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1.

Background, aim, and scope  

In literature, the environmental applications of green rust (GR) have mainly been pointed out through the reduction of inorganic contaminants and the reductive dechlorination of chlorinated organics. However, reactions involving GR for the oxidation and mineralization of organic pollutants remain very scantly described. In this study, the ability of three synthetic Fe(II)–Fe(III) green rusts, GR(CO32−), GR(SO42−), and GR(Cl), to promote Fenton-like reaction was examined by employing phenol as a model pollutant. Unlike the traditional Fenton’s reagent (dissolved Fe(II) + H2O2), where the pH values have to be lowered to less than 4, the proposed reaction can effectively oxidize the organic molecules at neutral pH and could avoid the initial acidification which may be costly and destructive for the in situ remediation of contaminated groundwater and soils. The green rust reactivity towards the oxidative transformation of phenol was thoroughly evaluated by performing a large kinetic study, chemical analyses, and spectroscopic investigations.  相似文献   

2.
Aherne J  Kelly-Quinn M  Farrell EP 《Ambio》2002,31(6):452-459
In 1997, as part of a national program to determine and map critical loads, a lake survey was carried out in the Republic of Ireland. In total 200 lakes were sampled, which represents approximately 3.3% of the total lake population. The majority of lakes were situated in remote, high-altitude, acid-sensitive areas along the coastal margins of the country. Lake chemistry was dominated by marine inputs. Approximately 50% of the lakes had DOC > 5 mg L-1 due to the presence of organic soils in a large proportion of the catchments. Nonmarine sulfate concentrations were at background levels (< 20 mu eq L-1) in 50% of the lakes. Exceedance of critical load was observed in 7% of the sampled lakes (13 lakes). However, there are uncertainties in the critical load calculations due to the interference of sea salts and organic acids; accurate estimation under such conditions requires long-term lake and deposition chemistry.  相似文献   

3.
Surface water concentrations of dissolved organic carbon ([DOC]) are changing throughout the northern hemisphere due to changes in climate, land use and acid deposition. However, the relative importance of these drivers is unclear. Here, we use the Integrated Catchments model for Carbon (INCA-C) to simulate long-term (1996–2008) streamwater [DOC] at the four Swedish integrated monitoring (IM) sites. These are unmanaged headwater catchments with old-growth forests and no major changes in land use. Daily, seasonal and long-term variations in streamwater [DOC] driven by runoff, seasonal temperature and atmospheric sulfate (SO4 2−) deposition were observed at all sites. Using INCA-C, it was possible to reproduce observed patterns of variability in streamwater [DOC] at the four IM sites. Runoff was found to be the main short-term control on [DOC]. Seasonal patterns in [DOC] were controlled primarily by soil temperature. Measured SO4 2− deposition explained some of the long-term [DOC] variability at all sites.  相似文献   

4.
Trace elements (n = 23) in Irish headwater lakes (n = 126) were investigated to determine their ambient concentrations, fractionation (total, dissolved, and non-labile), and geochemical controls. Lakes were generally located in remote upland, acid-sensitive regions along the coastal margins of the country. Total trace metal concentrations were low, within the range of natural pristine surface waters; however, some lakes (~20 %) had inorganic labile aluminum and manganese at levels potentially harmful to aquatic organisms. Redundancy analysis indicated that geochemical weathering was the dominant controlling factor for total metals, compared with acidity for dissolved metals. In addition, many metals were positively correlated with dissolved organic carbon indicating their affinity (or complexation) with humic substances (e.g., aluminum, iron, mercury, lead). However, a number of trace metals (e.g., aluminum, mercury, zinc) were correlated with anthropogenic acidic deposition (i.e., non-marine sulfate), suggesting atmospheric sources or elevated leaching owing to acidic deposition. As transboundary air pollution continues to decline, significant changes in the cycling of trace metals is anticipated.  相似文献   

