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1.
We examined the uptake of ligand-bound metals (Cd and Zn) by the green mussel Perna viridis using defined artificial seawater. Different free ion concentrations (1 pM to 10 microM) in uptake solutions were created by adding different amounts of total metals (Cd 0.1 nM to 0.1 mM; Zn 0.5 nM to 0.05 mM) and ligands (EDTA, NTA, citric acid). Our results showed that Cd and Zn uptake could not be fully explained by the free Cd and Zn concentrations in the presence of different ligands, indicating that metal-ligand complexes were at least partially available for uptake by the mussels. Total Zn concentrations appeared to be a better predictor of metal uptake than the free Zn ion concentrations in the presence of different ligands. Uptake of lipophilic organic metal complexes was substantially greater than the hydrophilic metal complexes, even though the free ion concentration was comparable or lower. Moreover, the radiolabeled ligand compounds were directly accumulated by the mussels. The accumulation of metal complexes may explain the increased metal uptake with increasing ligand and total metal concentration, even though the free ion metal concentration was constant. Overall, our experimental results indicated that free metal ion cannot fully explain metal uptake since metal complex species were also available to the mussels to some extent, apparently through a co-transport process.  相似文献   

2.
The presence of dissolved organic matter (DOM), as humic acids (HA), in natural waters is assumed to decrease dissolved metal bioavailability by binding metal ions and, therefore, decreasing the free ion concentration in solution. In this study, Pb complexation by HA in artificial seawater was checked by means of square wave anodic stripping voltammetry (SWASV). Uptake and toxicity of this metal in the absence and presence of HA was tested using excised gills of Mytilus edulis and the Paracentrotus lividus embryo-larval bioassay respectively. Both Pb uptake by mussel gills and Pb toxicity to sea urchin larvae increased in the presence of HA, and this increase was higher at higher HA concentrations. Since it is shown that the presence of DOM can enhance the uptake and toxicity of lead in some important marine invertebrate species, these results challenge the general applicability of the free ion activity and related models used for deriving environmental water quality criteria for metals.  相似文献   

3.
Labile Cd complexes increase Cd availability to plants   总被引:2,自引:0,他引:2  
Dissolved trace metals are present in the environment as free ions and as complexes. Commonly used models to predict metal bioavailability consider the free ion as the major bioavailable species. However, increases in metal availability in the presence of metal complexes have repeatedly been found. We measured the uptake of cadmium (Cd) by spinach (Spinacia oleracea) from solution in absence or presence of synthetic ligands. At the same free ion concentration, the uptake of Cd ranged over almost 3 orders of magnitude and was largest in treatments with fast dissociating (i.e. labile) complexes. Similar results were found for the diffusional fluxes in these solutions, as measured with the DGT technique. The observed effect of Cd complexes on the plant uptake was in agreement with model calculations in which plant uptake was assumed to be governed by the diffusional flux. These results strongly suggest that Cd uptake is rate-limited by diffusion of the free ion to the root surface, even in stirred solutions. As a result, dissolved Cd complexes can increase Cd uptake, resulting in apparent exceptions from the free ion activity model. The magnitude of this increase depends both on the concentration and on the lability of the complexes. The free ion concept should therefore be reconsidered when transport limitations of the metal ion to the uptake site prevail.  相似文献   

4.
Dissolved organic matter (DOM) is generally thought to lower metal bioavailability in aquatic systems due to the formation of metal-DOM complexes that reduce free metal ion concentrations. However, this model may not be pertinent for metal nanoparticles, which are now understood to be ubiquitous, sometimes dominant, metal species in the environment. The influence of DOM on Hg bioavailability to microorganisms was examined under conditions (0.5-5.0 nM Hg and 2-10 μM sulfide) that favor the formation of β-HgS(s) (metacinnabar) nanoparticles. We used the methylation of stable-isotope enriched (201)HgCl(2) by Desulfovibrio desulfuricans ND132 in short-term washed cell assays as a sensitive, environmentally significant proxy for Hg uptake. Suwannee River humic acid (SRHA) and Williams Lake hydrophobic acid (WLHPoA) substantially enhanced (2- to 38-fold) the bioavailability of Hg to ND132 over a wide range of Hg/DOM ratios (9.4 pmol/mg DOM to 9.4 nmol/mg DOM), including environmentally relevant ratios. Methylmercury (MeHg) production by ND132 increased linearly with either SRHA or WLHPoA concentration, but SRHA, a terrestrially derived DOM, was far more effective at enhancing Hg-methylation than WLHPoA, an aquatic DOM dominated by autochthonous sources. No DOM-dependent enhancement in Hg methylation was observed in Hg-DOM-sulfide solutions amended with sufficient l-cysteine to prevent β-HgS(s) formation. We hypothesize that small HgS particles, stabilized against aggregation by DOM, are bioavailable to Hg-methylating bacteria. Our laboratory experiments provide a mechanism for the positive correlations between DOC and MeHg production observed in many aquatic sediments and wetland soils.  相似文献   

