mol⁻¹ [CO₂] with doubled biomass accumulation relative to the ambient control. The growth enhancement was maintained at 5000 μmol mol⁻¹ [CO₂], but declined when [CO₂] rose above 1%, in association with a strong photosynthetic inhibition. Although acidic components (SO₂ and NO₂) significantly offset the CO₂ enhancement, the aboveground yield increased considerably when the concentration of pollutants was moderate (200 times dilution). Our results indicate that using excess CO₂ from the power plant emissions to optimize growth in commercial green house could be viable.     

钛基IrO2-SnO2电极在烟气海水脱硫恢复系统中的应用

采用浸渍-热分解法制备了含IrOx-TiO2中间层的IrO2-SnO2电极,得到的电极具有较高的析氯电催化活性和较强的稳定性,并通过电化学氧化法对Na2SO3海水脱硫模拟液进行处理,考察了电流密度、温度、pH值和电解时间等电解工艺参数对Na2SO3去除率和化学需氧量COD的影响.结果表明,在电流密度为200 mA/cm...     

Satellite derived trends in NO2 over the major global hotspot regions during the past decade and their inter-comparison

We assessed satellite derived tropospheric NO₂ distribution on a global scale and identified the major NO₂ hotspot regions. Combined GOME and SCIAMACHY measurements for the period 1996-2006 have been used to compute the trends over these regions. Our analysis shows that tropospheric NO₂ column amounts have increased over the newly and rapidly developing regions like China (11 ± 2.6%/year), south Asia (1.76 ± 1.1%/year), Middle East (2.3 ± 1%/year) and South Africa (2.4 ± 2.2%/year). Tropospheric NO₂ column amounts show some decrease over the eastern US (−2 ± 1.5%/year) and Europe (0.9 ± 2.1%/year). We found that although tropospheric NO₂ column amounts decreased over the major developed regions in the past decade, the present tropospheric NO₂ column amounts over these regions are still significantly higher than those observed over newly and rapidly developing regions (except China). Tropospheric NO₂ column amounts show some decrease over South America and Central Africa, which are major biomass burning regions in the Southern Hemisphere.     

Observation and origin of organochlorine compounds and polycyclic aromatic hydrocarbons in the free troposphere over central Europe

On Zugspitze (2670 m a.s.l.), Alps, higher concentrations were observed during a winter than during a summer measurement campaign of PAHs, chlorobenzenes (43.6 vs. 2.0 pg m⁻³) and DDTs (3.7 vs. 1.2 pg m⁻³), while hexachlorocyclohexanes and PCBs were found at similar levels. The PCB, HCH and DDT levels are among the lowest ever reported from outside the Arctic. Mostly lower levels were found in samples collected in summer than in winter despite a significant boundary layer air influence, but no such influence on samples collected during the winter campaign. Boundary layer influence was quantified by Lagrangian particle dispersion model retroplume analyses. Photochemical lifetimes corresponding to k_OH < 1.5 × 10⁻¹² cm³ molec⁻¹ s⁻¹ are found for p,p′-DDT, k_OH < 0.75 × 10⁻¹² cm³ molec⁻¹ s⁻¹ for p,p′-DDE and k_OH < 1.0 × 10⁻¹² cm³ molec⁻¹ s⁻¹ for p,p′-DDD.     

ACF脱除SO2/NOx反应器数学模型的建立

在大量试验研究获得数据基础上,结合机理分析,考虑ACF同时脱除多种污染物的主要影响因素,运用气固催化反应动力学方法进行分析,采用"混合模型法"建立ACF反应器数学模型,并用MATLAB软件与实验数据相结合迭代求取了模型参数,求出了宏观反应速率方程,并将计算模拟值与实验值进行比对,发现模拟结果与实验结果基本吻合,证实了模型的可靠性.为ACF反应器从试验研究的成果放大到工业规模的应用奠定了基础.     

Fate of citalopram during water treatment with O3, ClO2, UV and Fenton oxidation

In the present study we investigate the fate of citalopram (CIT) at neutral pH using advanced water treatment technologies that include O₃, ClO₂ oxidation, UV irradiation and Fenton oxidation. The ozonation resulted in 80% reduction after 30 min treatment. Oxidation with ClO₂ removed >90% CIT at a dosage of 0.1 mg L⁻¹. During UV irradiation 85% reduction was achieved after 5 min, while Fenton with addition of 14 mg L⁻¹ (Fe²⁺) resulted in 90% reduction of CIT. During these treatment experiments transformation products (TPs) were formed from CIT, where five compounds were identified by using high resolution and tandem mass spectrometry. Among these desmethyl-citalopram and citalopram N-oxide have been previously identified as human metabolites, while three are novel and published here for the first time. The three TPs are a hydroxylated dimethylamino-side chain derivative, a butyrolactone derivative and a defluorinated derivative of CIT.     