5.
Environmental properties of organic matter contained halogen and sulfur were studied in sediments of bleached kraft pulp mill effluent (BKME) recipient lakes and 2 m3 outdoor enclosures (mesocosms). The BKME contributed to 1% (v/v) of the total water flow in the lake downstream of the pulp mill where the sediments contained 1.7 to 4 mg of tetrahydrofuran extractable organic halogen (EOX-Cl) and 0.6 to 0.8 mg of tetrahydrofuran extractable organic sulfur (EOS-S) g−1 of organic matter. Upstream sediment contained 0.03 mg of EOXCl and 0.7 mg of EOS-S g−1 of organic matter. EOX was a better indicator for the influence of BKME in the recipient sediment than EOS. The polarity of BKME contained EOX corresponded to log Kow of < 1, and that of the downstream sediment contained EOX to > 4.5. HP-SEC analysis of the molecular weight distribution (MWD) of the EOX showed a peak between 300 to 600 g mol−1 for the BKME and between 1000 to 2000 g mol−1 for the downstream sediment. The MWD of the BKME contained EOS peaked at 300 to 1000 g mol−1, and that of the downstream sediment contained EOS at 1000 to 5000 g mol−1. These results indicate that BKME contained organic halogen and sulfur undergo major structural transformations when incorporated into sediment. The biota-to-sediment accumulation factor (BSAF) of EOX from sediments formed downstream of the mill and in the mesocosms to the lipids ofLumbriculus variegatus was 0.4 to 0.7. This is of a similar order of magnitude to the BSAF reported for 2,3,7,8-tetrachlorodibenzop-dioxin and 2,3,7,8-tetrachlorodibenzofuran.  相似文献   

6.
Annual volume-weighted mean (VWM) concentrations in rainwater collected at La Castanya (LC, Montseny Mountains, NE Spain) were analysed from 1983 to 2000 to study the temporal trends in precipitation chemistry, and the causes behind the changes. A significant positive correlation was found between annual rainwater SO42− concentrations at LC and Spanish SO2 emissions (r=0.73, P=0.0008) both decreasing remarkably during this period. Rainwater alkalinity increased during the period, shifting from negative values at the beginning (VWM in the 5 initial years=−2.7 μeq l−1) to alkaline values in recent years (VWM in the 5 final years=18.0 μeq l−1). Stepwise regression analysis indicated that 88% of the variation of alkalinity could be accounted for by the variability of non-marine Ca2+ and non-marine SO42−, with a more prominent dependence on Ca2+.Rains of African provenance were highly enriched in alkalinity and Ca2+, but no significant increases in their occurrence were found for the study period. Because of the reported higher dust updraft in northern Africa during years of high North Atlantic Oscillation (NAO) index, we also explored the relationship between rainwater variables associated with an African provenance and NAO. Annual precipitation was inversely related to NAO (r=−0.61, P=0.007). The annual wet deposition of African dust-related elements showed no correlation with NAO, probably because wet deposition of these elements depends on two factors (precipitation and dust updraft) which have opposite behaviour with respect to NAO. We hypothesise that dry deposition of African dust during dry spells (not sampled in this study) might be higher during high NAO-index years.  相似文献   

7.
The effect of elemental carbon (EC) on global as well as regional climate forcing is potentially very important. However, the EC data for northeastern U.S. is sparse. Daily EC concentrations, [EC], and [SO4] were measured in the northeastern U.S. at a regionally representative rural site, Whiteface Mountain (WFM; 44.366°N, 73.903°W, 1.5 km amsl, above mean sea level), New York (NY), for 1997. The air mass origin was determined using 6-h backward in time air trajectories obtained from the Hybrid Single-Particle Lagrangian Integrated Trajectory Model (HYSPLIT 4). [EC] and [SO4] were highly variable and influenced by synoptic–scale meteorology (rainy vs dry periods). The maximum daily [EC] and [SO4] were 364 ± 55 and 28,800 ± 3000 ng m?3, respectively. [EC] and [SO4] also showed seasonal variations at WFM. Occurrences of high daily [EC] were mainly in spring months, while peak daily [SO4] concentrations occurred in summer months. This behavior of aerosols is due to the fact that the sources of EC and SO4 are not the same and also due to the enhanced photochemical activity during summer months that increased the production of SO4 from SO2. High [EC] and [SO4] values were associated with westerly air flow from the industrialized Midwestern U.S. Sector analysis using HYSPLIT 4 air trajectories showed that regions lying between the southwest and northwest of the WFM contributed 81% and 83% of the [EC] and [SO4], respectively. The monthly net direct radiative forcing for shortwave (SW) due to EC and SO4 aerosols at the top of the atmosphere (TOA) varied from ?0.05 to ?0.50 W m?2, with an annual average of ?0.20 ± 0.15 W m?2 that gives a net cooling effect. Average net radiative forcing at WFM for clear sky is lower than the global average radiative forcing reported by IPCC (Foster and Ramaswamy, 2007).  相似文献   

