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1.
In order to evaluate thermodynamic speciation calculations inherent in biotic ligand models, the speciation of dissolved Cd, Cu, Pb, and Zn in aquatic systems influenced by historical mining activities is examined using equilibrium computer models and the diffusive gradients in thin films (DGT) technique. Several metal/organic-matter complexation models, including WHAM VI, NICA-Donnan, and Stockholm Humic model (SHM), are used in combination with inorganic speciation models to calculate the thermodynamic speciation of dissolved metals and concentrations of metal associated with biotic ligands (e.g., fish gills). Maximum dynamic metal concentrations, determined from total dissolved metal concentrations and thermodynamic speciation calculations, are compared with labile metal concentrations measured by DGT to assess which metal/organic-matter complexation model best describes metal speciation and, thereby, biotic ligand speciation, in the studied systems. Results indicate that the choice of model that defines metal/organic-matter interactions does not affect calculated concentrations of Cd and Zn associated with biotic ligands for geochemical conditions in the study area, whereas concentrations of Cu and Pb associated with biotic ligands depend on whether the speciation calculations use WHAM VI, NICA-Donnan, or SHM. Agreement between labile metal concentrations and dynamic metal concentrations occurs when WHAM VI is used to calculate Cu speciation and SHM is used to calculate Pb speciation. Additional work in systems that contain wide ranges in concentrations of multiple metals should incorporate analytical speciation methods, such as DGT, to constrain the speciation component of biotic ligand models.  相似文献   

2.
The effect of cell wall-associated extracellular polymeric substances (EPS) of the Gram-negative bacterium Shewanella oneidensis strain MR-1 on proton, Zn(II), and Pb(II) adsorption was investigated using a combination of titration/batch uptake studies, surface complexation modeling, attenuated total reflectance - Fourier transform infrared (ATR-FTIR) spectroscopy, and Zn K-edge extended X-ray absorption fine structure (EXAFS) spectroscopy. Both unmodified (wild-type (WT) strain) and genetically modified cells with inhibited production of EPS (ΔEPS strain) were used. Three major types of functional groups (carboxyl, phosphoryl, and amide groups) were identified in both strains using ATR-FITR spectroscopy. Potentiometric titration data were fit using a constant capacitance model (FITEQL) that included these three functional groups. The fit results indicate less interaction of Zn(II) and Pb(II) with carboxyl and amide groups and a greater interaction with phosphoryl groups in the ΔEPS strain than in the WT strain. Results from Zn(II) and Pb(II) batch adsorption studies and surface complexation modeling, assuming carboxyl and phosphoryl functional groups, also indicate significantly lower Zn(II) and Pb(II) uptake and binding affinities for the ΔEPS strain. Results from Zn K-edge EXAFS spectroscopy show that Zn(II) bonds to phosphoryl and carboxyl ligands in both strains. Based on batch uptake and modeling results and EXAFS spectral analysis, we conclude that the greater amount of EPS in the WT strain enhances Zn(II) and Pb(II) uptake and hinders diffusion of Zn(II) to the cell walls relative to the ΔEPS strain.  相似文献   