Linking chemical elements in forest floor humus (Oh-horizon) in the Czech Republic to contamination sources

While terrestrial moss and other plants are frequently used for environmental mapping and monitoring projects, data on the regional geochemistry of humus are scarce. Humus, however, has a much larger life span than any plant material. It can be seen as the “environmental memory” of an area for at least the last 60-100 years. Here concentrations of 39 elements determined by ICP-MS and ICP AES, pH and ash content are presented for 259 samples of forest floor humus collected at an average sample density of 1 site/300 km² in the Czech Republic. The scale of anomalies linked to known contamination sources (e.g., lignite mining and burning, metallurgical industry, coal fired power plants, metal smelters) is documented and discussed versus natural processes influencing humus quality. Most maps indicate a local impact from individual contamination sources: often more detailed sampling than used here would be needed to differentiate between likely sources.     

离子液体R3NANR3的制备及其脱硫性能

以二元酸和短链叔胺为原料,合成了已二酸三乙胺盐离子液体———R3NANR3。对该离子液体进行SO2气体的循环吸收和解吸行为的研究。实验结果表明,R3NANR3离子液体能对SO2气体进行有效的化学吸收。该吸收过程分二步进行,以第一步吸收为主。室温下(20℃)该离子液体在3 h以内吸收速率较快,3 h后吸收速率减慢并逐渐达到平衡。R3NANR3离子液体与SO2气体饱和吸收量的物质的量之比为1.08。较高温度将导致SO2气体的解吸,在90℃时饱和吸收液能较充分地解吸,残留量为0.0010 mol/L。多次吸收和解吸测试表明,R3NANR3离子液体能实现对SO2气体的循环吸收和分离,将成为烟气中SO2气体的脱除和利用的重要循环吸收剂。     

PM2.5 chemical source profiles for vehicle exhaust, vegetative burning, geological material, and coal burning in Northwestern Colorado during 1995

PM_2.5 (particles with aerodynamic diameters less than 2.5 μm) chemical source profiles applicable to speciated emissions inventories and receptor model source apportionment are reported for geological material, motor vehicle exhaust, residential coal (RCC) and wood combustion (RWC), forest fires, geothermal hot springs; and coal-fired power generation units from northwestern Colorado during 1995. Fuels and combustion conditions are similar to those of other communities of the inland western US. Coal-fired power station profiles differed substantially between different units using similar coals, with the major difference being lack of selenium in emissions from the only unit that was equipped with a dry limestone sulfur dioxide (SO₂) scrubber. SO₂ abundances relative to fine particle mass emissions in power plant emissions were seven to nine times higher than hydrogen sulfide (H₂S) abundances from geothermal springs, and one to two orders of magnitude higher than SO₂ abundances in RCC emissions, implying that the SO₂ abundance is an important marker for primary particle contributions of non-aged coal-fired power station contributions. The sum of organic and elemental carbon ranged from 1% to 10% of fine particle mass in coal-fired power plant emissions, from 5% to 10% in geological material, >50% in forest fire emissions, >60% in RWC emissions, and >95% in RCC and vehicle exhaust emissions. Water-soluble potassium (K⁺) was most abundant in vegetative burning profiles. K⁺/K ratios ranged from 0.1 in geological material profiles to 0.9 in vegetative burning emissions, confirming previous observations that soluble potassium is a good marker for vegetative burning.     

Reductive transformation of 2,4-dichlorophenoxyacetic acid by nanoscale and microscale Fe3O4 particles

Reductive transformation of 2,4-dichlorophenoxyacetic acid (2,4-D) by nanoscale and microscale Fe₃O₄ was investigated and compared. Disappearance of the parent species and formation of reaction intermediates and products were kinetically analyzed. Results suggest that the transformation of 2,4-D followed a primary pathway of its complete reduction to phenol and a secondary pathway of sequential reductive hydrogenolysis to 2,4-dichlorophenol (2,4-DCP), chlorophenol (2-CP, 4-CP) and phenol. About 65% of 2,4-D with initial concentration of 50 μ M was transformed within 48 h in the presence of 300 mg L^?1 nanoscale Fe₃O₄, and the reaction rates increased with increasing dosage of nanoscale Fe₃O₄. The decomposition of 2,4-D proceeded rapidly at optimum pH 3.0. Chloride was identified as a reduction product for 2,4-D in the magnetite–water system. Reductive transformation of 2,4-D by microscale Fe₃O₄ was slower than that by nanoscale Fe₃O₄. The reactions apparently followed pseudo-first-order kinetics with respect to the 2,4-D transformation. The degradation rate of 2,4-D decreased with the increase of initial 2,4-D concentration. In addition, anions had a significant adverse impact on the degradation efficiency of 2,4-D.     

