Trace Metal Solid State Speciation in Aerosols of the Northern Levantine Basin,East Mediterranean   总被引：3，自引：0，他引：3  

Mustafa Koçak  Nilgun Kubilay  Barak Herut  Malcolm Nimmo 《Journal of Atmospheric Chemistry》2007,56(3):239-257

An established three stage sequential leach scheme was applied to a series of selected high volume aerosol samples (n = 35) collected from the Turkish Eastern Mediterranean coastline (Erdemli). Samples were selected according to their air mass back trajectory history to reflect the contrasting mixtures of aerosol material present in the Eastern Mediterranean marine aerosol. Two populations were adopted, those samples which were classed as “anthropogenic” and those which were “Saharan” dominated aerosol populations. Applying the three stage leach it was possible to define the proportion for each of the considered metals (Al, Fe, Cu, Pb, Cd, Zn and Mn) present in the (a) “exchangeable” (b) “carbonate / oxide” and (c) “refractory” phases, representing novel solid state aerosol speciation data for this marine system. Clear trends were established, conforming with data from previous studies with mainly crustal derived metals (Al and Fe) being present in the refractory phases (Al > 88%; Fe > 84%) and those influenced by anthropogenic sources being dominating in the exchangeable phase, although for these metals the variability was comparatively high (12–64%; 19–85%; 40–100% for Zn, Pb and Cd, respectively). For the majority, greater exchangeable fractions were present the lower the crustal source contribution to the aerosol population, whereas the “refractory” fraction exhibited contrasting behaviour. This was illustrated by the novel application of the mixing diagram, presenting each of the three speciation stages against the corresponding percent anthropogenic contribution to each collected sample. Zn, Pb and Cd all illustrated progressive decrease in the percent exchangeable with increasing crustal contribution to the aerosol population. The percent exchangeable was discussed in terms of its use to represent the upper limit of the bioavailable fraction of metal associated with the aerosol, post deposition. The mixing diagram approach enabled the prediction of the residual fractions for Cd, Pb and Zn (41 ± 4%; 62 ± 4% and 82 ± 5%, respectively,) in Saharan end-member material.  相似文献   

Photochemical degradation of organic iron complexing ligands in seawater     

Rodney?T.?PowellEmail author  Amy?Wilson-Finelli 《Aquatic Sciences - Research Across Boundaries》2003,65(4):367-374

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Evaluation of aluminum speciation in surface waters in China and its environmental risk assessment     

S.?P.?BiEmail author  N.?Gan  X.?C.?Lu  H.?Y.?Ni  H.?Lin  X.?L.?Wang  Z.?B.?Wei 《Environmental Geology》2003,45(1):65-71

As the ongoing global research on acid precipitation is developing in depth, more and more attention has been paid to the ecological effects of aluminum (Al) due to its toxicity to plants and animals, which is caused by acid precipitation. As a very serious problem of terrestrial and aquatic environmental acidification occurs in China, especially in southwestern China, a systematic investigation of Al speciation in these regions is very important. In this paper, the Al speciation results of surface waters in China are reported and its ecological impacts is evaluated. More than 100 water samples were collected from about twenty provinces of China. Driscoll's Al speciation scheme combined with the modified MINQEL computer model is used for speciation of Al. This study shows that the ecological impacts of acidification are quite different between China and Western countries, because of different geographical environments and geological settings. In Western countries, acidification is mainly caused by NO₂^-. Due to low concentrations of K⁺, Na⁺, Ca²⁺, Mg²⁺, the buffer capacities of soil and water are weak. Therefore, natural waters can be acidified to pH<5 very easily, resulting in a considerable mobilization of Al and worsening of the ecological environment. In China, acid precipitation is mainly in the form of sulfuric acid. In northwestern China, concentrations of K⁺, Na⁺, Ca²⁺, Mg²⁺ are high in soil and surface waters. This leads to much higher capacity and a high resistance ability to acidification. The pH values of waters in this region are high (around 7) and no serious Al toxicity is found at present. However, in northeastern and southeastern China, the soil is rich in Al (unsaturated aluminosilicates in northeastern China, saturated aluminosilicates in north and central China, aluminum-rich soil in southeastern and southwestern China). The concentrations of K⁺, Na⁺, Ca²⁺, Mg²⁺ in soil and waters are lower than those of northwestern China. Therefore the buffer capacity is limited. Numerous surface waters have already been acidified and pH values declined to 5. The impacts of Al toxicity on ecological systems in these regions are very serious, especially in Jiangxi, Hubei Provinces and Chongqing Municipality.  相似文献   

L'archivage des activités humaines par les neiges et glaces polaires : le cas du plomb     

Claude Boutron  Kevin Rosman  Carlo Barbante  Michael Bolshov  Freddy Adams  Sungmin Hong  Christophe Ferrari 《Comptes Rendus Geoscience》2004,336(10):847-867

