Modelling photochemical oxidant formation, transport, deposition and exposure of terrestrial ecosystems

The chemical processes responsible for production of photochemical oxidants within the troposphere have been the subject of laboratory and field study throughout the last three decades. During the same period, models to simulate the atmospheric chemistry, transport and deposition of ozone (O(3)) from individual urban sources and from regions have been developed. The models differ greatly in the complexity of chemical schemes, in the underlying meteorology and in spatial and temporal resolution. Input information from land use, spatial and temporally disaggregated emission inventories and meteorology have all improved considerably in recent years and are not fully implemented in current models. The development of control strategies in both North America and Europe to close the gaps between current exceedances of environmental limits, guide values, critical levels or loads and full compliance with these limits provides the focus for policy makers and the support agencies for the research. The models represent the only method of testing a range of control options in advance of implementation. This paper describes currently applied models of photochemical oxidant production and transport at global and regional scales and their ability to simulate individual episodes as well as photochemical oxidant climatology. The success of current models in quantifying the exposure of terrestrial surfaces and the population to potentially damaging O(3) concentrations (and dose) is examined. The analysis shows the degree to which the underlying processes and their application within the models limit the quality of the model products.     

多环芳烃在黄河水体颗粒物上的表面吸附和分配作用特征

通过模拟实验研究了多环芳烃在黄河水体颗粒物上的吸附特征,重点探讨了表面吸附和分配作用对吸附的贡献,结果表明:①随着泥沙含量的增加,总吸附量在增加,而单位颗粒物的吸附量却在减少;且泥沙含量不同时,吸附等温式的拟合方程也不同;②颗粒物对多环芳烃的吸附等温线与吸附-分配复合模式拟合较好;表面吸附和分配作用对多环芳烃的吸附实验值与吸附-分配模式中的理论值比较吻合;③在实验浓度范围内,黄河颗粒物对多环芳烃的吸附以表面吸附为主,如当颗粒物含量为3、8和15g/L,液相平衡浓度分别为2.84、2.35和3.4μg/L时,表面吸附对总吸附的贡献分别为67.85%、65.6%和62.69%;且表面吸附对总吸附的贡献大小顺序可以用泥沙含量表示为:3g/L>8g/L>15g/L,即随着泥沙含量的增加,表面吸附的贡献有减小的趋势;④单一多环芳烃在颗粒物上的单位吸附量大于3种多环芳烃共存时的单位吸附量,这从另一角度证实多环芳烃在黄河水体颗粒物上的吸附以表面吸附为主.     

Life cycle assessment of active and passive groundwater remediation technologies

Groundwater remediation technologies, such as pump-and-treat (PTS) and funnel-and-gate systems (FGS), aim at reducing locally appearing contaminations. Therefore, these methodologies are basically evaluated with respect to their capability to yield local improvements of an environmental situation, commonly neglecting that their application is also associated with secondary impacts. Life cycle assessment (LCA) represents a widely accepted method of assessing the environmental aspects and potential impacts related to a product, process or service. This study presents the set-up of a LCA framework in order to compare the secondary impacts caused by two conceptually different technologies at the site of a former manufactured gas plant in the city of Karlsruhe, Germany. As a FGS is already operating at this site, a hypothetical PTS of the same functionality is adopted. During the LCA, the remediation systems are evaluated by focusing on the main technical elements and their significance with respect to resource depletion and potential adverse effects on ecological quality, as well as on human health. Seven impact categories are distinguished to address a broad spectrum of possible environmental loads. A main point of discussion is the reliability of technical assumptions and performance predictions for the future. It is obvious that a high uncertainty exists when estimating impact specific indicator values over operation times of decades. An uncertainty analysis is conducted to include the imprecision of the underlying emission and consumption data and a scenario analysis is utilised to contrast various possible technological variants. Though the results of the study are highly site-specific, a generalised relative evaluation of potential impacts and their main sources is the principle objective rather than a discussion of the calculated absolute impacts. A crucial finding that can be applied to any other site is the central role of steel, which particularly derogates the valuation of FGS due to the associated emissions that are harmful to human health. In view of that, environmental credits can be achieved by selecting a mineral-based wall instead of sheet piles for the funnel construction and by minimising the steel consumption for the gate construction. Granular activated carbon (GAC) is exclusively considered as the treatment material, both in-situ and on-site. Here it is identified as an additional main determinant of the relative assessment of the technologies since it is continuously consumed.     