5.
In the analysis of metal biouptake from complexing environments, both chemical speciation and biological uptake characteristics have to be taken into account. The commonly used free ion activity model is based on equilibrium speciation and implies that diffusion of the bioactive free metal toward the organism is not rate-limiting. In the presence of complexes, however, sufficiently labile species might contribute to the biouptake via preceding dissociation. Coupling of the ensuing diffusional mass transfer flux of metal with the biouptake flux of free metal, the supposedly bioactive species, shows under which conditions labile metal complexes can contribute to the uptake. The goal of the present paper is to apply this type of analysis to experimental data on metal uptake by mussel (Mytilus edulis) and carp (Cyprinus carpio) in complexing environments. These biosystems have fairly well-characterized uptake parameters, but the uptake fluxes cannot be fully explained by considering equilibrium speciation only. For Zn(II) uptake by mussel, evidence was found for diffusional limitation at low concentrations, whereas for Cd(III) uptake by carp, diffusion is not limiting at all. The analysis provides an example of how a more comprehensive treatment of complex systems can be applied to real experimental data.  相似文献   

6.
Partition coefficients of two estrogenic compounds, 17beta-estradiol (E2) and p-nonylphenol (NP), between synthetic membrane vesicles (K'lipw values) and water were determined using equilibrium dialysis to evaluate the potential biological uptake of these compounds with and without the presence of dissolved natural organic matter (DOM) surrogates, Suwannee River fulvic acid, dialyzed Aldrich humic acid, and polyphenolic tannic acid. Overall, K'lipw values for E2 and NP reduced by 20-30% with the increase of DOM concentration from 0 to approximately 4 mg of C/L, a typical DOM concentration in the aquatic environment. This trend for E2 and NP is similar to that obtained by other researchers for moderately hydrophobic compounds including polycyclic aromatic hydrocarbons with three or four rings. A three-phase compartment model with three independent interactions, the sorption of E2 or NP by DOM surrogate (Koc), the sorption of DOM surrogates by membrane vesicles (KlipDOM), and the partition of E2 or NP by membrane vesicles (Klipw), was proposed, and K'lipw values for E2 or NP in the presence of DOM were calculated. The model predicted the decrease in Klipw values with the increase of DOM concentration, and the predictions using the three linear interactions agreed satisfactorily with the experimental results at relatively lower concentration of DOM.  相似文献   

7.
The complexation of heavy metals with dissolved organic matter (DOM) in the environment influences the solubility and mobility of these metals. In this paper, we measured the complexation of Cu, Cd, Zn, Ni, and Pb with DOM in the soil solution at pH 3.7-6.1 using a Donnan membrane technique. The results show that the DOM-complexed species is generally more significant for Cu and Pb than for Cd, Zn, and Ni. The ability of two advanced models for ion binding to humic substances, e.g., model VI and NICA-Donnan, in the simulation of metal binding to natural DOM was assessed by comparing the model predictions with the measurements. Using the default parameters of fulvic and humic acid, the predicted concentrations of free metal ions from the solution speciation calculation using the two models are mostly within 1 order of magnitude difference from the measured concentrations, except for Ni and Pb in a few samples. Furthermore, the solid-solution partitioning of the metals was simulated using a multisurface model, in which metal binding to soil organic matter, dissolved organic matter, clay, and iron hydroxides was accounted for using adsorption and cation exchange models (NICA-Donnan, Donnan, DDL, CD-MUSIC). The model estimation of the dissolved concentration of the metals is mostly within 1 order of magnitude difference from those measured except for Ni in some samples and Pb. The solubility of the metals depends mainly on the metal loading over soil sorbents, pH, and the concentration of inorganic ligands and DOM in the soil solution.  相似文献   

