水处理氧化还原过程的电动化学特性

以流动电流为参数,研究了水处理条件下氧化还原过程的电动化学特性.考察了水中KMnO_4及其与Mn~(2+),Fe~(2+)之间氧化还原作用的流动电流(SC)规律,探讨了氧化还原的初始条件、水处理环境、原水水质、氧化剂与还原剂的投加方式等对流动电流的影响.结果表明,水中约0.5mg·l~(-1)的KMnO_4可产生SC的峰值,而且当它与Mn~(2+)和Fe~(2+)经不同条件进行氧化还原作用时,可通过SC值的变化表现出更为明显的电动化学特性.     

Natural pollution caused by the extremely acidic crater lake Kawah Ijen, East Java, Indonesia

Background. Aims and Scope Lakes developing in volcano craters can become highly acidic through the influx of volcanic gases, yielding one of the chemically most extreme natural environments on earth. The Kawah Ijen crater lake in East Java (Indonesia) has a pH 〈 0.3. It is the source of the extremely acid and metal-polluted river Banyupahit (45 km). The lake has a significant impact on the river ecosystem as well as on a densely populated area downstream, where agricultural fields are irrigated with water with a pH between 2.5 and 3.5. The chemistry of the river water seemed to have changed over the past decade and the negative effect in the irrigation area increased. A multidisciplinary approach was used to investigate the altered situation and to get insight in the water chemistry and the hydrological processes influencing these alterations. Moreover, a first investigation of the effects of the low pH on ecosystem health and human health was performed. Methods Water samples were taken at different sites along the river and in the irrigation area. Sampling for macroinvertebrates was performed at the same sites. Samples of soil and crop were taken in the irrigation area. All samples were analysed for metals (using ICP-AES) and other elements, and concentrations were compared to local and international standards. Results and Discussion The river carries a very high load of SO4, NH4, PO4, Cl, F, Fe, Cu, Pb, Zn, Al and other potentially toxic elements. Precipitation and discharge data over the period of 1980 – 2000 clearly show that the precipitation on the Ijen plateau influences water chemistry of the downstream river. Metal concentrations in the river water exceed the concentrations mentioned in Indonesian and international quality guidelines, even in the downstream river and the irrigation area. Some metal concentrations are extremely high, especially iron (up to 1600 mg/l) and aluminium (up to 3000 mg/l). The food-webs in the acidic parts of the river are highly underdeveloped. No invertebrates were present in the extremely acid water and, at pH 2.3, only chironomids were found. This also holds true for the river water with pH 3.3 in the downstream area. Agricultural soils in the irrigation area have a pH of 3.9 compared to a pH of 7.0 for soils irrigated with neutral water. Decreased yields of cultivated crops are probably caused by the use of Al containing acid irrigation water. Increased levels of metals (especially Cd, Co, Ni and Mn) are found in different foodstuffs, but still remain within acceptable ranges. Considering local residents” diets, Cd levels may lead to an increased risk for the human health. Fluoride exposure is of highest concern, with levels in drinking water exceeding guideline values and a lot of local residents suffering from dental fluorosis. Conclusions, Recommendations and Outlook In short, our data indicate that the Ijen crater lake presents a serious threat to the environment as well as human health and agricultural production.     

Formation of Nitrate and Sulfate in the Plume of Berlin (8 pp)

Background, Aims and Scope Secondary inorganic aerosol (SIA), i.e. particulate sulphate (S(VI)), ammonium and nitrate (N(V)) is formed from gaseous precursors i.e., sulfur dioxide (S(IV)), ammonia and nitrogen oxides, in polluted air on the time-scale of hours to days. Besides particulate ammonium and nitrate, the respective gaseous species ammonia and nitric acid can be formed, too. SIA contributes significantly to elevated levels of respirable particulate matter in urban areas and in strongly anthropogenically influenced air in general. Methods The near-ground aerosol chemical composition was studied at two stationary sites in the vicinity of Berlin during a field campaign in summer 1998. By means of analysis of the wind field, two episodes were identified which allow to study changes within individual air masses during transport i.e., a Lagrangian type of experiment, with one station being upwind and the other downwind of the city. By reference to a passive tracer (Na+) and estimates on dry depositional losses, the influences of dispersion and mixing on concentration changes can be eliminated from the data analysis. Results and Discussion Chemical changes in N(-III), N(V) and S(VI) species were observed. SIA i.e., N(V) and S(VI), was formed from emissions in the city within a few hours. The significance of emissions in the city was furthermore confirmed by missing SIA formation in the case of transport around the city. For the two episodes, SIA formation rates could be derived, albeit not more precise than by an order of magnitude. N(V) formation rates were between 1.4 and 20 and between 1.9 and 59 % h-1 on the two days, respectively, and S(VI) formation rates were > 17 and > 10 % h-1. The area south of the city was identified as a source of ammonia. Conclusion The probability of occurrence of situations during which the downwind site (50 km downwind of Berlin) would be hit by an urban plume is > 7.4%. Furthermore, for the general case of rural areas in Germany it is estimated that for more than half of these there is a significant probability to be hit by an urban plume (> 8%). The S(VI) formation rates are higher than explainable by homogeneous gas-phase chemistry and suggest the involvement of heterogeneous reactions of aerosol particles. Recommendation and Outlook The possible contribution of heterogeneous processes to S(VI) formation should be addressed in laboratory studies. Measurements at more than two sites could improve the potential of Lagrangian field experiments for the quantification of atmospheric chemical transformations, if a second downwind site is chosen in such a way that, at least under particular stability conditions, measurements there are representative for the source area.     