3.
《Applied Geochemistry》1998,13(2):213-233
Porewater concentration profiles were determined for Fe, trace elements (As, Cd, Co, Cu, Mn, Ni, Pb, Zn), sulfide, SO4 and pH in two Canadian Shield lakes (Chevreuil and Clearwater). Profiles of pyrite, sedimentary trace elements associated with pyrite and AVS were also obtained at the same sites. Thermodynamic calculations are used, for the anoxic porewaters where sulfide was measured, to characterize diagenetic processes involving sulfide and trace elements and to illustrate the importance of sulfide, and possibly polysulfides and thiols, in binding trace elements. The ion activity products (IAP) of Fe sulfide agree with the solubility products (Ks) of greigite or mackinawite. For Co, Ni and Zn, IAP values are close to the KS values of their sulfide precipitates; for Cu and Pb, IAP/Ks indicate large oversaturations, which can be explained by the presence of other ligands (not measured) such as polysulfides (Cu) and thiols (Pb). Cobalt, Cu, Ni and Zn porewater profiles generally display a decrease in concentration with increasing ΣH2S, as expected for transition metals, whereas Cd, Pb and Zn show an increase (mobilisation). The results suggest that removal of trace elements from anoxic porewaters occurs by coprecipitation (As and Mn) with FeS(s) and/or adsorption (As and Mn) on FeS(s), and by formation of discrete solid sulfides (Cd, Cu, Ni, Pb, Zn and Co). Reactive Fe is extensively sulfidized (51–65%) in both lakes, mostly as pyrite, but also as AVS. Similarities between As, Co, Cu and Ni to Fe ratios in pyrite and their corresponding mean diffusive flux ratios suggest that pyrite is an important sink at depth for these trace elements. High molar ratios of trace elements to Fe in pyrite from Clearwater Lake correspond chronologically to the onset of smelting activities. AVS can be an important reservoir of reactive As, Cd and Ni and, to a lesser extent, of Co, Cu and Pb. Overall, the trace elements most extensively sulfidized were Ni, Cd and As (maximum of 100%, 81% and 49% of the reactive fraction, respectively), whereas Co, Cu, Mn, Pb and Zn were only moderately sulfidized (11–16%).  相似文献   

4.
In this paper, the behaviors of aqueous zinc sorption by hydroxyapatite in the co-existence of Pb^2＋, Cd^2＋ and Cu^2＋ are investigated, the effects of Pb^2＋, Cd^2＋ and Cu^2＋ on the sorption of Zn^2＋ are discussed, and the hydroxyapatite sorption capabilities for Pb^2＋, Cd^2＋, Cu^2＋ and Zn^2＋ are compared. The experimental results show that the Zn^2＋ removal efficiency decreases gradually with the increase of the Cd^2＋ concentration of the solution, and there is no sorption preference between Cd^2＋ and Zn^2＋. On the other hand, the Zn^2＋ removal efficiency rapidly decreases rapidly with the increase of the Cu^2＋ concentration of the solution, and there is a clear sorption preference between Cu^2＋ and Zn^2＋. It is noticed that the Zn^2＋ removal efficiency is hardly changed with the variance of Pb^2＋ concentration because the removal mechanisms for these two ions are totally different. It is concluded that the adsorption affinities of the heavy metals for the hydroxyapatite follows this sequence： pb^2＋〉 Cu^2＋〉 Cd^2＋〉 Zn^2＋.  相似文献   

5.
This study analyzed the concentrations and chemical forms of Zn,Cu,Pb,Sb,Cd and Mn in airborne particles,road dusts and soils collected along three expressways in Jiangxi Province,China,with different traffic densities,and identified the levels and sources of heavy metal contamination.The concentrations of Zn,Cu,Pb,Sb,and Cd except Mn in airborne particles,road dusts and soils were all in direct proportion to traffic volume.Cd concentrations were low compared with other metals.For instance,the concentrations of Zn,Cu,Pb,Sb,Mn and Cd were 6.6,0.7,2.2,0.1,0.1 and 0.1μg·m-3in PM10along the Changjiu Expressway,792.8,241.4,248.3,9.6,340.5and 8.0 mg·kg-1in road dusts,and 201.1,143.2,59.5,9.5,338.9 and 2.3 mg·kg-1in soils,respectively,but in the case of the ratio of concentration to the environmental background value,most serious contamination was caused by Cd.The sources of the heavy metals were judged by comparisons of the chemical forms of the heavy metals in different environmental media.Pb and Mn in airborne particles were both derived from traffic;Pb in road dusts and soils resulted mainly from the use of leaded gasoline in the past;and Mn in road dusts and soils was derived from parent rocks.Zn,Cu,Sb and Cd in airborne particles,road dusts and soils were derived primarily from traffic,and differences in chemical forms of the heavy metals in different media were due to the interaction between heavy metals in airborne particles and organic matter and other surfaces in road dusts and soils.We also discussed the change of chemical forms of heavy metals in particles of different sizes and under different weather conditions.Bioavailability of heavy metals in airborne particles was much higher than that in road dusts and soils,especially Pb(0.676 in airborne particles,0.159 in road dusts and 0.095 in soils).  相似文献   

