区域大气环境中PM2．5／PM10空间分布研究

提出了一种利用移动监测技术研究区域大气环境中PM2.5／PM10空间分布的方法,并在2004年12月进行了宁波市全市域PM2.5／PM10空间分布的研究。数据显示：相同路径所代表的地区PM2.5和PM10具有很好的相关性,多数路径上PM2.5与PM10数据的相关系数平方在0．95以上,而不同路径上PM2.5与PM10的比值不同。文中给出了宁波市PM2.5／PM10污染的空间分布图,直观地显示出PM2.5／PM10污染的空间分布情况,突出了污染的重点点位和地区。     

Continuous measurement of peroxyacetyl nitrate (PAN) in suburban and remote areas of western China

Knowledge on atmospheric abundance of peroxyacetyl nitrate (PAN) is important in assessing the severity of photochemical pollution, and for understanding chemical transformation of reactive odd nitrogen and its impact on the budget of tropospheric ozone (O₃). In summer 2006, continuous measurements of PAN were made using an automatic GC–ECD analyzer with an on-line calibrator at a suburban site of Lanzhou (LZ) and a remote site of Mt. Waliguan (WLG) in western China, with concurrent measurements of O₃, total reactive nitrogen (NO_y) and carbon monoxide (CO). At LZ, several photochemical episodes were observed during the study, and the average mixing ratio of PAN (plus or minus standard deviation) was 0.76 (±0.89) ppbv with the maximum value of 9.13 ppbv, compared to an average value of 0.44 (±0.16) ppbv at remote WLG. The PAN mixing ratios in LZ exhibited strong diurnal variations with a maximum at noon, while enhanced concentrations of PAN were observed in the evening and a minimum in the afternoon at WLG. The daily O₃ and PAN concentration maxima showed a strong correlation (r² = 0.91) in LZ, with a regression slope (PAN/O₃) of 0.091 ppbv ppbv^?1. At WLG, six well-identified pollution plumes (lasting 2–8 h) were observed with elevated concentrations of PAN (and other trace gases), and analysis of backward particle release simulation shows that the high-PAN events at WLG were mostly associated with the transport of air masses that had passed over LZ.     

Measurement of gas-phase total peroxides at the summit of Mount Tai in China

Measurement of ambient gas-phase total peroxides was performed at the summit of Mount Tai (Mt. Tai, 1534 m above sea level) in central-eastern China during March 22–April 24 and June 16–July 20, 2007. The hourly averaged concentration of peroxides was 0.17 ppbv (± 0.16 ppbv, maximum: 1.28 ppbv) and 0.55 ppbv (± 0.67 ppbv, maximum: 3.55 ppbv) in the spring and summer campaigns, respectively. The average concentration of peroxides at Mt. Tai, which is in a heavily polluted region, was much lower than hydrogen peroxide measurements made at some rural mountain sites, suggesting that significant removal processes took place in this region. An examination of diurnal variation and a correlation analysis suggest that these removal processes could include chemical suppression of peroxide production due to the scavenging of peroxy and hydroxy radicals by high NO_x, wet removal by clouds/fogs rich in dissolved sulfur dioxide which reacts quickly with peroxides, and photolysis. These sinks competed with photochemical sources of peroxides, resulting in different mean concentrations and diurnal pattern of peroxides in the spring and summer. A principal component analysis was conducted to quantify the major processes that influenced the variation of peroxide concentrations. This analysis shows that in the spring photochemical production was an important source of peroxides, and the major sink was scavenging during upslope transport of polluted and humid air from the lower part of the planetary boundary layer (PBL) and wet removal by synoptic scale clouds. During the summer, highly polluted PBL air (with high NO_x) was often associated with very low peroxides due to the chemical suppression of HO₂ by high NO_x and wet-removal by clouds/fogs in this sulfur-rich atmosphere, especially during the daytime. Higher concentrations of peroxides, which often appeared at mid-nighttime, were mainly associated with subsidence of air masses containing relatively lower concentrations of NO_y.     

Single particle mass spectrometry of oxalic acid in ambient aerosols in Shanghai: Mixing state and formation mechanism

Oxalic acid in individual aerosol particles was measured using single particle aerosol time-of-flight mass spectrometry (ATOFMS) in the summer of 2007 in Shanghai, China. Oxalate was found in 3.4% of total particles with diameters in the range of 0.2 – 2.0 μm. Size, chemical composition and hourly temporal counts of single particles that contained oxalic acid were measured. The predominant types of oxalate-containing particles were characterized to distinguish the primary and secondary sources of oxalic acid. Biomass burning was revealed as a major primary source of oxalic acid which contributed more than 20% of the oxalate-containing particles. Evidences for two different formation pathways of oxalic acid were observed in our experiment. The number fraction of oxalate-containing particles correlated with that of sulfate particles and the changes of air parcel backward trajectories, suggesting that in-cloud processing played important roles in oxalic acid formation. The diurnal patterns of dust and sea salt particle counts fitted well with the ambient relative humidity variation, suggesting that heterogeneous reactions occurring in hydrated/deliquesced aerosols also contributed to the production of oxalic acid.     