8.
Background, aim, and scope  The Arctic holds large stores of minerals, and extracted materials are provided to the world’s economy; in this sense, the Arctic issue associated with mining is not local but global. In a part of the Arctic region (the Kola Peninsula, 66–70° N and 28–41° E), metal levels are generally elevated in the lake sediment. There is a question as to what results in elevated metal levels—a natural process (naturally abundant minerals) or an anthropogenic process (mining and metallurgy). In terms of solving this question, Staroe lake located on the Kola Peninsula was researched as a case study. Materials and methods  The following parameters were determined in relation with Staroe lake: (1) the current quality of the lake’s water—each 1,000-ml sample was collected at a surface point and a deep point (near the bottom layer), and the collected samples were directly analyzed after filtration; (2) atmospheric bulk deposition—bulk deposition was collected using a set of three rainwater samplers near the lake. In addition, bulk deposition was collected in a background site (250 km to the southwest of the smelter complex) as a reference; and (3) sediment profile (plus principal component analysis)—lake-bottom sediment was collected by an open-gravimetric column sampler equipped with an automatic diaphragm. After collection, the sample columns were cut at a 1-cm interval for analysis. Eigenvalues and variances by factor were calculated from the correlation coefficients. Results  The obtained data show that (1) naturally poor elements (Cu, Ni, Si, and SO4 2−) dominantly influence the lake’s water quality; (2) they are transported from the anthropogenic sources to the study lake through the atmospheric pathway; (3) mainly the contents of Cu, Ni, Sr, and Ca have influenced the sediment quality since the 1950s, corresponding to the industrial movement; and (4) Cu, Ni, and Sr originate from an anthropogenic source (smelter), and Ca originates from both natural and anthropogenic sources. Discussion  As compared with the Russian standard (San Pin 2.1.980–00), the contents of NO3 (50.3 ± 0.1 mg l−1) and particulates (2.3 ± 0.2 mg l−1) exceeded the standard levels (0.7 mg l−1 NO3 and 45 mg l−1 particulates); Staroe lake may be slightly contaminated. However, the contamination factor (comparison with the background data) implies that Staroe lake is considerably contaminated. There is a strong possibility that fine overburden detritus (<0.1 mm diameter) may be transported from an open pit to the study lake by natural forces such as wind. Although it is difficult to suppose that one factor dominantly affects the sediment quality, it follows from a factor analysis that factors 1 and 2 account for about 70% of the total variance: Factor 1 is the most dominant, and factor 2 is the second most dominant in the variability of sediment quality. It is considered that Cu, Sr, and Ni in factor 1 originate from anthropogenic sources because they are poor in sediment rocks. Conclusions  The field survey conducted in Staroe lake can give the following answers to the key objectives: (1) The present water quality is affected by Cu, Ni, Si, and SO4 2− in light of the contamination factor, and these elements originate from anthropogenic sources (the smelter and the open pit) and are transported to the lake through the atmospheric pathway; (2) the sediment profile and statistic analysis show that the lake quality has been influenced by deposition of metals since the 1950s; and (3) Cu, Ni, Sr, and Ca have influenced the sediment quality in light of the most dominant factor—Cu, Ni, and Sr originate from an anthropogenic source, whereas Ca comes from both natural and anthropogenic sources. Recommendations and perspectives  The presented lake survey shows that the dispersion of human-related pollutants via the atmospheric pathway takes place in the Arctic region. If the current pollution continues without countermeasures, the high-latitude environment may lose its original characteristics; hence, this subject is important when considering how to implement a wide range of environmental protection measures in the Arctic.  相似文献   

