Distribution and mobility of heavy metals in paddy soils of the Kočani Field in Macedonia

Contamination of soils with heavy metals is widespread and poses a long-term risk to ecosystem health. Abandoned and active mining sites contain residues from ore-processing operations that are characterised by high concentrations of heavy metals. The distribution and mobility characteristics of heavy metals (As, Cd, Cu, Pb, and Zn) in paddy soil samples from Kočani Field (Macedonia) using ICP-EAS and a sequential extraction procedure was evaluated. The results indicate that highly elevated concentrations of As, Cd, Cu, Pb, and Zn were detected in the paddy soil sample from location VII-2 in the vicinity of Zletovo mine and Zletovska river in the western part of Kočani Field, which drains the untreated acid mine waters and mine wastes from the active Zletovo mine. The degree of contamination based on index of geoaccumulation (I _geo) from strong to weak in the paddy soils samples is Pb > As > Cd > Zn > Cu. The mobility potential of heavy metals in all paddy soil samples increases in the order As < Cu < Pb < Zn < Cd. According to the results of the anthropogenic impact on the paddy soils, a further study on the heavy metal concentrations in rice and other edible crops, the remediation process of the paddy soils and a dietary study of the local population are needed.     

Chemical speciation of heavy metals and arsenic in tailings and soils contaminated by mining activities （Northern Portugal）

A chemical sequential speciation of heavy metals （Fe, Mn, Cu, Zn, Pb, Cd, Sn, W, Bi, Ni, Cr, Mo, Co） Al, Ti and As in tailings and soils around five W/Sn mines （Adoria Mine, Ervedosa Mine, Regoufe Mine, Rio de Frades Mine and Tarouca Mine-Northern Portugal） was realized using a 7-steps fractionation procedure. Each of the chemical fractions was operationally defined as （Dold and Fontbote 2001）： （1） water-soluble; （2） exchangeable; （3） bound to Fe oxyhydroxides （or easily reducible）; （4） bound to Fe oxides （or moderately reducible）; （5） bound to organic matter and secondary Cu-sulfides; （6） bound to primary sulfides; and （7） residual. The extracted element contents at each step were measured by ICP-MS. Samples were also analyzed for pH, electrical conductivity and organic matter. The results allowed us to notice that： （1） the pH was the main factor controlling the geochemical distribution of the studied elements. The tailing and soil samples were very acid, with an average pH of approximately 4.37. Some metal cations （Mn, Cd, Cu, Zn, Pb, Co, Cr, Ni） behave in a similar way, revealing important enrichments in the most bioavailable fractions （water-soluble and exchangeable fractions）. In contrast, oxyanions such as Mo and As show low mobility through adsorption to Fe（Ⅲ） oxyhydroxides dissolved in the two reducible fractions. These results reflect the pH dependent adsorption on the clay minerals, Fe and Mn oxyhydroxides and the co-precipitation with these secondary minerals; （2） residual fraction was the most important fraction for Sn, Ti, Al, Mn, V, Cr and Zn. These results suggest that in these soils these elements are in a detrital, non-available form; （3） large amounts of Fe, Mn, Cu, Zn, Pb, Cd, Bi, Cr, Ni, Co and As were present in the most bioavailable fractions in all sampling sites as consequence of the oxidation and acidification processes in sulfidic mine wastes;     

Genetic investigation and comparison of Kartaldağ and Madendağ epithermal gold deposits in Çanakkale,NW Turkey