8.
To determine whether preexposure of green mussel Perna viridis to Ag influenced metal uptake kinetics we compared various physiological indicators of metal uptake kinetics between the control mussels and mussels preexposed to Ag in both diet and water at different levels (up to 5 weeks). In all preexposed mussels, the assimilation of Ag increased by 1.1-3.0 times with increasing Ag body concentration (0.651-19.3 microg g(-1)) as compared with the controls (Ag body concentration of 0.311-0.479 microg g(-1)), whereas the efflux rate constants decreased by 45-88%. There was no significant increase in Ag associated with the metallothionein-like protein (MTLP) fraction following exposure of the mussels to Ag through either the dissolved or food phase. The clearance rates were little affected or depressed byAg preexposure, and the relationship between the Ag influx rate from the dissolved phase and the Ag preexposure was somewhat complicated. The influx rate decreased with increasing Ag body burden at <2.5 microg g(-1), above which it increased with increasing Ag body burden. Our results indicate that the mussels may modify physiological processes to ambient chronic Ag exposure, consequently accumulating more Ag. Ag body concentration in these mussels may therefore increase disproportionally in response to increasing Ag concentration in the ambient environments. Ag preexposure and resulting body burden should be considered carefully when interpreting the observed Ag concentration in biomonitoring animals to evaluate the Ag pollution in seawater.  相似文献   

9.
Adsorption to dissolved organic matter (DOM) may significantly decrease the freely dissolved concentration of many hydrophobic organic compounds and, hence, result in reduced bioavailability to aquatic organisms. Here, the suitability of using triolein-embedded cellulose acetate membrane (TECAM) as a biomimetic surrogate to assess the bioavailability of organochlorine pesticides (OCPs) in water in the presence of DOM was explored. The accumulation of OCPs was measured in TECAM and pelagic Japanese medaka (Oryzias latipes) in the laboratory after 12 h exposure to water containing different levels of Aldrich humic acid. Further, OCP uptake by TECAM and medaka in real aqueous environments was evaluated after 30 d exposures in two sites. Laboratory results showed that OCP uptake by medaka consistently decreased with increasing levels of humic acid in the range of 0-15 mg C/L in sample solutions. This tendency was closely mimicked by OCP accumulation in TECAM under the same conditions. Field results showed that TECAM accumulated similar OCP patterns as medaka (r2 = 0.92 for site 1 and r2 = 0.94 for site 2), although comparison of the in-field eight OCP concentrations in TECAM to those in medaka yielded approximately a factor of 3 (on a wet weight basis). These results suggest that the TECAM method can be used as a simple and useful tool to predict the bioavailability and bioaccumulation potential of poorly biotransformed organic compounds in pelagic fish in aqueous environment.  相似文献   

10.
The widespread invasion of freshwaters by the zebra mussel, Dreissena polymorpha, during the last 2 decades has made it one of the world's most economically and ecologically important pests. Since arriving in the North American Great Lakes in the 1980s, zebra mussels have become a major biofouler, blocking the raw water cooling systems of power stations and water treatment works and costing U.S. dollars 1-5 billion per year. Despite the development of numerous control methods, chlorination remains the only widespread and licensed technique. Zebra mussels are able to sense chlorine and othertoxins in their surrounding environment and respond by closing their valves, thus enabling them to avoid toxic effects for up to 3 weeks. Furthermore, prolonged dosing of chlorine in raw water produces ecotoxic trihalomethanes (THMs) by reaction with organic material in the water. We have developed a novel, environmentally safe, and effective method for controlling the zebra mussel: the BioBullet. Our method uses the encapsulation of an active ingredient (KCI) in microscopic particles of edible material. The mussels' natural filtering ability then removes and concentrates the particles from the water, without stimulating the valve-closing response. By using the mussels' filtering behavior to concentrate BioBullets the absolute quantity of active ingredient added to the water can be reduced substantially. Our approach allows us to engineer the particles to break up and dissolve completely within a few hours, thus eliminating the risk of polluting the wider ecosystem. We demonstrate that the effectiveness of a toxin in the control of biofouling filter-feeders can be enhanced greatly by using our technique. This paves the way for a new approach to the control of some of the world's most important economic pests.  相似文献   

