WRF-Chem simulation of East Asian air quality: Sensitivity to temporal and vertical emissions distributions

This study develops fine temporal (seasonal, day-of-week, diurnal) and vertical allocations of anthropogenic emissions for the TRACE-P inventory and evaluates their impacts on the East Asian air quality prediction using WRF-Chem simulations in July 2001 at 30-km grid spacing against available surface measurements from EANET and NEMCC. For NO₂ and SO₂, the diurnal and vertical redistributions of emissions play essential roles, while the day-of-week variation is less important. When all incorporated, WRF-Chem best simulates observations of surface NO₂ and SO₂ concentrations, while using the default emissions produces the worst result. The sensitivity is especially large over major cities and industrial areas, where surface NO₂ and SO₂ concentrations are reduced by respectively 3–7 and 6–12 ppbv when using the scaled emissions. The incorporation of all the three redistributions of emissions simulates surface O₃ concentrations higher by 4–8 ppbv at night and 2–4 ppbv in daytime over broad areas of northern, eastern and central China. To this sensitivity, the diurnal redistribution contributes more than the other two.     

Characteristics of springtime profiles and sources of ozone in the low troposphere over northern Taiwan

To quantify the possible sources of the high ambient ozone concentration in the low troposphere over Taiwan, ozone sounding data from a two-year intensive field measurement program conducted in April and early May of 2004 and 2005 in northern Taiwan has been examined. We found that the vertical ozone distributions and occurrence of enhanced ozone in the lower troposphere (below 6 km) mainly resulted from (1)Type NE: the long-range transport of ozone controlled by the prevailing northeasterly winds below 2 km, (2)Type LO: the local photochemical ozone production process, and (3)Type SW: the strong southwest/westerly winds aloft (2–6 km). In the boundary layer (BL), where Asian continental outflow prevails, the average profile for type NE is characterized by a peak ozone concentration of nearly 65 ppb at about 1500 m altitude. For type LO, high ozone concentration with an average ozone concentration greater than 80 ppb was also found in the BL in the case of stagnant atmospheric and sunny weather conditions dominated. For type SW, significant ozone enhancement with average ozone concentration of 70–85 ppb was found at around 4 km altitude. It is about 10 ppb greater than that of the types NE and LO at the same troposphere layer owing to the contribution of the biomass burning over Indochina. Due to Taiwan's unique geographic location, the complex interaction of these ozone features in the BL and aloft, especially features associated with northeasterly and south/southwesterly winds, have resulted in complex characteristics of ozone distributions in the lower troposphere over northern Taiwan.     

Carbon dioxide and methane fluxes in the littoral zones of two lakes,east Antarctica

During the summertime of 2007/2008, carbon dioxide (CO₂) and methane (CH₄) fluxes across air–water interface were investigated in the littoral zones of Lake Mochou and Lake Tuanjie, east Antarctica, using a static chamber technique. The mean fluxes of CO₂ and CH₄ were ?70.8 mgCO₂ m^?2 h^?1 and 144.6 μgCH₄ m^?2 h^?1, respectively, in the littoral zone of Lake Mochou; The mean fluxes were ?36.9 mgCO₂ m^?2 h^?1 and 109.8 μgCH₄ m^?2 h^?1, respectively, in the littoral zone of Lake Tuanjie. Their fluxes showed large temporal and spatial dynamics. The CO₂ fluxes showed a significantly negative correlation with daily total radiation (DTR) and a weakly negative correlation with air temperature and water temperature, indicating that sunlight intensity controlled the magnitude of CO₂ fluxes from the open lakes. The CH₄ fluxes significantly correlated with local air temperature, water table and total dissolved solids (TDS), indicating that they were the predominant factors influencing CH₄ fluxes. Summertime CO₂ budgets in the littoral zones of Lake Mochou and Lake Tuanjie were estimated to be ?152.9 gCO₂ m^?2 and ?79.7 gCO₂ m^?2, respectively, and net CH₄ emissions were estimated to be 312.3 mgCH₄ m^?2 and 237.2 mgCH₄ m^?2, respectively. Our results show that shallow, open, alga-rich lakes might be strong summertime CO₂ absorbers and small CH₄ emitters during the open water in coastal Antarctica.     

Ambient TSP concentration and dustfall in major cities of China: Spatial distribution and temporal variability

Based on environmental monitoring data in 93 major cities and meteorological records at 398 weather stations in China from 1981 to 2007, total suspended particle (TSP) concentration, the intensity of dustfall, and sand and dust storm frequency (F_d) were analysed. During the past 27 years, the annual average TSP concentration (C_TSP) in 93 cities was 402 μg m^?3. Annual average C_TSP decreased from the north to the south and from inland to the coast areas with a peak value of 628.8 μg m^?3 in Lanzhou. In the 1980s, 1990s and 2000s, annual average C_TSP was 628.7, 319.2, and 250.1 μg m^?3, respectively. Annual average intensity of dustfall (I_d) was 240.5 t km^?2 a^?1, decreased from northern to southern China and from inland to the coast areas with the maximum value of 717.2 t km^?2 a^?1 in Baotou. In the 1980s, 1990s and 2000s, annual average I_d was 334.8, 220.9, 146 t km^?2 a^?1 respectively. Annual average I_d in the Loess Plateau region was commonly higher than 200 t km^?2 a^?1. The annual average F_d decreased from arid regions in northwestern China to humid areas in southeastern China with two sand and sand storm centers existing in Xinjiang Taklamakan Desert and western Inner Mongolia. The annual average F_d in the 1980s, 1990s, 2000s was 16, 8, 6 days respectively, decreased steadily from 18 days in 1981–5 days in 2007. Annual average I_d had a positive linear relation to annual average C_TSP (R² = 0.96). Annual average F_d had a positive relation with annual average C_TSP (R² = 0.97) as well as annual average I_d (R² = 0.94). TSP was the chief pollutant influencing Air Pollution Index (API) in northern China in spring and winter seasons. Sand and dust storm might be a major factor affecting the temporal variability and spatial distribution of TSP and dustfall in China.     