Two epithermal gold deposits (Kartaldağ and Madendağ) located in NW Turkey have been characterized through the detailed examinations involving geologic, mineralogical, fluid inclusion, stable isotope, whole-rock geochemistry, and geochronology data.The Kartaldağ deposit (0.01–17.65 ppm Au), hosted by Eocene dacite porphyry, is associated with four main alteration types with characteristic assemblage of: i) chlorite/smectite–illite ± kaolinite, ii) quartz–kaolinite, iii) quartz–alunite–pyrophyllite, iv) quartz–pyrite, the last being characterized by three distinct quartz generations comprising massive/vuggy (early), fine–medium grained, vug-lining (early), and banded, colloform, comb (late) textures. Observed sulfide minerals are pyrite, covellite, and sphalerite. Oxygen and sulfur isotope analyses, performed on quartz (δ¹⁸O_(quartz): 7.93 to 8.95‰ and calculated δ¹⁸O_(H2O): − 7.95 to 1.49‰) and pyrite (δ³⁴S_(pyrite): − 4.8‰ and calculated δ³⁴S_(H2S): − 6.08 to − 7.20‰) separates, suggest a meteoric water source for water in the hydrothermal fluid, and an igneous source for the sulfur dissolved in ore-related fluids. Microthermometric analyses of primary fluid inclusion assemblages performed on quartz (late quartz generation) yield temperatures (Th) dominantly in the range of 245–285 °C, and generally low salinity values at 0 to 1.7 wt.% NaCl eq. Based on the quartz textures and the associated base metal concentrations, along with fluid inclusion petrography, the early vug-lining quartz is considered to have been associated with the mineralization possibly through a boiling and a late mixing process at > 285 °C.The Madendağ deposit (0.27–20.60 ppm Au), hosted by Paleozoic mica schists, is associated with two main alteration types: sericite–illite–kaolinite, and quartz–pyrite dominated by two distinct quartz generations i) early colloform, comb and banded quartz and ii) late quartz, forming the cement in hydrothermal breccia. Whereas oxygen isotope analyses of quartz (δ¹⁸O_(quartz): 9.55 to 18.19‰ and calculated δ¹⁸O_(H2O): − 2.97 to 5.54‰) suggest varying proportions of meteoric and magmatic sources for the ore bearing fluid, sulfur isotope ratios (δ³⁴S_(pyrite): − 2.2‰ and calculated δ³⁴S_(H2S): (− 3.63) to (− 3.75) ‰) point to an essentially magmatic source for sulfur with or without contribution from sedimentary sources. Microthermometric analysis carried out on primary fluid inclusion populations of a brecciated sample (early quartz), give a temperature (Th) range of 235–255 °C and 0.0 to 0.7 wt.% NaCl eq. salinity. Based on the textural relationship, base metal and high gold contents, the ore precipitation stage is associated with late stage quartz formation via a possible boiling process.The presence of alunite, pyrophyllite and kaolinite, vuggy quartz and covellite suggest a high-sulfidation type of epithermal deposit for Kartaldağ. On the other hand, Madendağ is identified as an adularia-sericite type owing to the presence of significant sericite, neutral pH clays (mostly illite, chlorite/smectite, and kaolinite), low temperature quartz textures (e.g., colloform, comb, and banded quartz), and limited sulfide minerals.Given the geographical proximity of Kartaldağ and Madendağ deposits, the similar temperature and salinity ranges obtained from their fluid inclusions, and the similar ages of igneous rocks in both deposits (Kartaldağ: 40.80 ± 0.36 to 42.19 ± 0.45 Ma, Madendağ: 43.34 ± 0.85 Ma) the mineralizing systems in both deposits are considered to be genetically related.     

Stabilities of heavy metals in soils treated with red mud

This paper discussed the stabilities of heavy metals in soils treated with red mud. Soil has been polluted by heavy metals more and more seriously during recent several decades, and they are harmful to mankind and animals. The current tendency is to develop in-situ technique by using industrial processing waste as additives to stabilized heavy metals to minimize the disturbance of contaminated soils. Soil samples were collected from the Niujiaotang mining area, Guizhou Province, southwestern China. They were farmed soils polluted weakly by fly ash （QBT） and polluted badly by waste water （BXT） from smelter, respectively. One of the red mud samples （BRM） was collected from Bayer process and the other （CRM） from confederate process in the Alumina Plant of Guizhou. Free metal ion concentrations were analyzed with Donnan Membrane Technique and predicted with ECOSAT. The concentrations of free heavy metal ions in QBT increased after appending CRM, but decreased when adding BRM. The more the red mud was added, the higher the concentration would be, and the free concentrations of nickel and cadmium ions would vary more greatly than those of copper and zinc ions. When appending red muds into BXT, the free concentrations of copper and zinc ions varied little. While those of free nickel and cadmium decreased obviously at the ratio of 2.00%. The variation of the concentration was still biggish after appending BRM at the ratio of 0.50%, but smaller than that of 2.00%. The concentrations of free cadmium ions increased after adding CRM at the ratio of 0.50%. All experimental processes were modeled through ECOSAT. The predicted and measured results were consistent, except for zinc. Contributions of soil sorbents to the heavy metal adsorptions were also modeled through ECOSAT. The sorbents in soil included soil organic matter, iron hydroxides, clay and the Donnan gel of soil organic matter. Compared to the soils without red muds, no matter what kind of red mud and how much was added in soil, the contributions changed slightly.     