The investigation of the occurrence of lead in dated snow and ice from Greenland and Antarctica has played a major role in our understanding of the history of the pollution of the atmosphere of our planet by this metal. Such studies have however proved to be very demanding, mainly because of the extreme purity of polar snow and ice. Reliable measurements can be obtained only if ultra-clean and highly sensitive procedures are used, as pioneered by Clair Patterson. The Greenland data show evidence of large-scale pollution of the atmosphere of the Northern Hemisphere for lead as early as two millennia ago during Greco–Roman times, especially because of mining and smelting activities in southern Spain. It peaked at the end of the 1960s, with lead concentrations in snow about 200 times higher than natural values, before declining during recent times because of the fall in the use of leaded gasoline. Lead pollution in Antarctica was already significant at the end of the 19th century as a consequence of whaling activities, the traffic of coal-powered ships crossing the Cape Horn, and mining activities in South America, South Africa and Australia. After declining because of the opening of the Panama Canal, the great economic depression and World War II, it reached a maximum during the 1980s, with lead concentrations 20 times higher than natural values. Other studies focus on past natural variations of lead in ancient ice dated from the last climatic cycles. To cite this article: C. Boutron et al., C. R. Geoscience 336 (2004).  相似文献   

Distribution and Elimination of Lead Species in Soils Related to GAP of Chinese Medicinal Materials of Ligusticum Chuanxiong Hort     

DENG Tian-long~ 《地球科学进展》2004,(Z1)

In this paper, the sequential extraction procedure was used for the selection of fractions of lead in seven stages corresponding to lead exchangeable, lead bounded to carbonates, to manganese oxides, to organic matters, to amorphous iron, and lead associated to crystallized iron, and to residuals. The vertical distributions of lead species were carried out in the soils related to good agriculture progress (GAP) of Chinese medical materials of Ligusticum chuanxiong Hort in Dujiangyan city and Wenchuan County, Sichuan Province. Based on those researches, it is found that the plant of Glycine Max (L.) Merr. has the character of lead enrichment and sorption, which is not reported in the literature. Using Glycine Max (L.) Merr. alternate planting with Ligusticum chuanxiong Hort is a valuable recommended in order to produce a high quality Chinese medical materials in order to eliminate the barrier on the beyond the lead limit for the import and export of Ligusticum chuanxiong Hort.  相似文献   

Experimental Study of Gold and Platinum Solubility in a Complex Fluid under Hydrothermal Conditions   总被引：2，自引：0，他引：2  

G. G. LIKHOIDOV  L. P. PLYUSNINA  J. A. SCHEKA  T. B. APHANAS EVA 《Resource Geology》2000,50(2):83-92

Abstract: The solubility of gold was studied in water and aqueous NaCl (1– 5 m) solutions under oxygen and sulfur buffered conditions between 300–500C at a constant pressure 1 kb. Two buffer assemblages HMP and PPM were used. Analysis of the scatter in measured values in log m_Au–m_NaCl–T frame fixed linear dependence between log m_Au and T at any studied iso‐pleth (m_NaCl) in the form of log m_Au = a. T(C) + b. Coefficients of the equation were calculated for water and NaCl (1, 3, 5 m) solutions. The maximum solubility characterizes the NaCl‐free system in the presence of HMP. In the case, Au solubility increases from (log m_Au) –6. 72 to –5. 04 at 300 and 500C, respectively. In the presence of PPM, maximum of Au solubility was obtained for the 5 mNaCl solution. In a similar manner solubility rises from –6. 54 to –5. 77 at 300 and 500C, accordingly. In studied f_O2/f_S2 area the behavior of Au solubility testified that: (i) – a composite interaction between chloride and hydrosulfide speciation of gold affects its total solubility; (ii) – in addition of NaCl up to about 1. 5 m the solubility decreases, more pronounced in the presence of HMP; (iii) – the contribution of chloride in total Au solubility is more for PPM despite of lower f_O2value, than for HMP. The solubility of platinum was studied in the Pt–Cl–S–H₂O system between 300 and 500C, 1 kb. PPM solid buffer controlled oxidation state, pH and sulfur activity of solutions (H₂O, 1 mNaCl and 0. 1 mHCl). Under the conditions, PtS precipitated from the solutions with increasing temperature and acidity. The PtS solubility in the 0. 1 m_HCl solutions lowers slightly in the range of 300–500C from –5. 30 to –5. 60 (in log m_Pt) that is typical to the hydrosulfide species. It was deduced that reducing media, regulated by the PPM assemblage, suppress activity of chloride species of Pt. More oxidizing conditions were modeled in runs using mixtures of Mn(II), Mn(III) and Mn(IV) oxides to buffer the aqueous‐chloride solutions between 300 and 500C, 1 kb. It was found that MnO tends to oxidize at T below 400C forming intermediate Mn‐hydroxides (β–MnOOH, Mn (OH)₂ and Mn₂(OH)₃Cl). These phases are metastable and transfer to Mn₃O₄ with increasing duration. Generation of the Mn‐hydroxides leads to a change of physical‐chemical parameters of the solutions, such as water activity, pH and Eh. The last results in abrupt increase in the noble metals dissolution. At stable existence of only Mn₃O₄, the solubility of both Pt and Au lowers to equilibrium values. Essential catalysis effect of Pt on intensity and rate of Mn(II) oxidation was found. The dominant role of chloride of Pt and Au was defined under most oxidized conditions, specified by Mn₂O₃–MnO₂ buffer. So at 400C, dissolved Au (log m_Au) increases from –4. 40 in water to –1. 00 in 0. 1 m_HCl, and ones of Pt (log m_Pt) from –4. 80 to –2. 90 accordingly. Thus, mixing of hydrosulfide and chloride solutions, as well as transformation of the systems to the stable state act upon total solubility of the noble metals.  相似文献   