9.
ABSTRACT

Fine particles in the atmosphere have elicited new national ambient air quality standards (NAAQS) because of their potential role in health effects and visibility-reducing haze. Since April 1997, Tennessee Valley Authority (TVA) has measured fine particles (PM2.5) in the Tennessee Valley region using prototype Federal Reference Method (FRM) samplers, and results indicate that the new NAAQS annual standard will be difficult to meet in this region. The composition of many of these fine particle samples has been determined using analytical methods for elements, soluble ions, and organic and elemental carbon. The results indicate that about one-third of the measured mass is SO4 -2, one-third is organic aerosol, and the remainder is other materials. The fraction of SO4 -2 is highest at rural sites and during summer conditions, with greater proportions of organic aerosol in urban areas throughout the year. Additional measurements of fine particle mass and composition have been made to obtain the short-term variability of fine mass as it pertains to human exposure. Measurements to account for semi-volatile constituents of fine mass (nitrates, semi-volatile organics) indicate that the FRM may significantly under-measure organic constituents. The potentially controllable anthropogenic fraction of organic aerosols is still largely unknown.  相似文献   

10.
Cloud water investigations have been performed at the highest elevation of Central Germany in 1997. Results of extensive trace element measurements are presented. Besides conductivity, pH, liquid water content and major ions the data set includes 49 minor and trace elements. Estimation of crustal enrichment factors (EFs) provides an indication of the anthropogenic contributions to the cloud water concentrations. The variation of cloud composition with time has been illustrated for two selected events with different air mass origins. The chemical composition of the cloud condensation nuclei on which the droplets grow mainly determines the cloud water chemistry. For a cloud event in June 1997 the concentrations of the crustally derived elements Si, Al, Fe, Ti, Ce, La and Nd follow each other closely. The fact that SO42−, NO3 and NH4+ are only moderately correlated with the particular pollutants with high enrichment factors such as Cd, Sb, Pb, Zn, Cu, As, Bi, Sn, Mo, Ni, Tl and V indicates that their source regions are more widespread. During an event in October 1997 the time trends for most minor and trace elements follow rather closely those for the major ions NH4+, SO42− and NO3. Back trajectories show that the transport from continental and marine European sources was the likely cause of the sample concentrations. EFs of trace elements in cloud water samples during the June and October event show a strong correlation with those obtained for urban particulate matter. Although both events are influenced by air masses of different origin, there is a good agreement between the EF signatures.  相似文献   

11.
本研究基于上向流曝气生物滤池污水处理系统,研究了该工艺不同气水比、不同水力停留时间、不同滤料高度层、反冲洗强度对污染物的处理效能的影响。结果表明,气水比为4∶1、水力停留时间2 h时,BAF出水中COD、NH+4-N和SS指标达到最佳;沿程污染物去除率随着滤料层高度的增加逐渐增大,当滤料高度大于1.6 m时趋于稳定,COD、NH+4-N和SS平均去除率分别达到80%、99%和80.3%。建议曝气生物滤池的反冲洗推荐程序为:先气冲(18 L/(m2·s)),单独气洗2~3 min;再气冲(18 L/(m2·s))加水冲(5 L/(m2·s)),联合反冲洗3~5 min;最后水冲(5 L/(m2·s)),漂洗5~8 min。  相似文献   