11.
Dissolved organic matter (DOM) in surface waters affects the fate and environmental effects of trace metals. We measured variability in the Cd, Cu, Ni, and Zn affinity of 23 DOM samples isolated by reverse osmosis from freshwaters in natural, agricultural, and urban areas. Affinities at uniform pH and ionic composition were assayed at low, environmentally relevant free Cd, Cu, Ni, and Zn activities. The C-normalized metal binding of DOM varied 4-fold (Cu) or about 10-fold (Cd, Ni, Zn) among samples. The dissolved organic carbon concentration ranged only 9-fold in the waters, illustrating that DOM quality is an equally important parameter for metal complexation as DOM quantity. The UV-absorbance of DOM explained metal affinity only for waters receiving few urban inputs, indicating that in those waters, aromatic humic substances are the dominant metal chelators. Larger metal affinities were found for DOM from waters with urban inputs. Aminopolycarboxylate ligands (mainly EDTA) were detected at concentrations up to 0.14 μM and partly explained the larger metal affinity. Nickel concentrations in these surface waters are strongly related to EDTA concentrations (R2=0.96) and this is underpinned by speciation calculations. It is concluded that metal complexation in waters with anthropogenic discharges is larger than that estimated with models that only take into account binding on humic substances.  相似文献   

12.
The capability of three dimensionally ordered macroporous (3DOM) hydroxyapatite, Ca10(PO4)6(OH)2 (HAp), to capture cadmium and lead ions from their respective salt solutions was studied as a function of temperature. Synthesis of 3DOM material was achieved by colloidal crystal templating of polystyrene spheres (1 microm diameter) using calcium nitrate (Ca(NO3)2) and orthophosphoric acid (H3PO4) as precursors. The macroporous product consisted primarily of HAp (>80% depending on the sintering temperature) together with amorphous calcium phosphate. The sorption ability of 3DOM material to Cd/Pb ion was benchmarked against HAp powder prepared via the same route without the template. On the basis of quantitative X-ray diffraction (XRD) and analytical transmission electron microscopy(ATEM) 3DOM HAp demonstrated a higher uptake of cadmium, viz. x = 0.71 in Ca10-xCdx(PO4)6(OH)2 than nonporous HAp (x = 0.42). The incorporation of Cd was homogeneous in the 3DOM HAp crystals (as compared to the powder) leading to a decrease in lattice parameters as Cd2+ has a smaller ionic radius compared to Ca2+. A preference for Cd to enter the Ca" tunnel site of HAp was consistent with this being the readily exchangeable site. The lead-bearing solution acted to collapse the macropores through the rapid crystallization of pyromorphite (Pb10(P04)6(OH)2) via a dissolution-precipitation mechanism, possibly promoted by the amorphous component, that overwhelmed HAp ion exchange. The rapid crystallochemical incorporation of Cd and fixation of Pb by 3DOM HAp demonstrates the potential of thin-walled porous structures for the treatment of contaminated waters.  相似文献   

13.
The biotic ligand model (BLM) is a mechanistic approach that greatly improves our ability to generate site-specific ambient water quality criteria (AWQC)for metals in the natural environment relative to conventional relationships based only on hardness. The model is flexible; all aspects of water chemistry that affect toxicity can be included, so the BLM integrates the concept of bioavailability into AWQC--in essence the computational equivalent of water effect ratio (WER) testing. The theory of the BLM evolved from the gill surface interaction model (GSIM) and the free ion activity model (FIAM). Using an equilibrium geochemical modeling framework, the BLM incorporates the competition of the free metal ion with other naturally occurring cations (e.g., Ca2+, Na+, Mg2-, H+), togetherwith complexation by abiotic ligands [e.g., DOM (dissolved organic matter), chloride, carbonates, sulfide] for binding with the biotic ligand, the site of toxic action on the organism. On the basis of fish gill research, the biotic ligands appear to be active ion uptake pathways (e.g., Na+ transporters for copper and silver, Ca2+ transporters for zinc, cadmium, lead, and cobalt), whose geochemical characteristics (affinity = log K, capacity = Bmax) can be quantified in short-term (3-24 h) in vivo gill binding tests. In general, the greater the toxicity of a particular metal, the higher the log K. The BLM quantitatively relates short-term binding to acute toxicity, with the LA50 (lethal accumulation) being predictive of the LC50 (generally 96 h for fish, 48 h for daphnids). We critically evaluate currently available BLMs for copper, silver, zinc, and nickel and gill binding approaches for cadmium, lead, and cobalt on which BLMs could be based. Most BLMs originate from tests with fish and have been recalibrated for more sensitive daphnids by adjustment of LA50 so as to fit the results of toxicity testing. Issues of concern include the arbitrary nature of LA50 adjustments; possible mechanistic differences between daphnids and fish that may alter log K values, particularly for hardness cations (Ca2+, Mg2+); assumption of fixed biotic ligand characteristics in the face of evidence that they may change in response to acclimation and diet; difficulties in dealing with DOM and incorporating its heterogeneity into the modeling framework; and the paucity of validation exercises on natural water data sets. Important needs include characterization of biotic ligand properties at the molecular level; development of in vitro BLMs, extension of the BLM approach to a wider range of organisms, to the estuarine and marine environment, and to deal with metal mixtures; and further development of BLM frameworks to predict chronic toxicity and thereby generate chronic AWQC.  相似文献   