An important pathway for ozonolysis of alpha-pinene and beta-pinene in aqueous phase and its atmospheric implications

The aqueous ozonolysis of α-pinene and β-pinene was conducted under simulated tropospheric conditions at different pHs and temperatures. Three kinds of products, peroxides, carbonyl compounds, and organic acids, were well characterized, and the detection of these products provides effective evidence for understanding the atmospheric aqueous reaction pathway. We have two interesting findings: (1) the unexpected formation of methacrolein (MACR), with a yield of ～40%, in the α-pinene–O₃ aqueous reaction indicates a potentially new SOA formation pathway, because MACR is one of the important precursors of SOA; and (2) the surprisingly high yields of H₂O₂, ～60% for the α-pinene–O₃ reaction and ～100% for the β-pinene–O₃ reaction, indicates that H₂O₂ can be a significant contributor to the origin and transformation of oxidants in the atmosphere, especially in the humid regions. Moreover, we have determined the rate constant for aqueous reaction between MACR and H₂O₂ in pH 2 to 7 and obtained its upper limit as 0.13 M L^?1 s^?1. A mechanism concerning the formation of the species mentioned above is proposed, and it differs from that in the gas-phase reaction. We suggest that water plays a key role in the mechanism, by participating in the reactions as a direct reactant and by removing the excess energy of intermediates formed in the reactions.     

Structure and thermal stability of toxic chromium(VI) species doped onto TiO2 powders through heat treatment

Chromium(VI)-containing sorbents in the form of sludge or solid residue from treatment processes are often landfilled or used as fill materials, therefore the long-term stability of metal binding is important. The reduction of Cr(VI)–Cr(III) through heat treatment may be a useful detoxification method. After heating at 500, 900, 1000, and 1100 °C for 4 h, the transformation of chemical states of chromium on 105 °C-dried, 7.9% Cr(VI)-doped TiO₂ powders was studied on the basis of surface area measurements, scanning electron microscopy (SEM) images, X-ray diffraction (XRD), and extended X-ray absorption fine structure (EXAFS) spectra. It was shown that Cr(VI) was reduced to Cr(III) in the Cr(VI)-doped samples after heating within 500–900 °C. The present results also suggested that the chromium octahedral was bridged to the titanium tetrahedral and was incorporated in TiO₂ minerals formed after 1000 °C treatment.     

Landfill site selection using spatial information technologies and AHP: A case study in Beijing,China

Site selection is an important and necessary issue for waste management in fast-growing regions. Because of the complexity of waste management systems, the selection of the appropriate solid waste landfill site requires consideration of multiple alternative solutions and evaluation criteria. Based on actual conditions of the study area, we considered economic factors, calculated criteria weights using the analytical hierarchy process (AHP), and built a hierarchy model for solving the solid waste landfill site-selection problem in Beijing, China. A geographic information system (GIS) was used to manipulate and present spatial data. All maps are graded from 1 (lowest suitability) to 5 (highest suitability) using spatial information technologies. The candidate sites were determined by aggregation based on the criteria weights. The candidate sites are divided by ‘best’, ‘good’ and ‘unsuitable’ landfill areas. Best landfill areas represent optimal sites; good landfill areas can be used as back-up candidate sites. Our work offers a siting methodology and provides essential support for decision-makers in the assessment of waste management problems in Beijing and other rapidly developing cities in developing countries.     

Study on the hydrolysis/precipitation behavior of Keggin Al13 and Al30 polymers in polyaluminum solutions