Enrichment and mobility of cadmium and other heavy metals in the area of the Three-Gorges Reservoir

This study focused on the geochemical distribution patterns and ecological effects of Cd and other heavy metals such as As, Hg, Cr, Cu, Ni, Pb, and Zn in rock, soil, water, sediment and crops in the area of the Three-Gorges Reservoir within Chongqing, and aimed at the protection of ecological environment and rational application of the local lands. This study found that the metals of Cd, Hg and Pb presented pollution in the surface environment along the Yangtze River, that is Cd〉Hg〉Pb （Cu）〉Zn〉As〉Ni〉Cr. The pollution of Cd in sediment was mainly attributable to the regional black shales, and partly to the urban sewage and garbage. The geochemical modes of metals in the sediment varied. Cr, Hg, Ni, and Pb mainly existed as residues, and Cd as carbonate. Cd exited as a high proportion in the modes of ion-exchange, carbonate, and iron-manganese oxidation, up to 63 percent. The contents of heavy metals in soiland sediment were correlated to the host clay minerals, such as illite, montmorillonite, kaolinite and chlorite. It is shown that Cd was transported with clay minerals in the Yangtze River over long distance and formed the regional anomaly. In the abnormal area of Jianping in Wushan County, higher Cd contents are reported in the local crops and local villagers＇ hairs than from the background areas.     

Assessment of heavy metals contamination in soils of Dexing region, Jiangxi Province, China

Heavy metal contamination has attracted huge concern due to its toxicity, abundance and persistence in the environment, and subsequent accumulation in soil, sediment and water. Mining is one of the most important sources of heavy metals in the environment. Mining-milling operations and disposal of tailings （the finely ground remains of milled ores） in addition to smelting and metal refining provide significant sources of pollution. Mining and mineral processing in the Dexing region of China have been carried out for over forty years and have contaminated the soils with heavy metals, Many studies were conducted to assess and establish the extent of heavy metal contamination in the soils due to mining. The aim of this work was to assess the environmental impact of mining on soils in the Dexing region and to identify the main factors involved in heavy metals dispersion. A 4800 km^2 study area was assessed with respect to its heavy metals on the basis of the current guideline values. In order to assess the extent of heavy metals contamination resulting from past mining activities in the Dexing region, 919 soil samples were collected and analyzed for As, Hg, Cd, Cr, Zn, Cu and Pb, Heavy metals levels were determined using inductively couple plasma-atomic emission spectrometry and X-ray fluorescence spectrometry. Results of soil samples reported concentrations between 1.790-899 mg/kg for As, 0.034-4.980 mg/kg for Hg, 0.043-8.330 mg/kg for Cd, 10-666 mg/kg for Cr, 25-18500 mg/kg for Zn, 6-1825 mg/kg for Cu, and 16-1312 mg/kg for Pb, respectively. The maximum values of As, Hg, Cd, Cr, Zn, Cu and Pb concentration in soils were up to 60, 33, 41, 7, 185, 52 and 37 times higher than the tolerable level, respectively. Meanwhile, the single-factor pollution index and Nemerow pollution index were used to assess the environment quality of heavy metals contamination.     

Assessment of spatial distribution and possible sources of heavy metals in the soils of Sariseki-Dörtyol District in Hatay Province (Turkey)

In this study, total heavy metal content of soil and their spatial distribution in Sar?seki-Dörtyol district were analyzed and mapped. Variable distance grids (0.5, 1.0 and 2.0 km) were established, with a total of 102 soil samples collected from two different soil depths (0–5 and 5–20 cm) at intersections of the grids (51 sampling point). Soil samples were analyzed for heavy metals (Cd, Co, Cr, Cu, Pb, Zn, Mn, Fe, and Ni). The most proper variogram models for the contents of all heavy metal were spherical and exponential ones. The ranges of semivariograms were between 1.9 and 31.1 km. According to the calculated geoaccumulation (I _geo) values, samples from both soil depths were classified as partly to highly polluted with Cd and Ni and partly polluted with Cr and as partly polluted-to-not polluted with Pb and not polluted with Cu, Fe and Mn. Similar results were also obtained when evaluated by the enrichment factor. The contamination levels of the heavy metals were Ni > Cd > Cr > Pb > Zn > Cu > Co > Fe > Mn in decreasing order. The soils in the study area are contaminated predominantly by Cd and Ni, which may give rise to various health hazards or diseases. Cadmium pollution results primarily from industrial activities and, to a lesser extent, from vehicular traffic, whereas Ni contents in the study area result from parent material, phosphorus fertilizer, industries, and vehicles.     

