Characterizing the interactions between polycyclic aromatic hydrocarbons and fulvic acids in water

Polycyclic aromatic hydrocarbons (PAHs) are persistent, bioaccumulative, and toxic chemicals and are listed as priority pollutants by the US EPA. Although they are sparsely soluble in water, their solubility can be increased by binding to dissolved organic matter in natural waters, which will further increase their environmental risk as toxic pollutants. In this study, the interaction between PAHs, exemplified by fluorene and anthracene, and fulvic acid (FA) was studied using fluorescence quenching titration method with fluorescence emission spectra, respectively. The association of FA with the mixture of fluorene and anthracene was also evaluated by excitation–emission matrix (EEM) fluorescence spectrometry combined with parallel factor (PARAFAC) analysis. Results demonstrate that EEM fluorescence spectrometry with PARAFAC analysis was sensitive and reliable to determine the binding properties of PAHs with FA in a mixed aqueous solution. The conditional stability constants and binding capacities show that both PAHs bind to FA tightly.     

Ozonation effects on emerging micropollutants and effluent organic matter in wastewater: characterization using changes of three-dimensional HP-SEC and EEM fluorescence data

The degradation of effluent organic matter (EfOM) in a municipal wastewater treated by ozonation was characterized using the methods of high-performance size-exclusion chromatography (HP-SEC) and excitation/emission matrix (EEM) fluorescence combined with parallel factor analysis (PARAFAC). The removal of 40 diverse trace-level contaminants of emerging concern (CEC) present in the wastewater was determined as well. Ozonation caused a rapid decrease of the absorbance and fluorescence of the wastewater, which was associated primarily with the oxidation of high and low apparent molecular weight (AMW) EfOM fractions. PARAFAC analysis also showed that components C1 and C2 decreased prominently in these conditions. The EfOM fraction of intermediate molecular weight ascribable to a terrestrial humic-like component (C3) tended to be less reactive toward ozone. Relative changes of EEM fluorescence were quantified using F _max values of PARAFAC-identified components (∆F/F ⁰ _max). Unambiguous relationships between ∆F/F ⁰ _max values and the extent of the degradation of the examined CECs (∆C/C₀) were established. This allowed correlating main parameters of the ∆C/C₀ vs. ∆F/F ⁰ _max relationships with the rates of oxidation of these CECs. The results demonstrate the potential of online measurements of EEM fluorescence for quantitating effects of ozonation on EfOM and micropollutants in wastewater effluents.

     

Novel insights into enhanced dewatering of waste activated sludge based on the durable and efficacious radical generating

This study aims to develop a high-efficiency radical oxidation process for enhancing the dewaterability of waste activated sludge (WAS). Radical scavenging studies combined with electron paramagnetic resonance (EPR) were carried out for the direct radical identification and effectiveness evaluation of radical oxidation. The results indicated that Fe(II)-activated CaO₂ can pose a superior effect on dewatering WAS due to its distinctive capacity of stable ?OH production and the high reaction efficiency of regulated-released ?OH with water-holding organics. The mechanism for the enhanced dewatering performance was also explored. The rupture of sludge colloidal flocs and the reduction of hydrophilic functional groups in loosely bound extracellular polymeric substances (LB-EPS) were found to be mainly responsible for the release of interstitial water and improved dewaterability, respectively. In addition, an inference about the relationship between interfacial water and zeta potential of different EPS fractions was established by the simultaneous measurement of the binding affinities of Ca²⁺ and Fe²⁺/Fe³⁺ for EPS and bound water content. All these results provide the direct evidence that Fe(II)-activated CaO₂ is a promising pretreatment reagent for sludge disposal.

Implications: Fe(II)-activated CaO₂ was first proposed to be highly effective in enhancing the dewaterability of waste activated sludge. Electron paramagnetic resonance (EPR) spectroscopy provided the direct evidence for the specific advantages of CaO₂, especially the capacity of durable and efficacious ?OH production leading to the excellent conditioning performance.     

