气溶胶质谱仪在研究有机气溶胶环境微界面过程中的应用

有机气溶胶非均相和多相反应是复杂的微界面过程,它涉及气体的吸附、扩散、反应和解吸,传统的化学分析仪器不能提供完整实时的微界面过程的化学反应信息.气溶胶质谱仪是近年来发展起来用于实时分析颗粒物化学组分的重要仪器,它弥补了传统化学分析仪器,如GC/MS在实时分析上的不足,为研究有机气溶胶非均相化学反应的微界面过程提供了新的方法.本文旨在介绍气溶胶质谱仪的结构及其在研究有机气溶胶环境微界面过程中的应用.     

Analysis of diffusion-adsorption equivalency of landfill liner systems for organic contaminants

The equivalence between multilayered barriers regarding diffusion and adsorption is analyzed by means of an analytical method. The bottom boundary of the liner system is defined by assuming concentration continuous and flux continuous conditions of the contaminant between the bottom liner layer and the underlying soil. Five different liner systems were compared in terms of solute breakthrough time. The results of the analysis show that breakthrough time of the hydrophobic organic compounds for a 2-meter-thick compacted clay liner (CCL) can be 3-4 orders of magnitude greater than the breakthrough time for a geosynthetic clay liner (GCL) composite liner. The GM/GCL and GM/CCL composite liner systems provide a better diffusion barrier for the hydrophilic organic compounds than that for the hydrophobic compounds due to their different Henry's coefficient. The calculated breakthrough times of the organic contaminants for the Chinese standard liner systems were found to be generally greater than those for the GCL alternatives, for the specific conditions examined. If the distribution coefficient increases to 2.8 for the hydrophobic compounds or 1.0 for the hydrophilic compounds, the thickness of the attenuation layer needed to achieve the same breakthrough time as the standard liner systems can be reduced by a factor of about 1.9-2.4. As far as diffusive and adsorption contaminant transport are concerned, GM or GCL is less effective than CCL.     

Combined fluorescence and electrochemical investigation on the binding interaction between organic acid and human serum albumin

Human serum albumin (HSA) is a plasma protein responsible for the binding and transport of fatty acids and a variety of exogenous chemicals such as drugs and environmental pollutants. Such binding plays a crucial role in determining the ADME (absorption, distribution, metabolism, and excretion) and bioavailability of the pollutants. We report investigation on the binding interaction between HSA and acetic acid (C2), octanoic acid (C8) and dodecanoic acid (C12) by the combination of site-specific fluorescent probe, tryptophan intrinsic fluorescence and tyrosine electrochemistry. Two fluorescent probes, dansylamide and dansyl-L-proline, were employed in the displacement measurement to study fatty acid interaction with the two drug-binding sites on HSA. Intrinsic fluorescence of tryptophan in HSA was monitored upon addition of the fatty acids into HSA. Electrocatalyzed response of the tyrosine residues in HSA by a redox mediator was used to investigate the binding interaction. Qualitatively, observations made by the three approaches are very similar. HSA did not show any change in either fluorescence or electrochemistry after mixing with C2, suggesting there is no significant interaction with the short-chain fatty acid. For C8, the measured signal dropped in a single-exponential fashion, indicative of independent and non-cooperative binding. The calculated association constant and binding ratio is 3.1×106 L/mol and 1 with drug binding Site I, 1.1×107 L/mol and 1 with Site II, and 7.0×104 L/mol and 4 with the tryptophan site. The measurement with C12 displayed multiple phases of fluorescence change, suggesting cooperativity and allosteric effect of C12 binding. These results correlate well with those obtained by the established methods, and validate the new approach as a viable tool to study the interactions of environmental pollutants with biological molecules.     

Effectiveness of fluidized pellet bed for removing soluble contaminants

Fluidized pellet bed (FPB) has been successfully applied in water and wastewater treatment. However, the removal mechanism of contaminants especially the soluble ones, is still unclear. This study aimed to evaluate the e ectiveness of FPB reactor for removing soluble contaminants from synthetic wastewater. By only coagulation through jar test operation with addition of polyaluminium chloride (PACl) as primary coagulant and polyacryamide (PAM) as coagulant-aid, the removals of soluble chemical oxygen demand (COD), total phosphorus (TP), and NH4 +-N were found to be only 2.2%–7.5%, 5.7%–25.5%, and 9.9%–18.5%, respectively. However, by FPB operation under the same dosage of coagulants, these values increased to 82.7%, 37.2%, and 50%, indicating that the formation of pellets in the FPB e ectively enhanced the removal of soluble contaminants. By careful comparison of the settleablility and filterability of the pollutants after coagulation, the originally soluble contaminants could be divided into three groups, namely: (1) coagulated-andsettleable, (2) coagulated-but-nonsettleable, and (3) uncoagulable. It was found that not only the first two groups but also a large part of the third group could be e ectively removed by FPB operation. However, the mechanism for the removal of the uncoagulable pollutants by FPB operation still needs further investigation.     