Spatial distribution of heavy metals and arsenic in soils of Aragón (northeast Spain): controlling factors and environmental implications

Legal regulation of heavy metal contents is an important issue in many European countries, where laws still do not exist establishing the heavy metal levels permitted in soils. As a first step to determine the reference levels of heavy metals, it is necessary to know their contents in soils under natural conditions. To achieve this goal in the Autonomous Community of Aragón, a total of 133 sites have been sampled. A balanced allotment of the sampling sites, according to soil spatial distribution in the region, has been carried out by selecting 9 soil types that represent 97.5% of its surface area. Fifteen elements (Cr, Cu, Ba, As, Sb, Hg, Sn, Mn, Fe, Al, Zn, Ni, Co, Cd and Pb) have been analysed by (ICP–AES) after a partial acid extraction. The content of analysed elements has been correlated to some soil parameters such as organic matter, pH, and granulometric fractions. Results of the statistical analyses have shown a large variety and complexity in some of these relationships. The main factors for variation in the heavy metal contents are both the soil type and the lithology. Gypsisols and Calcisols developed on sedimentary rocks have the lowest contents while Leptosols overlying metamorphic and igneous rocks have the highest contents. The spatial distribution of heavy metal contents shows a large variability with the highest contents in the mountain ranges (Iberian and Pyrenees) and the lowest in the plains of the central Ebro valley.     

Mineralogy, geochemistry and release of heavy metals in wastes from indigenous zinc smelting in Northwest Guizhou

Environmental impact resulting from mining activities is serious and ubiquitous all over the world, and it has become one of the important aspects in environmental geochemistry. The environment was seriously damaged by wastes from historical zinc smelting in Northwest Guizhou. The geochemical distributions of Pb and Zn in the different grain-size fractions of wastes indicate that the coarser particles show similar or even higher heavy metal concentrations than finer ones in the samples, although the concentrations of heavy metals tend generally to increase as the size fractions get finer. The heavy metal contents are very high, with maximum values of 31631, 57178, 2367 and 311.5 mg/kg for Pb, Zn, Cu and Cd, respectively. It is also shown that the residual fraction of Pb is less than that of Zn, accounting for 0.39%-15.75% and 14.3%-46.2%, respectively, of the total, and this is likely relative to Zn-silicate minerals formed from smelting. Although the relative partitioning of Pb and Zn is very low （0.03%- 1.3.% for Pb; 0.03% -3.3% for Zn）, the exchangeable fraction of the waste contains large amounts of heavy metals （1.5%-385 μg/g for Pb; 3-590 μg/g for Zn）. Heavy metals in exchangeable forms have the highest solubility to give the highest potential bioavailability in contrast to other chemical forms. Mineralogical study indicates that the wastes were found to be highly heterogeneous materials, dominated by quartz, feldspar, carbonatite, iron or/and aluminum vitric compounds and a few secondary mineral phases, and their contents vary with the type of smelting wastes. The secondary minerals formed from smelting and sequentially weathering are the major chemical phase for heavy metals. Complex composition of many phases and substitution of elements suggested that many of the phases were found to be non-stoichiometric compounds. Pb was found to be the main Pb phase in the wastes by precipitation or/and adsorption.     