Effect of NaCl on nitrification performance and extracellular polymeric substance characteristic of Klebsiella sp. TN-10

Klebsiella sp. TN-10, isolated from tannery wastewater, exhibited excellent nitrification ability cultivated in media with NaCl contents ranging from 0 to 35 g/L. Analysis of antioxidative enzyme activities of TN-10 stressed by NaCl showed that the stain produced more superoxide dismutase (SOD) and catalase (CAT) to fight against salt stress conditions. Moreover, the auto-aggregation index of TN-10 decreased with the increment of NaCl contents, which is consistent with results of zeta potentials. Extinction-emission matrix (EEM) and Fourier-transform infrared (FT-IR) spectrum analyses showed that the compositions of extracellular polymeric substances (EPS) by TN-10 after NaCl shock were similar. Furthermore, proteins and polysaccharides were the main components of EPS, and the contents were greatly influenced by salinity. Then, circular dichroism (CD) spectrum was used to calculate the contents of each protein secondary structure. These results provided further insights into the knowledge of nitrification characteristics, auto-aggregation performance, and EPS compositions of TN-10 during NaCl shock.

     

盐类对模拟胞外聚合物(EPS)膜污染的影响

实验旨在研究盐类对模拟胞外聚合物(EPS)溶液在超滤和微滤过程中膜污染影响,通过添加与无添加盐类的模拟溶液的比较,研究盐类对EPS膜过滤在死端过滤过程的影响。实验考察了不同模拟溶液的膜通量衰减情况和滤饼比阻,并利用Hermia模型对实验数据进行拟合分析验证膜污染机理。实验结果表明,在超滤过程中,Ca2+和Al3+能在一定程度上提高膜通量,降低滤饼比阻,延缓膜污染;在微滤过程中,两者的添加反而降低了初始通量,添加Ca2+后滤饼比阻值反而有所增大;Na+对超/微滤过程影响很小。通过Hermia模型拟合分析发现,在超滤过程中,添加盐和无添加的溶液均以滤饼堵塞机理为主,而在微滤过程中则是以中间堵塞和滤饼堵塞机理为主。     

Effects of Sulfur Dioxide and Nitric Oxide on Mercury Oxidation and Reduction under Homogeneous Conditions

Abstract

This paper is particularly related to elemental mercury (Hg⁰) oxidation and divalent mercury (Hg²⁺) reduction under simulated flue gas conditions in the presence of nitric oxide (NO) and sulfur dioxide (SO₂). As a powerful oxidant and chlorinating reagent, Cl₂ has the potential for Hg oxidation. However, the detailed mechanism for the interactions, especially among chlorine (Cl)-containing species, SO₂, NO, as well as H₂O, remains ambiguous. Research described in this paper therefore focused on the impacts of SO₂ and NO on Hg⁰ oxidation and Hg²⁺ reduction with the intent of unraveling unrecognized interactions among Cl species, SO₂, and NO most importantly in the presence of H₂O. The experimental results demonstrated that SO₂ and NO had pronounced inhibitory effects on Hg⁰ oxidation at high temperatures when H₂O was also present in the gas blend. Such a demonstration was further confirmed by the reduction of Hg²⁺ back into its elemental form. Data revealed that SO₂ and NO were capable of promoting homogeneous reduction of Hg²⁺ to Hg⁰ with H₂O being present. However, the above inhibition or promotion disappeared under homogeneous conditions when H₂O was removed from the gas blend.     

Aqueous photoreduction of oxidized mercury species in presence of selected alkanethiols

Mercury is a global environmental contaminant with severe toxicity impact. The chemical processes resulting in the transformation of oxidized mercury species (Hg²⁺) to elemental mercury (Hg⁰), greatly affects the fate and transport of mercury in the natural environment. We hereby provide the first study on the photochemistry of Hg²⁺ with selected alkanethiols (R-SH) as model compounds to represent thiols and thiol-type binding sites on humic substances in natural waters because of the common sulfhydryl functional group (-SH). Kinetic studies were performed using cold vapor atomic fluorescence spectroscopy (CVAFS), the formation of Hg²⁺-thiol complexes (Hg(SR)₂) were confirmed by UV-visible spectrometry and Atmospheric Pressure Chemical Ionization-Mass Spectrometry (APCI-MS), and the reaction products were analyzed using Electron Impact-Mass Spectrometry (EI-MS) and Solid Phase Microextraction coupled with Gas Chromatography-Mass Spectrometry (SPME/GC-MS). Our results indicated that the photoreduction of Hg²⁺ by selected alkanethiols may be mediated by Hg²⁺-thiol complexes to produce Hg⁰. Under our experimental conditions, the apparent first order rate constants obtained for 1-propanethiol, 1-butanethiol, and 1-pentanethiol were (2.0 ± 0.2) × 10⁻⁷ s⁻¹, (1.4 ± 0.1) × 10⁻⁷ s⁻¹, (8.3 ± 0.5) × 10⁻⁸ s⁻¹, respectively. The effects of ionic strength, dissolved oxygen or chloride ion on reaction rates were found to be minimal under our experimental conditions. The identified products of the reaction between oxidized mercury species with selected alkanethiols (C₃-C₅) were Hg⁰ and disulfides (RS-SR). The potential environmental implications are herein discussed.     