Pesticides in the groundwater of a spring draining a sandy aquifer: temporal variability of concentrations and fluxes

A 250 ha agricultural catchment has been characterized with respect to its hydrogeology and groundwater contamination by pesticides from October 1999 to August 2004. Five years after the ending of atrazine (At) application, used since the sixties, At and deethylatrazine (DEA) are still systematically quantified at the outlet of the watershed with concentrations from 0.07 to 0.43 microg l(-1) for At, and between 0.14 and 1.16 microg l(-1) for DEA. Isoproturon and chlortoluron are detected in only one (0.3 microg l(-1)) and two (0.7 and 2.0 microg l(-1)) of the 124 semi-monthly samples, respectively. DEA concentrations can be very different between two samples with a 15-day time step. The annual mean exported fluxes of cumulated At and DEA are stable, which indicates a long time transfer in the unsaturated or saturated zone with a progressive leaching of the stock of At and DEA probably accumulated in the soil and the vadose zone. These fluxes, between 0.90% and 2.82% of the annual mean dose of At applied before 1999, similar to those calculated in several studies at the bottom of the root zone, could be explained by low adsorption and degradation properties of At and DEA in the unsaturated and saturated zone.     

Determination of biodegradation potential by two culture-independent methods in PAH-contaminated soils

Biodegradation potentials of polycyclic aromatic hydrocarbons (PAHs) were determined with soil samples collected from various depths of a PAH-contaminated site and of a site nearby where PAHs were not found. Putative dioxygenase genes were amplified by a primer set specific for initial dioxygenases and identified by web-based database homology search. They were further categorized into several groups of which four dioxygenases were selected as probes for DNA hybridization. The hybridization signals according to the presence of putative dioxygenases were positively related to the extent of PAH contamination. However, the signal intensities varied depending on the probes hybridized and moreover were not consistent with PAH biodegradation activities determined by CO2 evolution. Despite widely accepted advantages of molecular biodegradation assessment, our data clearly present the variations of assessment results depending on the genetic information used and suggest that the methodology may tend to underestimate the real biodegradation capacity of a site probably due to the limited dioxygenase database available at the moment. Therefore, the molecular assessment of biodegradation potential should involve a very careful primer and probe design and an extensive microbiological examination of a site of interest to accurately delineate the biodegradation potential of the site.     

Successful Treatment of Low PAH-Contaminated Sewage Sludge in Aerobic Bioreactors (7 pp) *

Background, Aims and Scope Polycyclic Aromatic Hydrocarbons (PAHs) are known for their adverse and cumulative effects at low concentration. In particular, the PAHs accumulate in sewage sludge during wastewater treatment, and may thereafter contaminate agricultural soils by spreading sludge on land. Therefore, sludge treatment processes constitute the unique opportunity of PAH removal before their release in the environment. In this study, the ability of aerobic microorganisms to degrade light and heavy PAHs was investigated in continuous bioreactors treating trace-level PAH-contaminated sludge. Methods Several aerobic reactors were operated under continuous and perfectly mixed conditions to simulate actual aerobic sludge digesters. Three sterile control reactors were performed at 35°C, 45°C or 55°C to assess PAH abiotic losses under mesophilic and thermophilic conditions. Three biological reactors were also operated at 35°C, 45°C or 55°C. Furthermore, 250 mM methanol were added in an additional mesophilic reactor (35°C). All reactors were fed with long-term PAH-contaminated sewage sludge, and PAH removal was assessed by inlet/outlet mass balance. In this study, PAH compounds ranged from 2 to 5-unsubstituted aromatic rings, i.e. respectively from Fluorene to Indeno(123cd)pyrene. Results and Discussion Significant abiotic losses were observed for the lightest PAHs (fluorene, phenanthrene and anthracene), while biodegradation occurred for all PAHs. More than 80% of the lightest PAHs were removed. Biodegradation rates inversely correlated with the increasing molecular weight, and seemed limited by the low bioavailability of the heaviest PAHs (only 50% of removal). The enhancement of PAH bioavailability by increasing the process temperature or adding methanol was tested. A temperature increase from 35°C to 45°C and then to 55°C significantly enhanced the biodegradation of the heaviest PAHs from 50% to 80%. However, high abiotic losses were observed for all PAHs at 55°C, which was attributed to volatilization. Optimal conditions were found at 45°C considering the low abiotic losses and the high PAH biodegradation rates. Similar performances were achieved by addition of methanol in the sludge. It was concluded that increasing temperatures or addition of methanol favored PAH diffusion from solids to an aqueous compartment, and enhanced their bioavailability to PAH-degrading microorganisms. Conclusion In this study, the use of long-term acclimated aerobic ecosystems showed the high potential of aerobic microorganisms to degrade a wide range of PAHs at trace levels. However, PAH biodegradation was likely controlled by their low bioavailability. Two aerobic processes have been finally proposed to achieve efficient decontamination of sewage sludge, at 45°C or in the presence of methanol. The PAH concentrations in reactor outlet were lower than the French requirements, and allow the treated sludge to be spread on agricultural land. Recommendations and Outlook The two proposed aerobic processes used physical or chemical diffusing agents. The global ecological impact of using the latter agents for treating trace level contamination must be considered. Since methanol was completely removed during the process, no additional harm is expected after treatment. However, an increase of temperature to 45°C could drastically increase the energy demand in full-scale plants, and therefore the ecological impact of the process. Moreover, since bioavailability controls PAH biodegradation, efficiency of the processes could also be influenced by the hydraulic parameters, such as mixing and aeration rates. Further experimentations in a pilot scale are therefore recommended, as well as a final assessment of the global environmental benefit of using such aerobic processes in the bioremediation of trace level compounds. - Abbreviations (PAHs): Ant – anthracene; B(a)A – benzo(a)anthracene ; B(b)F – benzo(b)fluoranthene; B(k)F – benzo(k)fluoranthene; B(ghi)P – benzo(g,h,i)perylene; B(a)P – benzo(a)pyrene; Chrys – chrysene; DB – dibenzo(a,h)anthracene; Fluor – fluoranthene; Fluo - fluorene; Ind – indeno(1,2,3-c,d)pyrene; Phe - phenanthrene; Pyr – pyrene - * The basis of this peer-reviewed paper is a presentation at the 9th FECS Conference on 'Chemistry and Environment', 29 August to 1 September 2004, Bordeaux, France.     

