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PubMed2005

Comparison of zinc complexation properties of dissolved natural organic matter from different surface waters.

The zinc binding characteristics of natural organic matter (NOM) from several representative surface waters were studied and compared. NOM samples were concentrated by reverse osmosis. The samples were treated in the laboratory to remove trace metals. Square wave anodic stripping voltammetry (SWASV) was used to study zinc complexing properties of those NOM samples at fixed pH, ionic strength, and dissolved organic carbon (DOC) concentrations. Experimental data were compared to the predictions from the Windermere Humic Aqueous Model (WHAM) Version VI. At the same pH, ionic strength, and temperature, the zinc titration curves for NOM samples from different surface water sources tested in our study almost overlapped each other, indicating similarity in zinc binding properties of the NOM. A discrete two-site model gave good fits to our experimental titration data. Non-linear fitting by FITEQL 4.0 shows that the conditional zinc binding constants at the same pH are similar for NOM from different sources, indicating that zinc complexation characteristics of the NOM used in our study do not depend on their origin and one set of binding parameters can be used to represent Zn-NOM complexation for NOM samples from those different surface water sources representing geographically diverse locations. In addition, the total ligand concentrations (L(1,T), L(2,T), and L(T)) of all NOM show no observable gradation with increasing pH (L(1,T)=2.06+/-0.80 mmol/g carbon; L(2,T)=0.12+/-0.04 mmol/g carbon; L(T)=2.18+/-0.78 mmol/g carbon), while the conditional binding constants of zinc by NOM (logK(ZnL)(c)) show a linear increase with increasing pH(logK(1)(c)(pH=6.0)=4.69+/-0.25; logK(1)(c)(pH=7.0)=4.94+/-0.10; logK(1)(c)(pH=8.0)=5.25+/-0.006; logK(2)(c)(pH=6.0)=6.29+/-0.13; logK(2)(c)(pH=7.0)=6.55+/-0.08; logK(2)(c)(pH=8.0)=6.86+/-0.023) with a slope of ca. 0.28, indicating the zinc-NOM complexes become more stable at higher pH. The WHAM VI predicted free zinc ion activities at high zinc concentrations agree with our experimental results at pH 6.0, 7.0, and 8.0. However, the zinc binding of these NOM samples is over estimated by WHAM VI at zinc concentrations below 10(-6) M at pH 8.0.

Carbon↗
PubMed2026

Optimizing eco-engineering pedogenesis of bauxite residues: Synergistic effects of humus and FeSO4/sulfur on microbial community and function.

Eco-engineered pedogenesis represents a promising approach for soil amelioration of bauxite residues (BRs) through exogenous organic matter. However, the role of humus in mediating this process remains poorly understood, significantly impeding the eco-engineering rehabilitation of BRs. In this study, we conducted pot experiments and subsequent microbial analysis to evaluate the individual improvement of humic acid (HA), fulvic acid (FA), and corn straw (SWZ) on the BRs' pedogenesis. High-throughput sequencing analysis revealed that both FA and SWZ were more effective than HA in steering microbial community assembly, as community diversity, dominant taxa enrichment, and species' interaction were all significantly higher (p < 0.05) in the FA/SWZ treatments than in HA treatments. Notably, the combination of FA with FeSO4 specifically enriched halophilic taxa, while FA coupled with sulfur (S) significantly improved the connectivity and complexity of the microbial network, as the average connection degree increasing from 1.008 to 1.113. Hydrolytic enzyme activity assays further indicated that FA, especially when combined with S, was the most effective treatment in restoring microbial function during BR pedogenesis. These findings highlight FA as a critical driver of microbial restructuring and functional recovery in BRs. Moreover, its efficacy can be enhanced by co-amendment with FeSO4 or S. This study provides important theoretical and practical insights for optimizing organic-inorganic amendment strategies to accelerate the eco-engineering pedogenesis of bauxite residues.