12.
Real-time chemical measurements have been made as part of a field study of air quality in the city and harbour of Cork, Ireland. The data relate to the year 2008, with particular attention paid to the period between May and August. Eight air quality parameters were measured: NO, O3, NO2, SO2, EC, OC, particulate SO42? and PM2.5. The data have been used in a novel way involving wind and temporal averaging, along with Principal Component Analysis (PCA) and Positive Matrix Factorisation (PMF) methodologies to extrapolate major source contributions for PM2.5. It is demonstrated that continuous monitoring of standard air quality parameters, such as NO, NO2, SO2, along with EC, OC and particulate SO42?, can be used to provide relevant, cost-effective initial estimates of source contributions to ambient PM2.5 levels. It is also shown that the benefit of including OC and particulate SO42? in the monitoring protocol is considerable. Three major source groups of ambient PM2.5 mass in Cork were identified and quantified using this combined monitoring and modelling approach; road transport (19%), domestic solid fuel burning (14%) and oil-fired domestic and industrial boilers, including power generation plants (31%).  相似文献   

13.
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.  相似文献   

14.
UASB处理硫酸盐有机废水的启动   总被引:1,自引:0,他引:1  
为了考察上流式厌氧污泥床反应器(UASB)处理含硫酸盐有机废水的特性,采用有效容积为10 L的UASB,研究了启动运行过程中COD和SO2-4降解情况、出水VFA和pH值、产气量及颗粒污泥比产甲烷活性(SMA)变化状况。结果表明,接种厌氧颗粒污泥,保持进水COD为1 500 mg/L,SO2-4浓度为100 mg/L,将HRT由24 h缩短至12 h以提高负荷,经历55 d成功启动了UASB反应器;当HRT为12 h,进水COD和SO2-4负荷为3.0 kg/(m3·d)和0.20 kg/(m3·d),COD和SO2-4的去除率分别达到80%和89%,出水VFA为3 mmol/L,产气量达9.5 L/d,颗粒污泥的SMA为86.4 mL/(g VSS·d)。  相似文献   

15.
The behavior of 20 PAH in the organic layers of a L mull, an Of mull and a mor was assessed by a combined approach of a soil profile study, and the analysis of particle-size separates. Increasing PAH concentrations with depth in the mor profile (L, 866 μg kg−3; Of, 2902 μg kg−1; Oh, 10489 ug kg−1) were assigned to selective enrichment during organic matter decomposition. PAH were further highly enriched within the finer separates. For the L horizons, significant positive correlations were established between the enrichment of individual PAH (as observed from the decomposition gradient between the >2-mm fraction and the < 0.05-mm fraction), and the KOW for each compound. The slope of the regression line, m, described the degree of differentiation between low- and high-molecular PAH during litter decomposition. Since m was greatest in the most biologically active humus type (L mull, 0.33) and smallest in the most inactive (mor, 0.20), microbial breakdown was assumed as the dominating process for this differentiation. The results also indicated that decomposition processes had already taken place in the L horizons, leading to morphological and chemical changes of organic matter, and to an enrichment of high molecular PAH.  相似文献   

16.
Size-resolved chemical compositions of non-refractory submicron aerosols were measured using a quadrupole Aerodyne aerosol mass spectrometer at a rural site near Guangzhou in the Pearl River Delta (PRD) of China in the summer of 2006. Two cases characterized as the outflows from the PRD urban region with plumes of high SO2 concentration were investigated. The evolution of sulfate size distributions was observed on a timescale of several hours. Namely mass concentrations of sulfate in the condensation mode (with vacuum aerodynamic diameters (Dva) < 300 nm) increased at a rate of about 0.17–0.37 ppbv h?1 during the daytime. This finding was consistent with the sulfuric acid production rates of about 0.17–0.3 ppbv h?1, as calculated from the observed gas-phase concentrations of OH (~3.3 × 106–1.7 × 107 cm?3) and SO2 (~3–21.2 ppbv). This implies that the growth of sulfate in the condensation mode was mainly due to gas-phase oxidation of SO2. The observed rapid increase was caused mainly by the concurrent high concentrations of OH and SO2 in the air mass. The evolution of the mass size distributions of m/z 44, a tracer for oxygenated organic aerosol (OOA), was very similar to that of sulfate. The mass loadings of m/z 44 were strongly correlated with those of sulfate (r2 = 0.99) in the condensation mode, indicating that OOA might also be formed by the gas-phase oxidation of volatile organic compound (VOC) precursors. It is likely that sulfate and OOA were internally mixed throughout the whole size range in the air mass.  相似文献   

17.