Spatial distribution, source identification and affecting factors of heavy metals contamination in urban–suburban soils of Lishui city, China

An investigation on spatial distribution, possible pollution sources, and affecting factors of heavy metals in the urban–suburban soils of Lishui city (China) was conducted using geographic information system (GIS) technique and multivariate statistics. The results indicated that the topsoils in urban and suburban areas were enriched with metals, such as Cd, Cu, Pb, and Zn. Spatial distribution maps of heavy metal contents, based on geostatistical analysis and GIS mapping, indicated that Cd, Cr, Cu, Mn, Ni, Pb, and Zn had similar patterns of spatial distribution. Their hot-spot areas were mainly concentrated in the densely populated old urban area of the city. Multivariate statistical analysis (correlation analysis, principal component analysis, and clustering analysis) showed distinctly different associations among the studied metals, suggesting that Cr, Cu, Ni, Pb, Cd, and Zn had anthropogenic sources, whereas Co and V were associated with parent materials and therefore had natural sources. The Cd, Cr, Ni, Pb, and Zn contents were positively correlated with soil organic matter, pH, and sand content (p < 0.01). It is concluded that GIS and multivariate statistical methods can be used to identify hot-spot areas and potential sources of heavy metals, and assess soil environment quality in urban–suburban areas.     

Contamination and bioavailability of heavy metals in sediments from the Yangtze River Delta Region

The Yangtze River Delta Region is one of the most important economic development areas in China. In the process of its industrialization and urbanization, a great deal of wastewater is poured into rivers, lakes and coasts. Researches on contamination and bioavailability of heavy metals can help us to assess the ecological risks in the aquatic environment of the Yangtze River Delta. The samples were collected from three environmental compartments including the Yangtze River, Taihu Lake, and the south coast of Jiangsu. The concentrations of heavy metals were determined by ICP-MS. Metal speciation was determined by the sequential extraction procedure modified based on Tessier＇s scheme. Among the seven elements of Cu, Pb, Zn, Cr, Cd, Co, Ni detected, the contents of Cr, Zn did not vary significantly, while Cd and Pb varied significantly. Compared to the background values （loess in the basement）, all metals detected except Co, Cr exceeded the background level. Cd had the greatest exceeding values, reaching 2 to 7 times. Ni and Pb were followed. The contents of Zn were comparatively high in lake sediments, especially in the lake bays. Ni was enriched in fiver sediments and Cu was highest in sediments from the Yangtze River estuary. Cd and Pb were concentrated in the coastal sediments. Comparatively, in space, Cr was associated with the carbonate fractions in the bay of lake. Cu-bound Fe-Mn oxides and Ni in residual form were highest in the open lake. In the river environment, Fe/Mn oxide-bound Pb, exchangeable Cd were the highest fractions. In the estuary environment, Pb and Zn bound carbonates, Cd-bound Fe-Mn oxides are the largest fractions. Cd in the exchangeable fraction, Cu-bound Fe-Mn oxides had the larger proportions in the coast. In general, the bioavailability of Cu and Cd were high in lake environment, the available Pb, Cd were remarked in river environment, and Pb and Zn were easily assimilated by creatures in estuary.     

Contamination and distribution of heavy metals in urban soil in Zhangzhou City, Fujian, China

The urban environment quality is of vital importance as the majority of people now live in cities. Due to the continuous urbanization and industrialization with rapidly increasing economy in China, metals are continuously emitted into soils, imposing a great threat on human health. Urban soils might be affected by industrial activities, transport, agricultural practice, and waste disposal. An extensive survey was conducted in the highly urbanized Zhangzhou City （Fujian Province, China） using a systematic sampling strategy. Concentrations of Hg, Cd, Pb, Zn, Cu, As, Cr and Ni were measured on 108 topsoil samples collected from parks （0-15 cm）, residential areas and suburban agricultural soils. Statistic approach （cluster analysis） was adopted for identification of natural and anthropogenic influence on heavy metal contents. The maps of metal concentrations in surface soils were made based on geographical information system （GIS） data. All of these aim at assessing the distribution of these heavy metals in the urban environment.     

Sedimentological and Petrographical Aspects of Upper Miocene Evaporites in the Beypazari and Çankiri-Çorum Basins,Central Anatolia,Turkey

The Southeast Anatolian orogen is a part of the eastern Mediterranean-Himalayan orogenic belt. Development of the Southeast Anatolian orogen began with the first ophiolite obduction onto the Arabian platform during the Late Cretaceous, and it continued until the Miocene. Its lingering effects continue to be discernible at present. During the Late Cretaceous-Miocene interval, three major deformational phases occurred, related to Late Cretaceous, Eocene, and Miocene nappe emplacements. The Miocene nappes are composed of ophiolites and metamorphic massifs.