Humic Substances↗
PubMed2005

Adsorption and thermochemical data of divalent cations onto silica gel surface modified with humic acid at solid/liquid interface.

Humic acid immobilized onto silica gel surface was studied by the calorimetric titration of divalent cations in aqueous solution. The adsorption isotherms were obtained by the batchwise method and were fitted to a modified Langmuir equation. The maximum number of moles per gram of the material gave: 10.42+/-0.75, 13.16+/-0.58, 7.87+/-0.58 for copper, nickel and zinc, respectively. Gibbs free energies were negative for all systems and the adsorption interactions calorimetrically followed presented endothermic enthalpic values: 6.24+/-0.47, 6.75+/-0.74, 6.97+/-0.58 kJ mol-1 for the same sequence of divalent cations. All liquid/solid interface adsorptions were entropically driven.

Adsorption↗
PubMed2005

Treatment of groundwater polluted by arsenic compounds by zero valent iron.

Batch experiments were carried out to study the kinetics and efficiency of inorganic arsenic removal by zero valent iron (ZVI) powder, and as well as the effects of pH, anions, and humic material (HM) on this process. Moreover, column experiment was conducted for 31 days to treat arsenate solution of 500 microg As/L using waste iron chippings as filling. Batch experiments showed that both arsenate and arsenite compounds could be removed efficiently from simulated groundwater by ZVI under aerobic and relative anaerobic conditions. Aerobic condition was favorable to arsenic removal especially for arsenate, while arsenite could be removed more rapidly than arsenate in relative anaerobic condition. Oxidation of arsenite to arsenate by iron species in aerobic environment was observed, which is thought to be an important pathway of arsenite removal. In an unsealed system, the removal efficiency of both arsenate and arsenite decreased at higher pH value. In a sealed system, acidic and alkaline condition seemed to be favorable for arsenate and arsenite removal, respectively. Phosphate and low concentration sulfate caused a decrease in arsenate removal, while high concentration sulfate as well as nitrate caused slight increase in arsenate removal. Presence of HM in solution slightly inhibited arsenic removal. Arsenic removal efficiency in column study was influenced by flow rate and work period of the column. More than 98% of arsenate could be removed stably with a hydraulic resident time of 2 h at last, and the effluent meet the drinking water standard.

Arsenic↗
PubMed2005

Lead adsorption by silica-immobilized humin under flow and batch conditions: assessment of flow rate and calcium and magnesium interference.

Batch and column experiments were performed to determine the Pb(II) binding ability of silica-immobilized humin biomass under different conditions. Batch experiments were performed to determine the interference of Ca(II) and Mg(II) and column experiments were used to determine the effect of flow rate and the presence of Ca(II) and Mg(II) on the Pb(II) adsorption by the humin biopolymer. The results from the batch experiments showed that Pb binding decreased as the concentrations of Ca and Mg increased. At a concentration of 100 mM, the interference of Ca alone was 36%, while for Mg it was 26%; however, when both cations were present, the interference increased up to 42%. Column experiments were performed at flow rates of 1, 1.5, 2, and 3 mL min(-1) using a 0.1 mM Pb(II) solution. The results showed that the highest Pb adsorption was obtained at the flow rates of 1 and 1.5 mL min(-1). The average Pb binding capacity at these two flow rates was 182.3 +/- 0.7 microMPbg(-1). In addition, a recovery of 99.5 +/- 0.3% was obtained. Immobilized humin exposed under flow conditions to Pb-Ca, Pb-Mg or Pb-[Ca + Mg] solutions (Pb used at 0.1 mM and Ca and Mg at 1 mM) showed a Pb binding capacity of 161+/- 5, 175 +/- 5, and 171+/- 1 microM g(-1), respectively. In mixtures containing Pb-Ca, Pb-Mg and Pb-Ca-Mg, the Pb recovery was 89.8% +/- 0.35, 90.3% +/- 0.43, and 88.1% +/- 0.5, respectively. Pb recovery was performed using 30 bed volumes of 0.1M HCl as stripping agent. The results of these experiments demonstrated that silica-immobilized humin biomass has the potential for Pb removal from aqueous solution even in the presence of 20 mM of calcium and magnesium.