Quantitative assessment of the toxic effects of heavy metals on 1,2-dichloroethane biodegradation in co-contaminated soil under aerobic condition

1,2-Dichloroethane (1,2-DCA) is one of the most hazardous pollutant of soil and groundwater, and is produced in excess of 5.44 × 10⁹ kg annually. Owing to their toxicity, persistence and potential for bioaccumulation, there is a growing interest in technologies for their removal. Heavy metals are known to be toxic to soil microorganisms at high concentrations and can hinder the biodegradation of organic contaminants. In this study, the inhibitory effect of heavy metals, namely; arsenic, cadmium, mercury and lead, on the aerobic biodegradation of 1,2-DCA by autochthonous microorganisms was evaluated in soil microcosm setting. The presence of heavy metals was observed to have a negative impact on the biodegradation of 1,2-DCA in both soil samples tested, with the toxic effect being more pronounced in loam soil, than in clay soil. Generally, 75 ppm As³⁺, 840 ppm Hg²⁺, and 420 ppm Pb²⁺ resulted in 34.24%, 40.64%, and 45.94% increase in the half live (t_½) of 1,2-DCA, respectively, in loam soil, while concentrations above 127.5 ppm Cd²⁺, 840 ppm Hg²⁺ and 420 ppm of Pb²⁺ and less than 75 ppm As³⁺ was required to cause a >10% increase in the t_½ of 1,2-DCA in clay soil. A dose-dependent relationship between degradation rate constant (k₁) of 1,2-DCA and metal ion concentrations was observed for all the heavy metals tested, except for Hg²⁺. This study demonstrated that different heavy metals have different impacts on the degree of 1,2-DCA degradation. Results also suggest that the degree of inhibition is metal specific and is also dependent on several factors including; soil type, pH, moisture content and available nutrients.     

Surface Compositions of Carbon Sorbents Exposed to Simulated Low-Rank Coal Flue Gases

Abstract

Bench-scale testing of elemental mercury (Hg⁰) sorption on selected activated carbon sorbents was conducted to develop a better understanding of the interaction among the sorbent, flue gas constituents, and Hg⁰. The results of the fixed-bed testing under simulated lignite combustion flue gas composition for activated carbons showed some initial breakthrough followed by increased mercury (Hg) capture for up to ～4.8 hr. After breakthrough, the Hg in the effluent stream was primarily in an oxidized form (>90%). Aliquots of selected activated carbons were exposed to simulated flue gas containing Hg⁰ vapor for varying time intervals to explore surface chemistry changes as the initial breakthrough, Hg capture, and oxidation occurred. The samples were analyzed by X-ray photoelectron spectroscopy to determine changes in the abundance and forms of sulfur, chlorine, oxygen, and nitrogen moieties as a result of interactions of flue gas components on the activated carbon surface during the sorption process. The data are best explained by a competition between the bound hydrogen chloride (HCl) and increasing sulfur [S(VI)] for a basic carbon binding site. Because loss of HCl is also coincident with Hg breakthrough or loss of the divalent Hg ion (Hg²⁺), the competition of Hg²⁺ with S(VI) on the basic carbon site is also implied. Thus, the role of the acid gases in Hg capture and release can be explained.     