For a decade, field studies in the region have shown that strike-slip tectonics played a role complementary to the major horizontal effects of the nappe movement, as indicated by: (1) fault systems active during the Eocene; (2) different Eocene rock units composed of coeval continental and deep-sea deposits and presently tectonically juxtaposed; and (3) other stratigraphic and structural data obtained across the present strike-slip fault zones.

These strike-slip faults possibly resulted from oblique subduction of the mid-oceanic ridge underneath the northerly situated Yuksekova ensimatic island-arc complex, causing a gradual cessation of the island-arc system. The subduction also led to the development of a back-arc pull-apart basin, i.e., the Maden basin, which opened on the upper plate. The geologic history in Southeast Anatolia resembles the development of the San Andreas fault system and subsequent tectonic evolution.     

Speciation and potential remobilization of heavy metals in sediments of the Taihu Lake, China

The species of Cu, Pb, Zn, Cd and Cr in sediments of the Taihu Lake, China, have been analyzed using the sequential chemical extraction method. Variations in the chemical fractions of these metals and their geographic distributions have also been studied. For all five metals, the residual fraction is highest but the exchangeable fraction is lowest among all the fractions. Compared to other metals, Cd has the highest percentage in the exchangeable fraction, and Cr is associated mainly with the residual fraction. Cu in the organic fraction and Pb in the Fe-Mn fraction are the important species, whereas the lowest percentages are found for Cd in the organic fraction, Cu in the Fe-Mn oxide fraction and Pb in the carbonate fraction. With respect to spatial differences, the total contents in the non-residual fractions of the metals in bay sediments are found to be higher than those in other sediments. The fractions of Cd, Cu and Cr showed significant variations in different regions. The fractions of Pb and Zn, however, did not show significant variations in spatial distribution, suggesting different amounts and different paths of anthropogenic input for the metals. Comparisons of the metal speciation indicated that Cd might be the most bioavailable metal, followed by Pb.     

Bioavailability of Tl in soils, uptake by crops and its environmental impact

This study draws attention to the fact that natural processes can mobilize thallium (Tl), a highly toxic metal, which may enter the food chain with severe health impacts on the local human population. A rural area having independent Tl mineralization in s…     

Estimation of environmental impacts on the water quality of the Tahtalıdam watershed in İzmir, Turkey

Water pollution is a widespread problem in different areas of the world. Some of these problems originated from point contamination sources and widespread contaminant outlet sources which are observed in every country. The major elements and chemical loads of surface water have been dominated by constituents derived directly or indirectly from human activities and/or industrial practices that have increased additives in the last several decades. The point sources of contamination may result from the direct wastewater discharges to the dam sites, which are considered to be the most commonly encountered water pollution problems. One of these problems is the eutrophication process which usually occurs in the static water mass of lakes and other surface water reservoirs. This process may be caused by the continuous increase of nitrogen and phosphorus contents and decrease of O₂ level in water causing an anaerobic condition which may stimulate algae-growth flow in these water bodies, consequently reducing the quality of water. Of course, there are many research methods for determining the various kinds of water pollution. In this research, the hydrochemical parameters were evaluated to estimate the types of pollution sources, the level of pollution, and its environmental impacts on the Tahtal dam reservoir.     

Distribution of heavy metals in urban soils – a case study of Danang-Hoian Area (Vietnam)

 This work is part of a research study which is intended to study the degree of anthropogenic influences of the trace metal distribution of soils from Danang-Hoian area (Vietnam). Cu, Ni, Zn and Zr show significant effects in most of the cultivated soil categories, especially in the industrial soils. Extremely high levels of Pb (up to 742 μg/g) are observed in the industrial soil category, which shows an enrichment factor 114 as compared to rural soils. Cd shows only a relative local enrichment with the maximum level of 4.6 μg/g in urban soils. Sequential extraction was performed in selected samples to evaluate the geochemical trace metals. The result indicates that Zn and Cr are mainly found in the crystal and amorphous Fe oxide bounded forms. The contents of Cr in these fractions comprise more than 94% of total extractable Cr. In the case of Zn, 85% of total extractable Zn is in fractions F_V and F_VI. Cu is mainly found in the organic fraction at an average of 39.3% of total extractable content. On the other hand, heavy metal contents show an increasing tendency in the fine fraction (silt and clay). Received: 4 February 1998 · Accepted: 26 November 1998