Adsorption↗
PubMed2006

Studies on copper(II)- and zinc(II)-mixed ligand complexes of humic acid.

Interactions between humic acid (HA), extracted from Brazilian peat soil, and cations of copper(II) and zinc(II) have been examined by infrared spectroscopy, and electrochemical and thermogravimetric analyses. Spectral studies revealed that the interaction with metals occurred mainly at the carboxylic acid groups of HA. The stability constants of HA complexes formed with Cu(2+) and Zn(2+) were found, by square wave voltammetry and application of the Lingane model, to be 8.93 x 10(10) and 2.92 x 10(2), respectively. Thermal analysis indicated that the stability of HA was increased by the presence of divalent cations of copper and zinc.

Algorithms↗
PubMed2006

Comparison of adsorption capacity of young brown coals and humic acids prepared from different coal mines in Anatolia.

Binding of Zn2+ and Cd2+ cations to relatively young brown coals YBC (lignite), humic acids (HAs) and commercial humic acid (CHA) were studied in aqueous media at pH 2.7-6 by polarographic method. This study was conducted to evaluate the removal of heavy metals in an aquatic system without prior treatment. The general principles of cation binding to YBC and humic materials are discussed. Sorption of heavy metal ions (Zn2+ and Cd2+) on samples of YBCs from three areas (Ilgin, Beysehir, and Ermenek) in the vicinity of the city of Konya in Anatolia (Turkey) were compared with sorption of these metal ions on HAs, prepared from these YBCs. The ability of both types of sorbent to remove metals from aqueous solutions was studied as a function of pH and concentration of initial metal solutions. Sorption depends strongly on pH, the origin of the YBC and on the nature of the metal ion. Whereas, for YBCs the main ligand groups seem to be carboxylate ions, this is not the case for the HA polymers, prepared from three YBCs, which differ substantially from properties of commercial samples of "HA". The process is very efficient especially in the case of low concentrations of pollutants in water, where common methods are either economically unfavorable or technically complicated. Of the two metal ions examined, Cd2+ was found to form the most stable HA complexes, followed by Zn. Effective removal of metals was demonstrated at pH-values of 5-5.7. The adsorption isotherm was measured at 25 degrees C, using adsorptive solutions at the optimum pH-value to determine the adsorption capacity. An important aspect of the proposed method was that the removal was performed on several metals at a pH-range in which a given metal undergoes an adsorption process making the method useful for wastewater treatment.

Adsorption↗
PubMed2006

Effect of contact order on the adsorption of inorganic arsenic species onto hematite in the presence of humic acid.

The speciation of aqueous and adsorbed As forms of arsenic (As) is a major environmental concern in the presence of humic acid (HA). The speciation during As adsorption process by the effect of contact order were evaluated in various equilibrated ternary systems consisting of As, HA and hematite. One ternary system was composed of the preequilibrated As(III)- or As(V)-HA complex, with the subsequent addition of hematite ((As-HA)-hematite system), and the other consisted of the preequilibrated HA-hematite, with the addition of As(III) or As(V) (As-(HA-hematite) system). The presence of HA led to a decrease in the As adsorption, opposite to cationic adsorption. The order of the amounts of As adsorption were found to follow as: As(V)-hematite>hematite-(As(V)-HA)>As(V)-(HA-hematite)>As(III)-hematite>hematite-(As(III)-HA)>As(III)-(HA-hematite). Free As(V) and As-HA complex were preferentially adsorbed onto the hematite surface. The immobilization of As can come from adsorbed HA on mineral surfaces, and formation of As-HA complex, following their slow kinetics.

Adsorption↗
PubMed2006

Removal of dieldrin from aqueous solution by a novel triolein-embedded composite adsorbent.