二氧化铅电极的制备、表征及其电催化性能研究

以电沉积法制备了Ti/PbO2和Ti/MnO2/PbO22种电极.采用SEM、XRD和XPS等分析方法表征了电极的形貌、元素组成及元素化学态,并以罗丹明B为目标有机物,考察了所制备电极的析氧极化曲线和电催化活性以及Ti/MnO2/PbO2电极的循环伏安曲线.研究结果表明,Ti/MnO2/PbO2电极的稳定性、使用寿命、析氧电位和电催化活性较Ti/PbO2电极都有所提高,并且罗丹明B在Ti/MnO2/PbO2电极上的反应主要发生在析氧反应区,且反应不可逆.     

SO2 inhalation causes synaptic injury in rat hippocampus via its derivatives in vivo

SO₂ remains a common air pollutant, almost half of the world’s population uses coal and biomass fuels for domestic energy. Limited evidence suggests that exposure to SO₂ may be associated with neurotoxicity and increased risk of hospitalization and mortality of many brain disorders. However, our understanding of the mechanisms by which SO₂ causes harmful insults on neurons remains elusive. To explore the molecular mechanism of SO₂-induced neurotoxic effects in hippocampal neurons, we evaluated the synaptic plasticity in rat hippocampus after exposure to SO₂ at various concentrations (3.5 and 7 mg m⁻³, 6 h d⁻¹, for 90 d) in vivo, and in primary cultured hippocampal neurons (DIV7 and DIV14) after the treatment of SO₂ derivatives in vitro. The results showed that SYP, PSD-95, NR-2B, p-ERK1/2 and p-CREB were consistently inhibited by SO₂/SO₂ derivatives in more mature hippocampal neurons in vivo and in vitro, while the effects were opposite in young hippocampal neurons. Our results indicated that in young neurons, SO₂ exposure produced neuronal insult is similar to ischemic injury; while in more mature neurons, SO₂ exposure induced synaptic dysfunctions might participate in cognitive impairment. The results implied that SO₂ inhalation could cause different neuronal injury during brain development, and suggested that the molecular mechanisms might be involved in the changes of synaptic plasticity.     

介质阻挡放电协同Ag/Al_2O_3对NO_x脱除的影响

为有效去除发电厂烟气中产生的NOx,利用介质阻挡放电(DBD)产生低温等离子体并结合催化剂Ag/Al2O3进行烟气脱硝实验,研究了在加入乙烯的条件下,平均负载量、催化温度和装置的布置方式对NOx脱除的影响。结果表明,随着负载的增多,NO脱除率呈现先增大后减小的趋势,5种负载量中最佳为1.76%;随着催化温度的升高,NO脱除率同样呈现先增大后减小的趋势,最佳的催化温度为150℃左右;3种不同布置方式对NO和NOx脱除有明显差别,单独催化剂在NO和NOx的脱除率都比较低;单独介质阻挡放电NO脱除率很高,但是NOx很却很低;而两者结合在NO和NOx都达到了很好的效果。     

Chemical compositions and radiative properties of dust and anthropogenic air masses study in Taipei Basin, Taiwan, during spring of 2004

Asia is one of the major sources of not only mineral dust but also anthropogenic aerosols. Continental air masses associated with the East Asian winter monsoon always contain high contents of mineral dust and anthropogenic species and transported southeastward to Taiwan, which have significant influences on global atmospheric radiation transfer directly by scattering and absorbing solar radiation in each spring. However, few measurements for the long-range transported aerosol and its optical properties were announced in this area, between the Western Pacific and the southeastern coast of Mainland China. The overall objective of this work is to quantify the optical characteristics of different aerosol types in the Eastern Asian. In order to achieve this objective, meteorological parameters, concentrations of PM₁₀ and its soluble species, and optical property of atmospheric scattering coefficients were measured continuously with 1 h time-resolved from 11 February to 7 April 2004 in Taipei Basin (25°00′N, 121°32′E). In this work, the dramatic changes of meteorological parameters such as temperature and winds were used to determine the influenced period of each air mass. Continental, strong continental, marine, and stagnant air masses defined by the back-trajectory analysis and local meteorology were further characterized as long-range transport pollution, dust, clean marine, and local pollution aerosols, respectively, according to the diagnostic ratios. The aerosol mass scattering efficiency of continental pollution, dust, clean marine, and local pollution aerosols were ranged from 1.3 to 1.6, 0.7 to 1.0, 1.4 and 1.4 to 2.3 m² g⁻¹, respectively. Overall, there are two distinct populations of aerosol mass scattering efficiencies, one for an aerosol chemical composition dominated by dust (<1.0 m² g⁻¹) and the other for an aerosol chemical composition dominated by anthropogenic pollutants (1.3–2.3 m² g⁻¹), which were similar to the previous measurements with high degree of temporal resolution.