6.
The spatial distributions of contaminant metals (Hg, Pb, Zn, Cd, Cu) and a metalloid (As) in vegetable plots and paddy fields located near a large scale Pb/Zn smelter in Hunan province, China, were investigated. Soil located 4 km from the smelter was severely contaminated, with maximum concentrations of Hg, Pb, Zn, Cd, Cu and As as high as 2.89, 1200, 3350, 41.1, 157 and 93 mg kg−1, respectively. Concentrations of soil metal and As decreased with distance in the dominant wind direction. Single-factor assessment indicated pollution levels of Hg, Pb, Zn and Cd were most severe, while pollution levels for Cu and As were less severe. Results from a potential ecological risk assessment indicated high risk associated with the soil within a 4 km radius, with the contribution for each contaminant calculated as follows: Cd (70.0%), Hg (19.4%), Pb (4.8%), As (3.0%), Cu (1.7%) and Zn (1.1%). The forest soil in the nearby city park was also affected by the atmospheric depositions from smelting activities. Soil profiles demonstrated the pollutants were mostly accumulated in the upper 20 cm layer. Contamination of the topsoil with Hg, Pb, Zn, Cd, Cu and As indicated remediation should be considered.  相似文献   

7.
The complexation of Cu and Cd by ligands observed in filtered unfractionated lakewaters is compared to the complexation by humic and fulvic acids. Complexation parameters (conditional stability constants and ligand concentrations) of Suwannee River fulvic acids (FA), purified peat humic acids (HA) and of ligands in lakewater samples have been determined using the same methods (ligand-exchange and CSV (cathodic stripping voltammetry) or ASV (anodic stripping voltammetry)), and the same titration ranges of Cu, Cd and organic carbon concentrations. The performance of the used techniques is first evaluated in FA and HA suspensions, and gives comparable results with the literature values for the same materials, according to published models (5-site model, NICA model) and parameters. Model calculations using the WHAM model for FA and HA (Tipping, 1994) are also presented. The comparison of titrations of FA and HA with Cu and Cd with those of lakewater samples indicates that stronger ligands than FA and HA are present at low concentrations in the lakewaters. Specific strong ligands occur in particular in eutrophic lake waters, whereas in a lake with higher metal concentrations and low biological productivity the ligands more closely match the fulvic acid characteristics.  相似文献   

8.
Different plant communities have established spontaneously on Sanmen Pb/Zn mine tailing. The site was inspected and four different plant communities were identified according to their species composition. To understand the effects of different communities on mine tailing physico-chemical properties, a community survey was carried out in Sanmen Pb/Zn mine tailing, and the physico-chemical properties and heavy metal (Cu, Pb, Cd and Zn) distribution of mine tailings were determined. Results showed that there were four types of communities (I, II, III and IV) in Sanmen Pb/Zn mine tailing. From community I to IV, the number of plant species and community characteristics (aboveground biomass, underground biomass, coverage and height) consistently increased. Moreover, the nutrient pool and physico-chemical properties of mine tailing consistently reestablished from community I to IV, while the total heavy metal content consistently decreased. The contents of residual fractions, Fe–Mn oxide fractions for Pb, Zn, Cu and Cd and exchangeable fractions for Pb and Zn also consistently decreased. However, the contents of organically bound fraction had no obvious change from community I to IV. Moreover, the contents of Cu organically bound fraction reversely increased. Results demonstrate that communities I, II, III and IV should be a progressive community succession. Moreover, along with the progressive community succession, phytostabilization and phytoextraction of mine tailings are more and more effective.  相似文献   