The Influence of Oxalate on Fe-Catalyzed S(IV) Oxidation by Oxygen in Aqueous Solution     

A. Wolf  F. Deutsch  P. Hoffmann  H. M. Ortner 《Journal of Atmospheric Chemistry》2000,37(2):125-135

This study demonstrates that oxalate has a strong inhibiting effect onFe-catalyzed S(IV) oxidation by oxygen in aqueous solution. While thepseudo-first order rate constant of S(IV) oxidation was determined to be1.6 × 10³ M^-1 s^-1 in experimentswithout oxalate, the oxidation of S(IV) was totally inhibited at a molarconcentration ratio of iron:oxalate = 1:5 at an oxalate concentration of 4M. Under these conditions, the Fe(II)/Fe(III) ratio remained nearlyconstant during the observed reaction time. The determined rate constants wereindependent of the initial oxidation state of iron. However, with increasingconcentrations of oxalate, a longer induction period is observed forexperiments with iron initially in the Fe(II) oxidation state.  相似文献   

Secondary geochemical dispersion in the Precambrian auriferous Hutti-Maski schist belt, Raichur district, Karnataka, India. Part I: anomalies of As, Sb, Hg and Bi in soil and groundwater     

N. R. Sahoo  H. S. Pandalai   《Journal of Geochemical Exploration》2000,71(3):353

The nature of secondary geochemical dispersion of As, Sb, Hg and Bi in soil and ground water of the semi-arid, tropical, Archaean, auriferous, Hutti-Maski greenstone belt has been investigated for identification of appropriate geochemical techniques for Au exploration in similar terrains.Results indicate that the <180 μm size-fraction of C-horizon soil is an appropriate sampling medium for delineating pedogeochemical anomalies of As, Sb, Hg and Bi related to gold mineralisation. These pedogeochemical anomalies along with anomalous values of alkalinity, chloride, sulphate, As and Sb in groundwater are controlled significantly by primary mineralisation located along shear zones in the greenstone belt. Arsenic anomalies in soil are broad, whereas, those of Sb and Bi are restricted to narrow zones directly over mineralised areas. In contrast, Hg anomalies around known mineralised areas are irregular and do not clearly demarcate the mineralised areas. The study indicates that anomalies of As, Sb and Hg in soil are principally hydromorphic, whereas those of Bi are clastic.The study recommends use of groundwater sampling at 2–3 km spacing with routine analysis of chloride, sulphate and alkalinity along with As and Sb in the first phase. This may be followed up with sampling of C-horizon of soils on a 1 km square grid for As-anomalies. Arsenic-anomalous areas may be sampled for As, Sb, Hg and Bi on a 500 m square grid for detailed exploration.  相似文献   

Influence of Temporal Variations in River Discharge, pH, Alkalinity and Ca on the Speciation and Concentration of Heavy Metals in Some Mining Polluted Rivers     

Pål Gundersen  Eiliv Steinnes 《Aquatic Geochemistry》2001,7(3):173-193

Dissolved (dialysis in situ) and total concentrations ofCu, Zn, Cd and Al in eight mining polluted rivers in the Røros area, central Norway, were determinedby atomic absorption spectrometry (flame and graphite furnace) and compared to pH, Caconcentration and alkalinity through seasonal variations in river discharge. Totalconcentrations of the metals were highest during early spring flood and during summer andautumn rain episodes. Dissolved concentrations also increased as the spring floodproceeded, but small discharge peaks within this 2 month period as well as a considerableautumn flood episode appeared to lower rather than to raise the dissolved metal concentrations.Consequently the dissolved fractions of Zn, Cd and Al showed a significant negative correlationwith river discharge, and were low at the discharge peaks. Possibly high sediment concentrationsoccurring at high flood conditions more than counteracted desorption induced by pHdecrease, and led to decreased dissolved fractions through adsorption. Cu speciationon the other hand seemed to be more closely linked to pH. Alkalinity and Ca concentration,both assumed to protect aquatic life from metal pollution, were significantly lowerduring episodes with high Cu and Al total concentrations.  相似文献   

气相色谱和薄层色谱法在形态分析中的应用   总被引：2，自引：0，他引：2  

方国桢  方梅 《岩矿测试》1996,15(4):299-310

评述了气相色谱和薄层色谱法用于氯、溴、碘、硫、硒、碲、铬、氮、磷、砷、钒、碳、锡、铅、铁和汞１６种元素的不同形态分析的进展。这些形态包括不同价态、有机态、无机态、阳离子和阴离子态等。由于气相色谱和薄层色谱法都具有分离和检测两种功能结合的特点，因此它们是用于元素形态分析的有效和方便的方法。引用１９８０～１９９４年文献９２篇  相似文献