Prediction of the adsorption capability onto activated carbon of a large data set of chemicals by local lazy regression method

Accurate quantitative structure–property relationship (QSPR) models based on a large data set containing a total of 3483 organic compounds were developed to predict chemicals’ adsorption capability onto activated carbon in gas phrase. Both global multiple linear regression (MLR) method and local lazy regression (LLR) method were used to develop QSPR models. The results proved that LLR has prediction accuracy 10% higher than that of MLR model. By applying LLR method we can predict the test set (787 compounds) with Q²_ext of 0.900 and root mean square error (RMSE) of 0.129. The accurate model based on this large data set could be useful to predict adsorption property of new compounds since such model covers a highly diverse structural space.     

Isotopes as tracers of sources of lead and strontium in aerosols (TSP & PM2.5) in Beijing

Even after its being phased out in gasoline in the late 90s, lead (Pb) is still present at relatively high levels in the atmosphere of Beijing, China (0.10–0.18 μg m^?3). Its origin is subject to debate as several distinct sources may contribute to the observed pollution levels. This study proposes to constrain the origin(s) of Pb and strontium (Sr) in aerosols, by coupling both Pb and Sr isotope systematics. The characterisation of the main pollution sources (road traffic, smelters, metal refining plants, coal combustion, cement factories, and soil erosion) shows that they can unambiguously be discriminated by the multi-isotope approach (²⁰⁶Pb/²⁰⁴Pb and ⁸⁷Sr/⁸⁶Sr). The study of total suspended particulates (TSP) and fine particles (PM_2.5) from Beijing and its vicinity indicates that both size fractions are controlled by the same sources. Lead isotopes indicate that metal refining plants are the major source of atmospheric lead, followed by thermal power stations and other coal combustion processes. The role of this latter source is confirmed by the study of strontium isotopes. Occasionally, emissions from cement plants and/or input from soil alteration are isotopically detectable.     

Degradation kinetics of anthracene by ozone on mineral oxides

To further understand the role of substrates on the heterogeneous reactions of polycyclic aromatic hydrocarbons, the reactions of ozone with anthracene adsorbed on different mineral oxides (SiO₂, α-Al₂O₃ and α-Fe₂O₃) and on Teflon disc were investigated in dark at 20 °C. No reaction between ozone and anthracene on Teflon disc was observed when the ozone concentration was ～1.18 × 10¹⁴ molecules cm^?3. The reactions on mineral oxides exhibited pseudo-first-order kinetics for anthracene loss, and the pseudo-first-order rate constant (k_1,obs) displayed a Langmuir–Hinshelwood dependence on the gas-phase ozone concentration. The adsorption equilibrium constants for ozone (K_O3) on SiO₂-1, SiO₂-2, α-Al₂O₃ and α-Fe₂O₃ were (0.81 ± 0.26) × 10^?15 cm³, (2.83 ± 1.17) × 10^?15 cm³, (2.48 ± 0.77) × 10^?15 cm³ and (1.66 ± 0.45) × 10^?15 cm³, respectively; and the maximum pseudo-first-order rate constant (k_1,max) on these oxides were (0.385 ± 0.058) s^?1, (0.101 ± 0.0138) s^?1, (0.0676 ± 0.0086) s^?1 and (0.0457 ± 0.004) s^?1, respectively. Anthraquinone was identified as the main surface product of anthracene reacted with ozone. Comparison with previous research and the results obtained in this study suggest that the reactivity of anthracene with ozone and the lifetimes of anthracene adsorbed on mineral dust in the atmosphere are determined by the nature of the substrate.     

钢渣吸附处理苯酚废水的研究

采用恒温振荡的方法,考察了钢渣粒径、吸附温度、振荡速度、溶液pH值、溶液初始浓度对苯酚去除率的影响。结果表明,在粒径为120~180目、pH=4.0、苯酚溶液浓度在500 mg/L以内、苯酚/钢渣质量比为1∶1 000时吸附效果最好。钢渣对苯酚的吸附能较好地符合Langmuir和Freundlich吸附等温线,线性相关系数分别为0.9971和0.9916,吸附机理为表面吸附。     

基于响应曲面法优化烧结烟气脱硫灰改性工艺

采用BOX-Behnken的中心组合实验设计及响应面分析方法对半干法烧结烟气脱硫灰进行改性研究,得到脱硫灰转化率的预测模型。结果表明:通过该预测模型可以很好地描述脱硫灰的转化率与反应温度、反应时间和气固比等重要操作参数之间的关系,R2=0.9903。因素分析表明,反应温度对脱硫灰的转化率影响最大,同时反应温度和气固比的交互作用与反应温度和时间的交互作用对脱硫灰的转化率的影响作用相同。利用得到的改进预测模型可以计算脱硫灰的转化率。