9.
 The potential use of treated solid by-product of oil shale to treat aqueous solutions containing several heavy metals, i.e., Cd(II), Cu(II), Cr(III), Ni(III), Pb(II) and Zn(II), was explored. Different experimental approaches including equilibrium batch mode experiments and X-ray fluorescence (XRF) were used to explore the feasibility of this material as a cheap adsorbent for the removal of these heavy metals from predetermined solutions. Results indicate that the solid by-product of oil shale removes Cd(II), Cu(II), Ni(II), and Pb(II), from aqueous solutions by adsorption, but did not remove the other heavy metals investigated in this study. Received: 20 April 1998 · Accepted: 20 November 1998  相似文献   

10.
Sixty-two soil samples collected from different functional zones of Guiyang were analyzed for total concentrations and sequential extraction of Cr, Cu, Pb, Zn and Cd by ICP spectrometry. The average total concentrations ofCr, Cu, Pb, Zn and Cd in the soils of Guiyang were 92.9, 51.6, 44.1,139.3 and 0.28 mg/kg, respectively. The soils have been polluted by Cr, Cu, Pb, Zn and Cd to some extent in comparison with the background values of Guiyang. Significant differences were recognized in the concentrations of Cr, Cu, Pb, Zn and Cd in different functional zones. As for the sequential extraction, Cr, Cu and Zn were present mainly in the residual fraction, and Pb was present mainly in the oxidizable fraction. The reducible fraction of Cd accounts for 47.5%, and the residual fraction is lowest. The mobility and bioavailability of heavy metals follow the order of Cd〉Pb〉Cu〉Cr〉Zn.  相似文献   

11.
《Applied Geochemistry》1998,13(3):359-368
Studies on the speciation (particulate, colloidal, anionic and cationic forms) of trace metals (Cd, Co, Cu, Fe, Mn, Mo, Ni, Pb, Zn) in the water column and in pore waters of the Gotland Deep following the 1993/94 salt-water inflows showed dramatic changes in the total “dissolved” metal concentrations and in the ratios between different metal species in the freshly re-oxygenated waters below 125 m. Changes in concentrations were greatest for those metals for which the solubility differs with the redox state (Fe, Mn, Co) but were also noted for those metals which form insoluble sulphides (Cd, Pb, Cu, Zn) and/or stable complexes with natural ligands (Cu). Pore water data from segmented surface muds (0–200 mm) indicated that significant redox and related metal speciation changes took place in the surface sediments only a few weeks after the inflow of the oxygenated sea water into the Gotland Deep.  相似文献   

12.
Conditional surface binding constants and complexation capacities for Zn, Pb, Cd, and Cu were determined from surface titration experiments of heterogeneous natural aquatic particulate matter of different origin and composition. Metals and particles were evaluated in naturally occurring concentration ranges in river water.The adsorption of trace metals can be adequately described with a single conditional binding constant over a wide range of metal : particle ratios. Binding constants for aquatic particles at pH 8.0 are remarkably independent from particle composition and are specific for each metal: log Kads Zn = 8.39, log Kads Pb = 9.67, log Kads Cd = 8.61, log ads Cu = 9.84. From competition experiments with Ca and Pb we extracted a sorption coefficient for Ca of log Kads Ca = 2.5 (pH 8.0). Maximum surface binding capacities for all metal ions were found for particles containing high fractions of Mn-oxides which are associated with large specific surface areas. Generally, we found sorption capacities to decrease in the sequence Cu Pb, Zn > Cd.The experiments suggest that the conditional surface binding constants and complexation capacities are applicable to model trace metal adsorption in the concentration ranges of natural waters under conditions similar to the experiments. Results also imply that the chemical nature of particle surface sites is rather uniform in the intermediate concentration range or that the array of binding sites averages out differences in sorption strength over the prevailing concentration range of metal ions, respectively.  相似文献   