In this study, a novel triolein-embedded activated carbon composite adsorbent (CA-T) was prepared and applied for the adsorption and removal of dieldrin from aqueous systems. Experiments were carried out to investigate the adsorption behavior of dieldrin on CA-T, including adsorption isotherms, adsorption kinetics, the influence of initial concentration, temperature, shaking speed, pH and the addition of humic acid (HA) on adsorption. The adsorption isotherms accorded with Freundlich equation. Three kinetics models, including pseudo-first-order, pseudo-second-order and intraparticle diffusion models, were used to fit the experimental data. By comparing the correlation coefficients, it was found that both pseudo-second-order and intraparticle diffusion models were used to well describe the adsorption of dieldrin on CA-T. The addition of HA had little effect on dieldrin adsorption by CA-T. Results indicated that CA-T appeared to be a promising adsorbent for removing lipophilic dieldrin in trace amount, which was advantageous over pure granular activated carbon (GAC). The adsorption rate increased with increasing shaking speed, initial concentration and temperature, and remained almost unchanged in the pH range of 4-8. Thermodynamic calculations indicated that the adsorption reaction was spontaneous with a high affinity and the adsorption was an endothermic reaction.

Adsorption↗
PubMed2006

Influence of Fenton oxidation on soil organic matter and its sorption and desorption of pyrene.

The influences of Fenton oxidation on the content and composition of soil organic matter (SOM) and the consequent change of its sorption and desorption of pyrene were investigated using three soil samples. The results showed that both the content and the composition of the SOM changed, with total SOM content decreasing. The content of humic acid (HA) was reduced, while the content of humin did not change significantly, however the content of fulvic acid (FA) had a tendency to increase. Correlation analysis of soil-water distribution coefficient (K(d)) and different parts of the SOM reveals that humin and HA are the key factors controlling the sorption of pyrene. Organic carbon normalized K(d) (K(OC)) varied to different extents after Fenton oxidation due to the change of SOM composition. The reduction of K(OC) is significant in Soils 1 and 2 where large part of HA was reduced to FA, whose sorption ability is low. The change of K(OC) by oxidation in Soil 3 is not so significant due to that the percentage of humin and HA in Soil 3 did not change greatly after oxidation. Desorption was hysteretic in all cases, and humin percentage was found to be the key factor on the extent of desorption hystersis. Oxidation made desorption more hysteretic due to the elevated proportion of humin.

Adsorption↗
PubMed2006

Competitive metal binding to a silicate-immobilized humic material.

The investigation of the competitive binding of metal ions to a biogenic material comprised of organic peat immobilized in a polysilicate matrix was undertaken. This material was packed into 5.0mL bed-volume columns using 40-60mesh size particles. Two separate mixtures of metal ions were studied by monitoring the solution pH and the concentration of each metal in the effluent as a function of the volume of influent introduced to the material. These mixtures contained either the metal ions Ca(2+), Mg(2+), and Cu(2+) or the ions Cu(2+), Hg(2+), and Pb(2+). A general order of binding affinities was determined to be Mg(2+)<Ca(2+)<<Cu(2+)<Pb(2+)<Hg(2+). Comparisons of amounts of metal ions bound and protons released indicated the initial release of two protons for each divalent metal ion bound. However, prolonged exposure of the material to the metal solutions yielded a molar ratio of 1:1. This suggests the involvement of ion exchange sites followed by that of sites using an alternate binding mechanism. The presence of binding sites with varied mechanisms and metal ion affinities was further illustrated through the initial binding and subsequent release of lower affinity metal ions (e.g., Mg(2+) and Ca(2+)).

Adsorption↗
PubMed2003

Identification of 6-aminochrysene photoproducts and study of the effect of a humic acid and riboflavin on its photolysis.