14.
Sorption coefficients (K(oc) values) of selected endocrine disruptors for a wide variety of dissolved organic matter (DOM) were measured using fluorescence quenching and solubility enhancement. 17beta-Estradiol, estriol, 17alpha-ethynylestradiol, p-nonylphenol, p-tert-octylphenol, and dibutylphthalate were selected as endocrine disruptors. Aldrich humic acid, Suwannee River humic and fulvic acids, Nordic fulvic acid, alginic acid, dextran, and tannic acid were selected as DOM surrogates. The resulting sorption coefficients (log K(oc)) were independent of octanol-water partitioning coefficients (log K(ow)) of the selected endocrine disruptors, indicating the hydrophobic interaction is not the predominant sorption mechanism. Moreover, the K(oc) values for the selected endocrine disruptors, especially the steroid estrogens, correlated much better with UV absorptivity at 272 nm (A272) and phenolic group concentration of the DOM than with either the H/O or the (O+N)/C atomic ratio of the DOM. This suggests that the sorption mechanism is closely related to the interaction between pi-electrons and the hydrogen bonds, i.e., the affinity between phenolic groups of the steroid estrogens and DOM is suggested to provide a relatively large contribution to the overall sorption and yield the K(oc) values of the steroid estrogens as high as those of the alkylphenols and dibutylphthalate, which are suggested to be dominated by nonspecific hydrophobic interaction.  相似文献   

15.
The influence of water temperature on the adsorption of natural dissolved organic matter (DOM) on activated carbon has not been investigated intensively yet. In this study, batch experiments with granular activated carbon (GAC) have been carried out at three temperatures (5 degrees C, 20 degrees C, 35 degrees C) using a humic acid model water and different types of surface water (lake, river, canal). Furthermore, the adsorption of an anthropogenic contaminant, atrazine, was quantified in the absence and presence of DOM. The results indicate a significant influence of water temperature on the adsorption equilibrium of DOM and atrazine. Contrary to expectations, DOM and atrazine adsorption in surface water tends to be increased with increasing water temperature, whereas the extent of this effect is dependent on the type and concentration of DOM. Furthermore, the temperature effect on atrazine adsorption is controlled by competition of DOM and atrazine on adsorption sites. Some assumptions are proposed and discussed for explaining the temperature effects observed in the batch studies.  相似文献   

16.
In Chile, upwellings occur periodically along the coasts, resuspending metals from the seafloor and reintroducing them to the food web. Chilean blue mussels, Mytilus chilensis, accumulate these toxic compounds and show high concentrations of cadmium. An in vitro simulated digestion method has been applied to specimens of M. chilensis previously contaminated with 109Cd, to measure the bioaccessibility of cadmium for humans. The effects of the cooking process on the cadmium content of this species and on the resulting change in dietary bioaccessibility have also been evaluated. While cooking resulted in an increase in cadmium concentration in mussel flesh, cadmium remaining in the cooked flesh was also significantly less bioaccessible than cadmium occurring in the raw tissue. Estimations made in this study show that the intake of Cd from mussels by the Chilean population does not exceed the toxicological reference values established by the FAO/WHO; consequently, a health risk situation is not indicated.  相似文献   