13.
Eleven surface soil samples from calcareous soils of industrial areas in Hamadan Province, western Iran were analyzed for total concentrations of Zn, Cd, Ni, Cu and Pb and were sequentially extracted into six fractions to determine the bioavailability of various heavy metal forms. Total Zn, Cd, Ni, Cu and Pb concentrations of the contaminated soils were 658 (57–5,803), 125.8 (1.18–1,361), 45.6 (30.7–64.4), 29.7 (11.7–83.5) and 2,419 (66–24,850) mg kg−1, respectively. The soils were polluted with Zn, Pb, and Cu to some extent and heavily polluted with Cd. Nickel values were not above regulatory limits. Copper existed in soil mainly in residual (RES) and organic (OM) fractions (about 42 and 33%, respectively), whereas Zn occurred essentially as RES fraction (about 69%). The considerable presence of Cd (30.8%) and Pb (39%) in the CARB fraction suggests these elements have high potential biavailability and leachability in soils from contaminated soils. The mobile and bioavailable (EXCH and CARB) fractions of Zn, Cd, Ni, Cu, and Pb in contaminated soils averaged (7.3, 40.4, 16, 12.9 and 40.8%), respectively, which suggests that the mobility and bioavailability of the five metals probably decline in the following order: Cd = Pb > Ni > Cu > Zn.  相似文献   

14.
基于地统计学和GIS相结合的方法,对承德全域表层土壤重金属As、Cd、Cr、Cu、Hg、Ni、Pb、Zn、微量元素Se正态分布特征、主导分布趋势及相互作用规律进行了分析,确定了不同元素最适宜的地统计插值模型并厘定出其空间分布规律。结果表明:As、Cd、Cr、Cu、Hg、Ni、Pb、Zn的质量含量平均值分别为8.28,0.200,60.85,24.37,0.034,27.76,26.65,77.10 mg/kg,Cd、Cu、Hg和Pb变异系数分别为385%、143%、350%、118%,分异性强。Zn含量均值受土壤类型影响显著,Cr、Cu、Ni含量均值则受土地利用类型影响显著。经过不同趋势阶数元素插值误差的综合对比,确定As、Cr、Pb、Zn、Ni、Se适宜选择无趋势参数,Hg和Cu适宜选择一阶趋势参数,而Cd适宜选择二阶趋势参数。As的理论模型为指数模型,主要受到结构性因素的影响;Cd、Cr、Cu、Hg、Ni、Pb、Zn、Se的理论模型为线性模型,主要受到随机性因素的影响。通过普通克里格插值图可见区内9种元素具有北低南高的特点,中部地区形成了一条较宽的Pb高值带,与Cd相似。按照含量分布特点,土壤中Cr和Ni、Cu和Hg、Zn和Pb、Se和Cd之间的高值空间展布区具有相似性且来源相同,仅As具有个性,分析结果与传统统计学结果数据保持部分一致性。  相似文献   

15.
Amorphous tin(VI) hydrogen phosphate (ATHP) was synthesized using the liquid phase precipitation method and served as an adsorbent to remove Pb(II), Cu(II), and Zn(II) from aqueous solutions. The ATHP was characterized by powder X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and nitrogen adsorption–desorption techniques. Adsorption properties were evaluated as a function of pH, reaction time, concentration of reactants, and salinity. Their equilibrium adsorption data were modeled using Freundlich, Langmuir, and Dubinin–Kaganer–Radushkevich isotherms, respectively. The results revealed that adsorption equilibrium reached within 180 min. ATHP indicated good adsorption even below the pHZPC, and best adsorption at pH 5 for Pb(II) and Cu(II) and at pH 5.5 for Zn(II) was observed. Equilibrium data fitted better to the Langmuir model for Pb(II) and Cu(II) and fitted better to the Freundlich model for Zn(II). The saturated adsorption capacities deduced from the Langmuir model were 2.425, 1.801, and 0.600 mmol/g for Cu(II), Pb(II), and Zn(II), respectively, indicating an adsorption affinity order of Cu > Pb > Zn. There is a negative correlation between the concentration of NaCl and adsorption capacity of ATHP, yet ATHP still exhibited excellent adsorption having an adsorption capacity of 19.35, 15.16, 6.425 mg/g when the concentration of NaCl was 0.6 mol/L. The free energy (E) was 12.33, 10.70, and 14.74 kJ/mol for Pb(II), Cu(II), and Zn(II), respectively. An adsorption mechanism based on ion exchange between heavy metal ions and H+ in the ATHP is proposed. Furthermore, the used ATHP was regenerated by HCl solution and the adsorbent was used repeatedly.  相似文献   