The effect of the photosensitizer riboflavin (0, 10, 25, 50, 100 microM) and a river humic acid (0, 20, 40, 80 ppm) on the photolysis of 6-aminochrysene (6AC) in 10 mM PBS solution (pH 7.0) was studied. The presence of riboflavin significantly enhanced photolysis rate of 6AC. The photo-transformation half-life of 6AC was 1 or 36 min, respectively, in the presence or absence of riboflavin. The humic acid inhibited the photo-transformation rate of 6AC. The photo-transformation half-lives of 6AC were 37, 56, 92 min at 20, 40, 80 ppm humic acid, respectively. By using LC-MS, the main 6AC photoproduct identified was 5,6-chrysene-quinone along with some minor products. Both 6AC and 5,6-chrysene-quinone exhibited photoinduced cytotoxicity. A photochemical transformation pathway for 6AC was derived.

Chrysenes↗
PubMed2004

Humic acid induces apoptosis in human premyelocytic leukemia HL-60 cells.

It has been shown that humic acid (HA), a phenolic polymer, exhibits pro-oxidant and cytotoxic effects. In this study, HA induction of apoptosis was studied using cultured human premyelocytic leukemia HL-60 cells. Treatment at a range of HA concentrations (50-400 microg/ml) resulted in dose-and time-dependent sequences of events marked by apoptosis, as demonstrated through by apoptotic features such as loss of cell viability, chromatin condensation, and internucleosomal DNA fragmentation. This HA-induced apoptosis in the HL-60 cells was mainly associated with the release of cytochrome c from the mitochondria. Furthermore, apoptosis in the HL-60 cells was accompanied by the activation of caspase-3 and the specific proteolytic cleavage of poly (ADP-ribose) polymerase (PARP), a major component in the apoptotic cell death mechanism. Although the HA-induced apoptosis was associated with Bax protein levels, negligible Bcl-2 reduction was observed. Analysis of the data reported herein reveals that HA exerts antiproliferative action and growth inhibition on HL-60 cells through induction of apoptosis, which may have anticancer properties potentially useful for the development of new drug products.

Antineoplastic Agents, Phytogenic↗
PubMed2005

The role of various dissolved organic matter forms on chlorpyrifos bioavailability to the estuarine bivalve Mercenaria mercenaria.

Dissolved organic matter (DOM) is comprised of a myriad of macromolecules with specific physical and chemical properties that may influence the bioavailability of hydrophobic pesticides to animals. This study was conducted to assess the role of various forms of DOM on the uptake and bioconcentration of the organophosphate insecticide chlorpyrifos (CHPY) to the bivalve Mercenaria mercenaria. Bivalves were exposed to DOM-free seawater (30 per thousand) or to seawater containing a single form of DOM. DOM forms included two filtrate fractions of natural salt-marsh sediment DOM (DOM-(<0.45 mum) and DOM-(<3 kDa)); natural purified humic (HA) and fulvic (FA) acids; and water soluble cyclic oligosaccharides alpha and beta cyclodextrins (CD-alpha and CD-beta). In (14)C-CHPY uptake and elimination experiments, juvenile bivalves were exposed to uniformly-labeled (14)C-CHPY and collected at time intervals during 48 h. The remaining bivalves were transferred to (14)C-CHPY-free elimination chambers with bivalve collection at time intervals over 144 h. Total uptake of (14)C-CHPY by bivalves in DOM-free seawater was >40% greater than in bivalves exposed to (14)C-CHPY in the presence of most DOM forms. These results are consistent with much faster (14)C-CHPY uptake rates estimated using a simple two parameter model. After the elimination period, bivalves exposed to DOM-free seawater had (14)C-CHPY body residue concentrations between 25% and 86% greater than bivalves in the presence of DOM forms. Experiments with larger bivalves showed that pulse-chase exposures with a 1.5 h exposure period to (14)C-CHPY was not long enough to detect differences in (14)C-CHPY tissue accumulation efficiencies across treatments. Our findings suggest that natural forms of DOM, at environmentally realistic organic carbon concentrations, reduced pesticide uptake and bioconcentration, consistent with much lower uptake rates relative to bivalves exposed to (14)C-CHPY in the absence of DOM. Interestingly, at the tested organic carbon concentrations CD-alpha and CD-beta did not reduce (14)C-CHPY bioconcentration in M. mercenaria.