Strategies of maintaining the natural purification potential of rivers and lakes

Surface waters have a great impact on ecology and life of man. Because of their current use and exploitation, chemical and biological pollution, as well as physical changes of rivers and lakes are common. Natural self-purification potential helps to compensate harms to a certain degree. Proposals are given to detect restrictions of the purification potential in time as well as to support and to enhance the natural purification potential.     

Aromatic photonitration in homogeneous and heterogeneous aqueous systems

This work describes the nitration of aromatics upon near-UV photolysis of nitrate and nitrite in aqueous solution and upon photocatalytic oxidation of nitrite in TiO2 suspensions. Phenol is used in this work as a model aromatic molecule and as a probe for *NO2/N2O4. The photoinduced nitration of phenol in aqueous systems occurs upon the reaction between phenol and *NO2 or N2O4, and is enhanced by the photocatalytic oxidation of nitrite to *NO2 by TiO2. Aromatic photonitration in the liquid phase can play a relevant role in the formation of nitroaromatics in natural waters and atmospheric hydrometeors, thus being a potential pathway for the condensed-phase nitration of aromatics. Furthermore, the photoinduced oxidation of nitrite to nitrogen dioxide suggests a completely new role for nitrite in natural waters and atmospheric aerosols.     

北京城市大气甲烷自动连续观测与结果分析

本文提出了自动连续监测北京城市背景下大气温室气体的方法 ,报道了 2 0 0 0年监测得到的CH4 日变化和总的变化趋势。对高密度观测获得的数据分析发现 ,北京大气CH4 的日变化呈现单周期正弦变化 ,平均浓度极大值 1.60 μg/L出现在凌晨 5 :0 0— 6:0 0 ,极低值 1.40 μg/L出现在午后 14:0 0— 15 :0 0 ,其原因很大程度上受制于光化学汇的日变化。通过研究不同季节、不同天气情况下CH4 的日变化规律发现 ,北京显然是CH4 的排放源 ,在强风条件下得到接近华北地区本底值的浓度。日变化季节差异反映了城市背景下大气CH4 的浓度主要受到汇的调制和人类活动的影响。同时 ,虽然北京大气CH4 浓度季变化仍呈双峰模态 ,但冬季峰值明显低于夏季 ,显示北京大气治理取得成效 ,人为源强度变小     

Strontium isotope constraints on the seasonal variation of the provenance of base cations in rain water at Kawakami, Central Japan

The ⁸⁷Sr/⁸⁶Sr ratios in monthly precipitation in the forested basin at Kawakami, central Japan, varied seasonally from 0.709 to 0.711 in spring to as low as 0.7062 ± 0.0004 in autumn over nine years from 1987 to 1995. The seasonal variation can be explained in terms of the mixing of three sources of Sr: sea salt (⁸⁷Sr/⁸⁶Sr 0.70917), soluble eolian minerals originating from deserts in continental Asia ( 0.711), and biogenic materials growing on soils derived from the volcanic rock substrates in the vicinity ( 0.706). It is estimated that the contribution of sea-salt Sr into the Kawakami rain Sr is relatively constant (10 ± 5%) and that more than half of the Sr is of biogenic origin throughout the year except during spring rains when 50% of the Sr is due to the dissolution of Ca-minerals from Asian dusts. The dominant contribution of eolian components to spring rains is consistent with the high concentration of ³H, which is typical of air masses from Asia.     

The distribution of the chlorinated solvents dichloromethane,perchloroethylene, and trichloroethylene in the global atmosphere

Dichloromethane, perchloroethylene, and trichloroethylene are commercially important chlorinated solvents whose health and environmental impacts are under scrutiny in the industrial world. Their distributions in the global atmosphere have been computed based on data from the Reactive Chlorine Emissions Inventory (RCEI) project using the Global Balance Environment (GLOBE) model, a 3-D radiative-dynamical-chemical model. Their atmospheric lifetimes, scaled to an observed methyl chloroform lifetime of 4.8 years, are 158 days, 105 days, and 4.3 days, respectively. They have strong interhemispheric gradients, with maximum zonal mean surface concentrations in the winter mid-latitude northern hemisphere of approximately 40 ppt, 9 ppt, and 2.5 ppt, respectively. Their spatial distributions show significant seasonal variability, and are sensitive to vertical mixing by cumulus convection and horizontal mixing by synoptic-scale turbulence. While the model interhemispheric exchange time (1.0 years) and computed atmospheric lifetimes are very sensitive to sub-grid scale diffusion, interhemispheric gradients of the chlorinated solvents are not. The simulated results suggest a greater importance for oceanic emissions of perchloroethylene and trichloroethylene than has previously been assumed.