16.
南京市大气降尘重金属含量特征及来源研究   总被引：19，自引：0，他引：19  
文中对南京市大气降尘重金属含量水平进行了研究,从2006年12月起连续收集一年的大气降尘样品,分析了As、Cd、Cr、Cu、Hg、Mn、Mo、Ni、Pb、Se、Zn等11个元素。结果表明,与土壤背景值相比,南京市大气降尘中除Cr、Fe、Mn外的重金属含量总体明显升高。采用相关分析和主成分分析,对降尘重金属元素来源进行解析,认为有三种主要来源:一是As、Cu、Hg、Pb、Se与燃煤活动、汽车尾气排放有关。二是Cd、Ni、Zn、Mo可能与化学工业有关,但Mo还受工业活动、土壤颗粒物的影响。分析还表明,在化工业园附近的样点,这些元素含量普遍较高。三是Mn、Cr主要与土壤颗粒物有关(自然来源)。以Fe作为参考元素计算重金属的富集因子表明,自然来源的Cr、Mn具有较小的富集因子,而受工业活动影响的Cd、Pb、Se、Zn具有较大的富集因子。  相似文献   

17.
In the aquatic system, heavy metals always exist in a number of physico-chemical forms: particulate (Cp), soluble which consists of labile (MALI) and bound (inorganic MAb and organic MLb). The environmental behaviors of a metal are critically dependent on these forms. In this paper, the forms of heavy metals in waters from the Changjiang River source to mainstream and lakes were determined by ASV method. The main results are as follows: 1. The total contents (Ct) of Zn, Pb, Cu and Cd in the source were 4.0, 1.88, 1.28 and 0.07 (g/L) respectively, while Ct (g/L) in the mainstem were in the order of Zn (20.1) > Cu (14.9) > Pb (6.73) > Cd (0.15). Ct (g/L) in Dianchi Lake were Zn (7.2) > Pb (0.72) > Cu (0.53) > Cd (0.05), and in Poyang Lake were Zn (12.5) > Pb (4.2) > Cu (3.4) > Cd (0.05), and in Poyang Lake were Zn (12.5) > Pb (4.2) > Cu (3.4) > Cd (0.05). However, most of them were presented as Cp. Their dissolved contents (Cs, /L) were lower. 2. The distribution of soluble forms was related to the type of metal and to environmental variables. In general, Zn and Cd have a tendency to be present in MALi, Pb in MAb and Cu in MLb.  相似文献   