Analysis of Variance↗
PubMed2005

Modulating effects of humic acids on genotoxicity induced by water disinfectants in Cyprinus carpio.

The use of chlorinated disinfectants during drinking-water production has been shown to generate halogenated compounds as a result of interactions of humic acids with chlorine. Such chlorinated by-products have been shown to induce genotoxic effects and consumption of chlorinated drinking-water has been correlated with increased risk for cancer induction in human populations. The aim of this work was to test the potential genotoxic effects on circulating erythrocytes of the fish Cyprinus carpio exposed in vivo to well-waters disinfected with sodium hypochlorite (NaClO), chlorine dioxide (ClO2) or peracetic acid (CH3COO2H, PAA), in the absence or presence of standard humic acids (HA). The effects were measured by use of the micronucleus (MN) and the single-cell gel electrophoresis (Comet) assays at different sampling times after a 3-day exposure period. The exposure to chlorine disinfectants without the addition of HA produced a clear toxic effect. Significant cytogenetic damage (i.e. MN induction) was detected in fish populations exposed to both NaClO and ClO2 with humic acids. In the Comet assay, a significant decrease of DNA migration was observed in erythrocytes of specimens after exposure to NaClO-disinfected water without HA. No effects were observed in any other experimental condition.

Animals↗
PubMed2005

Humic acids reduce the genotoxicity of mitomycin C in the human lymphoblastoid cell line TK6.

The antimutagenic/desmutagenic activity of a leonardite humic acid (LHA) and a soil humic acid (SHA) was studied in the cultured human lymphoblastoid cell line TK6 treated with mitomycin C (MMC) as reference mutagen by evaluating the induction of micronuclei (MN). Two different concentrations of HA were used, 2.5 and 10 microg/ml, in three different treatments: (1) HA alone (genotoxic test); (2) HA after 2-h pre-incubation with 0.3 microM of MMC (desmutagenic test) and (3) combinations of HA and MMC at 0.3 microM without pre-incubation (antimutagenic test). Neither of the HA used alone did produce genotoxic effects, but both HAs reduced significantly the frequencies of MN induced by MMC, especially in the desmutagenic test. A slight cell-protective effect against the cytotoxicity of MMC was also exhibited by the two HAs in the desmutagenic test. The LHA showed a desmutagenic/antimutagenic activity that was more pronounced than that of SHA, which is possibly related to the higher carboxylic group content and lower phenolic group content of LHA. These results confirm the antigenotoxic action exerted by HAs in human cells, similarly to what has been previously observed in various plant species.

Antibiotics, Antineoplastic↗
PubMed2004

Organic matter transformation in the environment investigated by quantitative electron paramagnetic resonance (EPR) spectroscopy: studies on lignins.

The lignins separated from angiosperm and gymnosperm trees, peat and xylitic brown coal were investigated by quantitative EPR. Observed free radicals in lignins are sensitive to alkaline environment. Gaseous ammonia interacting with solid lignins in resonance cavity shifts quinone-hydroquinone equilibria towards formation of semiquinone anions. Complexation of copper(II) by lignins causes drastic decrease of the semiquinones in the matrices. Formation of lignin-Pb(II) complexes yielded radicals characterised by unusually low g-value (1.9999-2.0003). Monomeric structural units of the investigated lignins were recognised by pyrolysis with in situ methylation by tetramethylammonium hydroxide. Although for the natural lignins the mixture of normal semiquinone signals at g about 2.0034 and signals at g 1.9999 were observed, some monomeric components of lignins (e.g., caffeic acid, pyrogallol) gave pure lines at g = 1.9999. The bacterial oxidative biodegradation of lignin monomeric components and their Pb(II) complexes resulted in increase of the radical signals.

Bacillus subtilis↗