Partitioning of water soluble organic carbon in three sediment size fractions： Effect of the humic substances

Water soluble organic carbon (WSOC) in sediments plays an important role in transference and transformation of aquatic pollutants. This article investigated the inherent mechanisms of how sediemnt grain size affect the partitioning coeffcient (k) of WSOC. Influences of NaOH extracted humic substances were particularly focused on. Sediments were sampled from two cross-sections of the middle Yellow River and sieved into three size fractions (< 63 μm, 63-100 μm, and 100--300 μm). The total concentration of WSOC in sediments (CWSOC) and k were estimated using multiple water-sediment ratio experiments. Results show that CWSOC ranges from 0.012 to 0.022 mg/g, while k ranges from 0.8 to 3.9 L/kg. Correlations between the spectrum characteristics of NaOH extracted humic substances and k were analyzed. Strong positive correlations are determined between k and the aromaticity indicators of NaOH extracted humic substances in different sediment size fractions. Comparing with finer fractions (< 63 μm), k is higher in larger size fractions (63--100 and 100--300 μm) related to higher aromaticity degree of NaOH extracted humic substances mostly. While negative relationship between k and the area ratio of fourier transform infrared spectroscopy (FT-IR) at 3400 and 1430 cm-1 implied that the lowest k was related to the highest concentration of the acidic humic groups in particles < 63 μm. WSOC in finer fractions (< 63 μm) is likely to enter into pore water, which may further accelerate the transportation of aquatic contaminants from sediment to water.     

Characterization of organic matter in total suspended particles by thermodesorption and pyrolysis-gas chromatography-mass spectrometry

The organic matter in tropospheric aerosol plays an important role in atmospheric physical and chemical processes. The bulk of organic matter, representing a significant proportion of the total suspended particulate (TSP) mass, is bound to polymeric material whose structure and properties are largely unknown. Here we used thermodesorption gas chromatography/mass spectrometry (Td- GC/MS) to study organic compounds of low molecular mass and pyrolysis gas chromatography/mass spectrometry (Py-GC/MS) to characterize the chemical structure of macromolecules in TSP samples collected in di erent seasons from di erent sites in Guangzhou. n-Alkanes, fatty acids and nitriles were the predominant compounds in the thermodesorption products, whereas aromatics, fatty acids, nitriles and n-alkanes/alkenes were the major compounds in the pyrolysates. The results indicated that aromatics were main units in macromolecules. The fatty acids and nitriles formed from carboxylic ammonium salts were detected in both thermodesorption products and pyrolysates at a certain concentration, indicating the importance of these compounds in TSP formation. The TSP source mainly determined the occurrence of compounds in samples from urban, suburban and forest sites, whereas the TSP source and formation process maybe controlled the seasonal variation in compounds detected. High levels of nitriles in summer samples from suburban and forest sites coincide with the release of ammonium from the land and of fatty acids from vegetation at these sites.     

Evaluating the e ects of granular and membrane filtrations on chlorine demand in drinking water

In this study, chlorine decay experiments were conducted for the raw water from Nakdong River that is treated by Chilseo Water Treatment Plant (CWTP) situated in Haman, Korea as well as the e uents from sand and granular activated carbon (GAC) filters of CWTP and fitted using a chlorine decay model. The model estimated the fast and slow reacting nitrogenous as well as organic/inorganic compounds that were present in the water. It was found that the chlorine demand due to fast and slow reacting (FRA and SRA) organic/inorganic substances was not reduced significantly by sand as well as GAC filters. However, the treated e uents from those filters contained FRA and SRA that are less reactive and had small reaction rate constants. For the e uents from microfiltration, ultrafiltration, and nanofiltration the chlorine demand because FRA and SRA were further reduced but the reaction rate constants were larger compared to those of sand and GAC filter e uents. This has implications in the formation of disinfection by products (DBPs). If DBPs are assumed to form due to the interactions between chlorine and SRA, then it is possible that the DBP formation potential in the e uents from membrane filtrations could be higher than that in the e uents from granular media filters.     