18.
 The Yamuna River sediments, collected from Delhi and Agra urban centres, were analysed for concentration and distribution of nine heavy metals by means of atomic adsorption spectrometry. Total metal contents varied in the following ranges (in mg/kg): Cr (157–817), Mn (515–1015), Fe (28,700–45,300), Co(11.7–28.4), Ni (40–538), Cu (40–1204), Zn (107–1974), Pb (22–856) and Cd (0.50–114.8). The degree of metal enrichment was compared with the average shale concentration and shows exceptionally high values for Cr, Ni, Cu, Zn, Pb and Cd in both urban centres. In the total heavy metal concentration, anthropogenic input contains 70% Cr, 74% Cu, 59% Zn, 46% Pb, 90% Cd in Delhi and 61% Cr, 23% Ni, 71% Cu, 72% Zn, 63% Pb, 94% Cd in Agra. A significant correlation was observed between increasing Cr, Ni, Zn, and Cu concentrations with increasing total sediment carbon and total sediment sulfur content. Based on the Müller's geoaccumulation index, the quality of the river sediments can be regarded as being moderately polluted to very highly polluted with Cr, Ni, Cu, Zn, Pb and Cd in the Delhi and Agra urban centres. The present sediment analysis, therefore, plays an important role in environmental measures for the Yamuna River and the planning of these city centres. Received: 21 June 1999 · Accepted: 1 October 1999  相似文献   

19.
A total of 29 surface sediments were collected from the Daihai Lake, China. Concentrations of metals (Cu, Pb, Zn, and Cd) were determined using HR-ICP-MS after digestion with the mixture of HNO3–HF–HCl (aqua regia), and chemically fractionated according to the modified the European Community Bureau of Reference sequential extraction procedure. Total organic carbon contents and grain size were also analyzed. Average concentrations (ppm) for Cu (39.4 ± 10.6), Pb (29.9 ± 6.1), Zn (102.6 ± 23.3), and Cd (0.21 ± 0.07) were found in the sediments. The concentrations of metals are relatively higher in the central area of lake, while lower nearby the area with a shallower water depth. Sequential extraction results show that Cu and Zn are mainly distributed in the residual fraction, while Cd is dominantly in the non-residual fraction. Enrichment factor values and geoaccumulation indexes suggest that there are not obvious enrichments of Cu, Pb, and Zn in the sediments, but Cd pollution can be found in most of the area of Daihai Lake. The sources for Cu, Pb, and Zn are attributed to atmospheric deposition, which might be mainly associated with coal combustion. Agricultural runoff in polluted soils and coal combustion might be main sources of the Cd pollution in the lake.  相似文献   

20.
《Applied Geochemistry》2001,16(9-10):1067-1082
Thermodynamic data for all fate-determining processes are needed in order to predict the fate and transport of metals in natural systems. The surface complexation properties of a synthetic MnO2, δ-MnO2, have accordingly been investigated using glass electrode potentiometry. Experimental data were interpreted according to the surface complexation model in conjunction with the diffuse double layer model of the solid/solution interface. Adsorption constants were determined using the non-linear optimisation program FITEQL. Surface complexation parameters determined in this way were validated against results obtained from the literature. Best fits of alkalimetric titration data were obtained with a 2-site, 3 surface-species model of the δ-MnO2 surface. Site concentrations of 2.23×10−3 mol g−1 and 7.66×10−4 mol g−1 were obtained. Corresponding logarithms of formation constants for the postulated surface species are −1.27 (≡XO−), −5.99 (≡YO−) and 3.52 (≡YOH2+) at I=0.1 M. The surface speciation of δ-MnO2 is dominated by ≡XO− over the pH range investigated. Metal adsorption was modelled with surface species of the type ≡XOM+, ≡XOMOH, ≡YOM+, ≡YOMOH (M=Cu, Ni, Zn, Cd and Pb) and ≡XOM2OH2+ (M=Pb). For Cu, Ni and Zn, titration data could be modelled with ≡XOM+, ≡XOMOH, ≡YOM+ and ≡YOMOH, whereas for Cd, ≡XOM+ and ≡YOM+ were sufficient. Lead data were best modelled by assuming the dinuclear species ≡XOM2OH2+ to be the only surface species to form. Adsorption constants determined for Ni, Cu and Zn follow the Irving-Williams sequence. The model suggests an adsorption order of (Pb, Cu) > (Ni, Zn) > Cd. The discrepancy between model predictions and published adsorption results is similar to the variability observed in experimental results from different laboratories.  相似文献   

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