Influence of the organic loading rate on the performance and the granular sludge characteristics of an EGSB reactor used for treating traditional Chinese medicine wastewater

The effects of the organic loading rate (OLR) on the performance and the granular sludge characteristics of an expanded granular sludge bed (EGSB) reactor used for treating real traditional Chinese medicine (TCM) wastewater were investigated. Over 90 % of the COD removal by the EGSB reactor was observed at the OLRs of 4 to 13 kg COD/(m³ day). However, increasing the OLR to 20 kg COD/(m³ day) by reducing the hydraulic retention time (HRT 6 h) reduced the COD removal efficiency to 78 %. The volatile fatty acid (VFA) concentration was 512.22 mg/L, resulting in an accumulation of VFAs, and propionic acid was the main acidification product, accounting for 66.51 % of the total VFAs. When the OLR increased from 10 to 20 kg COD/(m³ day), the average size of the granule sludge decreased from 469 to 258 μm. There was an obvious reduction in the concentration of Ca²⁺ and Mg²⁺ in the granular sludge. The visible humic acid-like peak was identified in the three-dimensional excitation-emission matrix (EEM) fluorescence spectra of the soluble microbial products (SMPs). The fatty acid bond, amide II bond, amide III bond, and C–H bond bending were also observed in the Fourier transform infrared (FTIR) spectra of the SMPs. Methanobacterium formicicum, Methanococcus, and Bacteria populations exhibited significant shifts, and these changes were accompanied by an increase in VFA production. The results indicated that a short HRT and high OLR in the EGSB reactor caused the accumulation of polysaccharides, protein, and VFAs, thereby inhibiting the activity of methanogenic bacteria and causing granular sludge corruption.     

Enhanced 1,2-dichloroethane degradation in heavy metal co-contaminated wastewater undergoing biostimulation and bioaugmentation

Biostimulation, bioaugmentation and dual-bioaugmentation strategies were investigated in this study for efficient bioremediation of water co-contaminated with 1,2-dichloroethane (1,2-DCA) and heavy metals, in a microcosm set-up. 1,2-DCA concentration was periodically measured in the microcosms by gas chromatographic analysis of the headspace samples, while bacterial population and diversity were determined by standard plate count technique and Polymerase chain reaction and denaturing gradient gel electrophoresis (PCR–DGGE) analysis, respectively. Dual-bioaugmentation, proved to be most effective exhibiting 22.43%, 26.54%, 19.58% and 30.49% increase in 1,2-DCA degradation in microcosms co-contaminated with As³⁺, Cd²⁺, Hg²⁺ and Pb²⁺, respectively, followed by bioaugmentation and biostimulation. Dual-bioaugmented microcosms also exhibited the highest increase in the biodegradation rate constant (k₁) resulting in 1.76-, 2-, 1.7- and 2.1-fold increase in As³⁺, Cd²⁺, Hg²⁺ and Pb²⁺ co-contaminated microcosms respectively, compared to the untreated microcosms. Dominant bacterial strains obtained from the co-contaminated microcosms were found to belong to the genera Burkholderia, Pseudomonas, Bacillus, Enterobacter and Bradyrhizobium, previously reported for 1,2-DCA and other chlorinated compounds degradation. PCR–DGGE analysis revealed variation in microbial diversity over time in the different co-contaminated microcosms. Results obtained in this study have significant implications for developing innovative bioremediation strategies for treating water co-contaminated with chlorinated organics and heavy metals.     

Removal of heavy metal ions from wastewaters using dendrimer-functionalized multi-walled carbon nanotubes

Dendrimer-functionalized multi-walled carbon nanotubes (MWCNT) for heavy metal ion removal from wastewaters were developed. Triazole dendrimers (TD) were built directly onto the carbon nanotube surface by successive click chemistry reactions affording the zero- and first-generation dendrimer-functionalized MWCNT (MWCNT-TD1 and MWCNT-TD2). The Moedritzer-Irani reaction carried out on the amino groups present on the MWCNT-TD2 sample gave the corresponding α-aminophosphonate nanosystem MWCNT-TD2P. Both MWCNT-TD2 and MWCNT-TD2P nanosystems have been characterized by physical, chemical, and morphological analyses. Their chelating abilities towards the toxic metal ions Pb²⁺, Hg²⁺, and Ni²⁺ and the harmless Ca²⁺ ion have been experimentally evaluated in the two different sets of experiments and at the salt concentrations of 1 mg/mL or 1 μg/mL by inductively coupled plasma mass spectrometry (ICP-MS). The results of these studies pointed out the interesting chelating behavior for the phosphonated nanosystem towards the Hg²⁺ ion. The complexation mode of the best chelating system MWCNT-TD2P with mercury was investigated through density functional theory (DFT) calculations, suggesting a chelation mechanism involving the two oxygen atoms of the phosphate group. The synthesized dendrimers, supported on the multi-walled carbon nanotubes, have shown the potential to be used for the selective toxic metal ion removal and recovery.     