17.
The present study examines the role of humic acid, as a representative of dissolved organic matter, in Cd(II), Cu(II), and Pb(II) speciation and biouptake by green microalgae. Cellular and intracellular metal fractions were compared in the presence of citric and humic acids. The results demonstrated that Cd and Cu uptake in the presence of 10 mg L(-1) humic acid was consistent with that predicted from measured free metal concentrations, while Pb biouptake was higher. By comparing Cd, Cu, and Pb cellular concentrations in the absence and presence of humic acid, it was found that the influence of the increased negative algal surface charge, resulting from humic acid adsorption, on cellular metal was negligible. Moreover, the experimental results for all three metals were in good agreement with the ternary complex hypothesis. Given that metal has much higher affinity with algal sites than humic acid adsorbed to algae, the contribution of the ternary complex to metal bioavailability was negligible in the case of Cd (II) and Cu (II). In contrast, the ternary complex contributed to over 90% of total cellular metal for Pb(II), due to the comparable affinity of Pb to algal sites in comparison with humic acid adsorbed to algae. Therefore, the extension of the biotic ligand model by including the formation of the ternary complex between the metal, humic acid, and algal surface would help to avoid underestimation of Pb biouptake in the presence of humic substances by green algae Chlorella kesslerii.  相似文献   

18.
The occurrence and composition of toxic algae, and presence of viruses and other human microbial pathogens in production areas of mussels are factors determining suitability of mussel products for human consumption. As bivalves feed by filtering large volumes of water, potentially toxic viruses, algae, and bacteria as well as phytoplankton are ingested. With the expansion of mussel aquaculture and subsequent increase in human consumption of mussel products, improved risk management is required for consumer protection. For example, shifting production to offshore areas (e.g. wind farms) can decrease the hazards of infection due to dilution of contaminants, and increase overall health of mussels. In addition, the deployment of off-bottom cultivation methods such as longlines increases the condition index, growth, and aesthetic appearance of mussels. However, other hazards like algal toxins not yet monitored on a regular basis, may play a more important rule offshore. Here, we present an analysis of biological, economic, and consumer health-related aspects of mussel cultivation under near- and offshore conditions.  相似文献   

19.
Metal ion toxicity is not simply related to the total concentration but to the free or labile metal ion concentration. One of the techniques that can measure the free metal ion concentration is the Donnan Membrane Technique (DMT). However, this method has limitations in terms of a relatively high detection limit (in relation to typical environmental concentrations) and a long equilibration time. We have therefore developed the Flux Donnan Membrane (FDM) Technique, which is a dynamic modification of the standard DMT with improved detection limits and a more rapid response. We show that experimental calibrations of metal ion transport in the FDM can be used to measure [M]free under conditions of either solution-controlled or membrane-controlled diffusive transport. The FDM was used to measure cobalt binding isotherms by a humic substance over a large range of free Co concentrations and pH.  相似文献   

20.
The performance of the technique of diffusive gradients in thin films (DGT) was characterized in well-defined systems containing cadmium with chloride and nitrate ions, simple organic ligands (nitrilotriacetic acid and diglycolic acid), and Suwannee river fulvic acid for the pH range 5-8. Cd was fully labile in all Cd, Cl-, and NO3- solutions tested (I= 0.1 and 0.01 M), even atvery low Cd concentrations (10 nM), consistent with there being no binding of Cd to the diffusive gel. Diffusion coefficients of Cd-nitritotriacetic acid (NTA) and Cd-diglycolic acid (DGA) species were measured and found to be ca. 25-30% lower than the equivalent coefficient for free metal ions. These values were used to calculate concentrations of labile Cd from DGT measurements in solutions of Cd with NTA or DGA. Cd-NTA and Cd-DGA species were found to be fully DGT-labile. DGT devices that used a diffusive gel with a reduced pore size, which retarded the passage of fulvic acid species through the gel, were used to estimate the proportion of Cd complexed by fulvic acid. These results were compared with predictions of the solution speciation from models with default parameter values. ECOSAT, incorporating the NICA-Donnan model, correctly predicted the magnitude of the binding and its pH dependence, while predictions from WHAM V (with humic ion binding model V) and WHAM 6 (with humic ion binding model VI) were less satisfactory at predicting the pH dependence. Reasonable fits to the data could be obtained from WHAM 6 when the effective binding constant log K(MA) was changed from 1.6 to 1.5, the value of deltaLK1 from 2.8 to 1.0 to minimize the dependence on pH, and the value of deltaLK2 from 1.48 to 1.0 to decrease the strength of the strong bidentate and tridentate binding sites.  相似文献   

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