Microbiological parameters and maturity degree during composting of Posidonia oceanica residues mixed with vegetable wastes in semi-arid pedo-climatic condition

The aim of this study was to characterize the biological stability and maturity degree of compost during a controlled pile-composting trial of mixed vegetable residues (VR) collected from markets of Tunis City with residues of Posidonia oceanica (PoR), collected from Tunis beaches. The accumulation in beaches (as well as their removal) constitutes a serious environmental problem in all Mediterranean countries particularly in Tunisia. Aerobic-thermophilic composting is the most reasonable way to profit highly-valuable content of organic matter in these wastes for agricultural purposes. The physical, chemical, and biological parameters were monitored during composting over 150 d. The most appropriate parameters were selected to establish the maturity degree. The main result of this research was the deduction of the following maturity criterion: (a) C/N ratio < 15; (b) NH₄⁺-N < 400 mg/kg; (c) CO₂-C < 2000 mg CO₂-C/kg; (d) dehydrogenase activity < 1 mg TPF/g dry matter; (e) germination index (GI) > 80%. These five parameters, considered jointly are indicative of a high maturity degree and thus of a high-quality organic amendment which employed in a rational way, may improve soil fertility and soil quality. The mature compost was relatively rich in N (13.0 g/kg), P (4.74 g/kg) and MgO (15.80 g/kg). Thus composting definitively constitutes the most optimal option to exploit these wastes.     

Runoff and dissolved organic carbon loss from a paired-watershed study of three adjacent agricultural Watersheds

Organic matter plays several important roles in the biogeochemistry of terrestrial and aquatic ecosystems including the mobilization and transport of nutrients and pollutants. Cropping, tillage practices and vegetative buffer strip installation affect losses of dissolved organic carbon (DOC). While many studies show reductions in pollutant export from agroecosystems where vegetative buffers have been implemented, buffer strips may be a source of DOC and contribute to surface water pollution. Using a paired-watershed approach, the objectives of this study were to determine the effect of grass and agroforestry buffers on runoff and DOC loss, compare runoff and DOC losses between the growing and fallow seasons, and investigate crop effects on runoff and DOC losses. The study design consisted of three small agricultural Watersheds in a no-till, maize-soybean rotation located in the claypan region of northeast Missouri, USA; one watershed was planted with grass buffer strips, one with agroforestry buffer strips, and one unaltered watershed served as the control. Runoff and DOC loss were measured during a six-year calibration period (1991–1997) prior to buffer installation and for a nine-year treatment period (1997–2006). The grass buffer strips significantly decreased runoff by 8.4% (p = 0.015) during the treatment period while the agroforestry buffer system exhibited no significant change in runoff (p = 0.207). Loss of DOC was not significantly affected by grass or agroforestry buffer installation (p = 0.535 and p = 0.246, respectively). Additionally, no significant difference in runoff or DOC loss was found between crops (maize and soybean) or between seasons (growing and fallow). Overall, this study indicates that grass buffer systems are effective at reducing runoff and that DOC contamination of surface waters is not exacerbated by either type of vegetative buffer strip.     

Simulated dynamics of carbon stocks driven by changes in land use, management and climate in a tropical moist ecosystem of Ghana

Sub-Saharan Africa is large and diverse with regions of food insecurity and high vulnerability to climate change. This project quantifies carbon stocks and fluxes in the humid forest zone of Ghana, as a part of an assessment in West Africa. The General Ensemble biogeochemical Modeling System (GEMS) was used to simulate the responses of natural and managed systems to projected scenarios of changes in climate, land use and cover, and nitrogen fertilization in the Assin district of Ghana. Model inputs included historical land use and cover data, historical climate records and projected climate changes, and national management inventories. Our results show that deforestation for crop production led to a loss of soil organic carbon (SOC) by 33% from 1900 to 2000. The results also show that the trend of carbon emissions from cropland in the 20th century will continue through the 21st century and will be increased under the projected warming and drying scenarios. Nitrogen (N) fertilization in agricultural systems could offset SOC loss by 6% with 30 kg N ha⁻¹ year⁻¹ and by 11% with 60 kg N ha⁻¹ year⁻¹. To increase N fertilizer input would be one of the vital adaptive measures to ensure food security and maintain agricultural sustainability through the 21st century.