新型重金属捕集剂NBMIPA处理含铜汞废水

研究了以间苯二甲酰氯和巯基乙胺盐酸盐为原料合成的重金属捕集剂NBMIPA对单一Cu2＋、Hg2＋电镀废水的捕集性能。结果研究表明,NBMIPA对Cu2＋和Hg2＋的捕集性能优良,NBMIPA投加量越大,捕集性能越高;NBMIPA对pH具有较宽适应性。NBMIPA对于单一含铜废水可无需调pH,投加捕集剂量为废水中含量的4～5倍（摩尔比）,静置后其上层清夜中所含Cu2＋为0.38 mg/L,Cu2＋的去除率可达99.5%以上;当NBMIPA的投加量（摩尔比）是Hg2＋的3.5～4.5倍时,Hg2＋的去除率达到99.83%,残余Hg2＋浓度为0.032 mg/L。     

Impact of cadmium and nickel on ion homeostasis in the yeast Schizosaccharomyces pombe

Abstract

Toxicity of heavy metals to living organisms is a worldwide research topic. Although, much has been discovered about cadmium and nickel impact on biological systems, a lot still remains unclear. We used inductively coupled plasma – optical emission spectroscopy to address the question of the effect of two different heavy metals nickel, and cadmium on intracellular ion balance. Increase or decrease of the content of several essential cations including Ca²⁺, Na⁺, K⁺, Mg²⁺, Cu²⁺, Fe³⁺ in the yeast Schizosaccharomyces pombe was determined. Our results revealed that the cell exposure to high nickel and cadmium concentrations led to significant elevation of Ca²⁺, Na⁺, Mg²⁺, Cu²⁺, Fe³⁺ levels in the yeast cell, while the content of K⁺ decreased. Correlation analyses showing in the presence of nickel and cadmium strong positive correlation among each tested element (Ca²⁺, Na⁺, Cu²⁺, Mg²⁺ and Fe³⁺) except for K⁺, demonstrate the significant impact of heavy metal treatment to ion homeostasis of the cell. Our data indicate that acute nickel and cadmium contamination leads to substantial ionome misbalance in yeast.     

Multivariate curve resolution of multidimensional excitation-emission quenching matrices of a Laurentian soil fulvic acid

Fluorescence excitation–emission matrices (EEM) of aqueous solutions of Laurentian soil fulvic acid (LFA) at three concentrations (50, 75 and 100 mg/l) were obtained at two pH values (pH = 4.0 and 6.0) and as function of the Cu(II) ion concentration. The presence of Cu(II) ion provokes quenching of the intrinsic LFA fluorescence due to complex formation. Multivariate curve resolution (MCR-ALS) was used to successfully decompose single EEM into excitation and emission spectra for the detected components. Moreover, multidimensional (up to six dimensions) data matrices were generated by adding EEM collected as function of the LFA and Cu(II) concentrations and pH. MCR-ALS was able to resolve the excitation and emission spectra from these multidimensional data matrices given further information about the spectral variation profiles induced by the experimental factors. Conditional stability constants (log K_LFACu) were calculated from the quenching profiles observed as function of the Cu(II) concentration, as well as, their trends as function of pH and LFA concentration were obtained – average (and standard deviation) of log K_LFACu = 4.6 ± 0.2. This EEM/MCR-ALS methodology constitutes a new tool for the study of natural organic matter under varying experimental conditions that characterize natural environmental systems.     