Trail discrimination signal of Lasius japonicus (Hymenoptera: Formicidae)

Summary. Trail-following behavior of Lasius japonicus was colony-specific in the field, while trail pheromone activity was not. We found that the footprint substance caused colony-specific trail-following behavior only when working in conjunction with the trail pheromone. The footprint substance alone did not lead the workers to follow trails. The substance consisted mainly of hydrocarbons with composition almost identical to that of cuticular hydrocarbons, except for the absence of n-alkanes. Nestmate workers shared footprint hydrocarbon profiles as well as cuticular hydrocarbons, but the profiles differed among colonies. We therefore consider that the footprint hydrocarbon profiles serve as the trail discrimination signal in L. japonicus.     

Shorter fries? An alternative policy to support a reduction of nitrogen contamination from agricultural crop production

Feeding the growing population of the world poses significant policy challenges for the sustainability of global ecosystems. A prime example is the degradation of water quality due to the growing imbalance in the terrestrial nitrogen (N) cycle linked to increasing production of reactive N (Nr). Environmental impacts such as groundwater quality degradation and eutrophication of coastal estuaries tend to be local in nature but may be closely connected to global economic factors. Environmental accounting of the N fluxes entering, leaving or remaining in Prince Edward Island (PEI), a small agricultural region, demonstrate the importance of a single industry (potato production) in controlling the local N cycle. The resulting burden of Nr has its most profound effect on groundwater, the sole source of drinking water and the primary pathway of N to the Province's economically and ecologically important estuaries. At the same time, agriculture is a vital part of the local economy, and regulators are faced with the challenge of meeting environmental goals and still maintaining an industry that is competitive and responsive to global market trends. New, innovative policy alternatives are needed to foster more effective implementation of sustainable agricultural practices. An approach that focuses on influencing consumer choices toward more environmentally responsible production practices at the point of origin may help remove some of the important, non-technical barriers to sustainable food production practices. In practice, a system that documents the environmental performance throughout the full supply chain from producer to retailer would have to be implemented.     

On the influence of chemical initial and boundary conditions on annual regional air quality model simulations for North America

The influence of chemical initial conditions and chemical lateral boundary conditions (CLBCs) on long-term regional air quality model simulations was investigated using outputs from an annual simulation of the year 2002 on a North American domain. This simulation was carried out using the AURAMS regional air quality model. It was subdivided into three multi-month segments with two overlap periods (May 15–30 and September 1–30) to allow the segments to be run in parallel. For this approach to work, model predictions had to match very closely by the end of the two-week and four-week overlap periods. The time required for the values of daily domain-average surface PM_2.5 concentration to match for the two simulation segments associated with each of the two overlap periods was four and six days, respectively. For individual locations within the model domain, however, the required spin-up period was as much as nine days, considerably longer than the 2–4-day spin-up period usually assumed in the literature. For ozone, on the other hand, the daily domain-average surface ozone concentration values did not converge for either overlap period. A zero-gradient CLBC had been used for all run segments and species. When a time-invariant CLBC for ozone was used instead, the daily domain-average surface ozone concentration values behaved more realistically and did converge after fewer than three days. A similar improvement was also obtained for individual locations, but with spin-up periods of up to nine days. Model chemical spin-up time thus seems to be dependent on the species considered, the time required for the influence of the inflow boundaries to reach all locations within the domain, and the impact of local emissions sources. These results suggest the use of a spin-up period of longer than one week for a large (continental) domain and long-term simulation of PM_2.5 and O₃ rather than the 2–4 days commonly assumed in the literature.     

根据具体情况优化EPA8310中色谱分离条件

运用Agilent（安捷伦）1200系列高效液相色谱和多环芳烃专用柱ZORBAX Eclipse PAH（4.6×250mm、5μm,P.N.959990-918,S.N.USPAB01066）,对16种多环芳烃化合物混合溶液进行分析,根据具体实验条件优化EPA8310中色谱分离条件并得到了更节省时间、分离效率更好的流动相梯度变化程序。