The hydrolysis/precipitation behaviors of Al³⁺, Al₁₃ and Al₃₀ under conditions typical for flocculation in water treatment were investigated by studying the particulates' size development, charge characteristics, chemical species and speciation transformation of coagulant hydrolysis precipitates. The optimal pH conditions for hydrolysis precipitates formation for AlCl₃, PAC_Al13 and PAC_Al30 were 6.5–7.5, 8.5–9.5, and 7.5–9.5, respectively. The precipitates' formation rate increased with the increase in dosage, and the relative rates were AlCl₃ ? PAC_Al30 > PAC_Al13. The precipitates' size increased when the dosage increased from 50 μM to 200 μM, but it decreased when the dosage increased to 800 μM. The Zeta potential of coagulant hydrolysis precipitates decreased with the increase in pH for the three coagulants. The iso-electric points of the freshly formed precipitates for AlCl₃, PAC_Al13 and PAC_Al30 were 7.3, 9.6 and 9.2, respectively. The Zeta potentials of AlCl₃ hydrolysis precipitates were lower than those of PAC_Al13 and PAC_Al30 when pH > 5.0. The Zeta potential of PAC_Al30 hydrolysis precipitates was higher than that of PAC_Al13 at the acidic side, but lower at the alkaline side. The dosage had no obvious effect on the Zeta potential of hydrolysis precipitates under fixed pH conditions. The increase in Zeta potential with the increase in dosage under uncontrolled pH conditions was due to the pH depression caused by coagulant addition. Al–Ferron research indicated that the hydrolysis precipitates of AlCl₃ were composed of amorphous Al(OH)₃ precipitates, but those of PAC_Al13 and PAC_Al30 were composed of aggregates of Al₁₃ and Al₃₀, respectively. Al³⁺ was the most un-stable species in coagulants, and its hydrolysis was remarkably influenced by solution pH. Al₁₃ and Al₃₀ species were very stable, and solution pH and aging had little effect on the chemical species of their hydrolysis products. The research method involving coagulant hydrolysis precipitates based on Al–Ferron reaction kinetics was studied in detail. The Al species classification based on complex reaction kinetic of hydrolysis precipitates and Ferron reagent was different from that measured in a conventional coagulant assay using the Al–Ferron method. The chemical composition of Al_a, Al_b and Al_c depended on coagulant and solution pH. The Al_b measured in the current case was different from Keggin Al₁₃, and the high Al_b content in the AlCl₃ hydrolysis precipitates could not used as testimony that most of the Al³⁺ was converted to highly charged Al₁₃ species during AlCl₃ coagulation.     

Diversity of Soil Nematodes in Areas Polluted with Heavy Metals and Polycyclic Aromatic Hydrocarbons (PAHs) in Lanzhou,China

This study investigated the soil nematode community structure along the Yellow River in the Lanzhou area of China, and analyzed the impact of heavy metals (Cd, Pb, Cr, Cu, and Zn) and polycyclic aromatic hydrocarbons (PAHs) on the nematode community. Soil samples from five locations (named A–E), which were chosen for soil analysis, showed significant differences in their heavy metal content (p < 0.01), as well as in the variety of nematodes (up to 41 genera) and families (up to 20) that were present. The different samples also differed significantly in the total PAH content (p < 0.05), as well as the six types of PAH present. Sites A–C showed the most severe contamination with heavy metals and PAHs; these sites had the lowest abundance of fungivores and omnivore/predators, but the proportion of bacteriovores was the highest (p < 0.05). Site E, in contrast, showed only minor pollution with heavy metals and PAHs, and it contained the highest abundance of plant parasites (p < 0.05). Several nematode ecological indicators were found to correlate with concentration of soil pollutants at all the sites tested: the maturity index (MI, in addition to plant parasites), plant parasite index (PPI), ΣMI (including all the soil nematodes), Shannon-Wiener diversity index (H′′), and Wasilewska index (WI). Disturbance to the soil environment was more severe when MI, ΣMI, and H′ values were lower. The results of the study show that the abundance and structure of the soil nematode communities in the sampling locations were strongly influenced by levels of heavy metals and PAHs in the soil. They also show that the diversity index H′ and the maturity index can be valuable tools for assessing the impact of pollutants on nematodes.     

An Interval-Parameter Waste-Load-Allocation Model for River Water Quality Management Under Uncertainty

A simulation-based interval quadratic waste load allocation (IQWLA) model was developed for supporting river water quality management. A multi-segment simulation model was developed to generate water-quality transformation matrices and vectors under steady-state river flow conditions. The established matrices and vectors were then used to establish the water-quality constraints that were included in a water quality management model. Uncertainties associated with water quality parameters, cost functions, and environmental guidelines were described as intervals. The cost functions of wastewater treatment units were expressed in quadratic forms. A water-quality planning problem in the Changsha section of Xiangjiang River in China was used as a study case to demonstrate applicability of the proposed method. The study results demonstrated that IQWLA model could effectively communicate the interval-format uncertainties into optimization process, and generate inexact solutions that contain a spectrum of potential wastewater treatment options. Decision alternatives can be generated by adjusting different combinations of the decision variables within their solution intervals. The results are valuable for supporting local decision makers in generating cost-effective water quality management strategies.