Purpose  

Increases in dissolved organic carbon (DOC) concentrations have been reported in surface waters worldwide in the last 10 to 20 years. The causes behind these increases have been attributed to many factors, including climate change and decreasing depositions of atmospheric sulphate ( \textSO42 - {\text{SO}}_4^{{{2} - }} ). Trends in DOC concentrations and their potential causal factors were examined in a network of 30 lakes lying in undisturbed temperate and boreal catchments in the province of Quebec, Canada.  相似文献   

18.

Background, aim and scope  

Precipitation samples collected from 1995 to 2000 at meteorological station in the eastern outskirts of Herceg Novi (Montenegro) were analysed on Na+, K+, Mg2+, Ca2+, Cl, SO4 2–, NO3 and NH4 +. Four-day backward trajectory simulations were conducted during the precipitation period to investigate the regional transport of main ions and their deposition in the region of the southeastern Adriatic Sea. The air mass trajectories were classified into six trajectory categories by the origin and direction of their approach to Herceg Novi.  相似文献   

19.
Besides well-known episodic Kosa during spring, high concentrations of Ca2+ in aerosols were observed early in summer as well as in the semi-continuous data of the aerosols at the summit of Mt. Fuji. We further analysed the data to study the chemical characteristics of the high calcium event during early summer. The back trajectory analyses of the event indicated that Ca was transported from arid and semi-arid regions (e.g. the Taklamakan desert) through the westerly-dominated troposphere higher than the height of the summit of Fuji. The amount of SO42? was always equivalent to that of NH4+ unlike the case of the normal Kosa period where SO42? is in excess with respect to NH4+. This shows the ‘after’ mixing of unreacted CaCO3 of Kosa origin with (NH4)2SO4, which was only realized by the downward injection of Kosa particles from higher altitudes to the air masses of different origin. In the case of normal Kosa, the air bearing Kosa particles passed through the polluted area to absorb unneutralized acids (‘on-the-way’ mixing), whereas in the case of the Kosa-like phenomena in summer, the acids from the polluted area have been neutralized by NH4+ and become inactive before mixing with CaCO3 (“after” mixing). We have simplified the chemistry of aerosols using their three major components, Ca2+, SO42? and NH4+, and introduced a new triangle diagram with the three assumed end-members of CaCO3, CaSO4 and (NH4)2SO4 to quantify the contribution of the ‘after’ mixing to the aerosols (AMI; ‘after’ mixing index). Based on the back trajectories of some high AMI cases, CaCO3 in Kosa particles was transported through the middle troposphere (5000–7000 m) and descended to meet another air mass where SO42? had been already neutralized by NH3.  相似文献   

20.
Abstract

Twenty-five MiniVol samplers were operated throughout the Mexico City metropolitan region from February 22 through March 22, 1997, to evaluate the variability of PM10 concentrations and composition. The highest PM10 concentrations were found in neighborhoods with unpaved or dirty roads, and elements related to crustal material were the main cause of differences from nearby (<200 m) monitors that were not adjacent to the roadbed. SO4 2?concentrations were homogeneous across the city. SO4 2?measured at the city boundaries was about two-thirds of the concentrations measured within the urbanized area, indicating that most SO4 2? is of regional origin. Elemental carbon (EC) and organic carbon (OC) concentrations were highly variable, with higher concentrations in areas that had high diesel traffic and older vehicles. Spatial correlations among PM10 concentrations were high, even though absolute concentrations were variable, indicating a common effect of meteorology on the concentration or dispersion of local emissions.  相似文献   

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