Structural and optical characterization of dissolved organic matter from the lower Athabasca River, Canada

Dissolved organic matter (DOM) is a ubiquitous constituent of natural waters and is comprised of a variety of chemically heterogeneous molecular structures and functional groups. DOM is often considered to be a major ligand for metals in most natural waters and its reactivity is thought to be strongly dependent on its chemical composition and structure. In this study, a combination of UV/visible, emission excitation matrix fluorescence (EEM) and ¹H NMR spectroscopies were used to characterize DOM from the Athabasca River (Alberta, Canada). The chemical characterization of river DOM showed that the most upstream samples located in agricultural areas were blue-shifted and less aromatic and contained more hydrogens connected with oxygen functional groups than those in the wetland dominated area in the Athabasca oil sand deposit region. The presence of paramagnetic ions (Fe and Al) was not found to significantly affect the structural composition of DOM as revealed by ¹H NMR. Such change in the quality of DOM may have a profound impact on metal binding in the Athabasca River watershed.     

Issues Related to Solution Chemistry in Mercury Sampling Impingers

ABSTRACT

Analysis of Hg speciation in combustion flue gases is often accomplished in standardized sampling trains in which the sample is passed sequentially through a series of aqueous solutions to capture and separate oxidized Hg (Hg²⁺) and elemental Hg (Hg⁰). Such methods include the Ontario Hydro (OH) and the Alkaline Mercury Speciation (AMS) methods, which were investigated in the laboratory to determine whether the presence of Cl₂ and other common flue gas species can bias the partitioning of Hg⁰ to front impingers intended to isolate Hg²⁺ species. Using only a single impinger to represent the front three impingers for each method, it was found that as little as 1-ppm Cl₂ in a simulated flue gas mixture led to a bias of approximately 10-20% of Hg⁰ misreported as Hg²+ for both the OH and the AMS methods. Experiments using 100-ppm Cl₂ led to a similar bias in the OH method, but to a 30-60% bias in the AMS method. These false readings are shown to be due to liquid-phase chemistry in the impinger solutions, and not necessarily to the gas-phase reactions between Cl₂ and Hg as previously proposed. The pertinent solution chemistry causing the interference     

Evaluation of effectiveness of EDTA and sodium thiosulfate in removing metal toxicity toward sea urchin embryo-larval applying the TIE

Since the development of the TIE (Toxicity Identification and Evaluation) in 1988 it has been assumed that the capacity of EDTA and sodium thiosulfate to complex some metals, and thus remove their toxicity, can be applied to both freshwater and seawater ecotoxicological tests and the results subsequently interpreted. However, it is now known that there is a wide variability in the extent of this complexation. In this context, the removal of toxicity caused by the presence of Hg²⁺, Cd²⁺, Cu²⁺, Cr⁶⁺, Zn²⁺, Ni²⁺, Pb²⁺, Ag¹⁺ and Se²⁺, through metal complexation by EDTA and sodium thiosulfate, in relation to the performance of embryo-larval tests with the sea urchin Arbacia lixula was investigated. It was observed that EDTA was capable of removing the toxicity of Pb²⁺, Zn²⁺ and Cu²⁺ while sodium thiosulfate only reduced the toxicity of Ag¹⁺. Compared to the complexation observed in freshwater ecotoxicological tests, the complexing agents used in this study (EDTA and sodium thiosulfate) have a lower capacity to complex metals in the marine ecotoxicological test with A. lixula.     

Study on substrate metabolism process of saline waste sludge and its biological hydrogen production potential

With the increasing of high saline waste sludge production, the treatment and utilization of saline waste sludge attracted more and more attention. In this study, the biological hydrogen production from saline waste sludge after heating pretreatment was studied. The substrate metabolism process at different salinity condition was analyzed by the changes of soluble chemical oxygen demand (SCOD), carbohydrate and protein in extracellular polymeric substances (EPS), and dissolved organic matters (DOM). The excitation-emission matrix (EEM) with fluorescence regional integration (FRI) was also used to investigate the effect of salinity on EPS and DOM composition during hydrogen fermentation. The highest hydrogen yield of 23.6 mL H₂/g VSS and hydrogen content of 77.6% were obtained at 0.0% salinity condition. The salinity could influence the hydrogen production and substrate metabolism of waste sludge.

     

Investigation of uranium binding forms in selected German mineral waters

Cryogenic time-resolved laser-induced fluorescence spectroscopy was successfully used to identify uranium binding forms in selected German mineral waters of extremely low uranium concentrations (<2.0 μg/L). The measurements were performed at a low temperature of 153 K. The spectroscopic data showed a prevalence of aquatic species Ca₂UO₂(CO₃)₃ in all investigated waters, while other uranyl–carbonate complexes, viz, UO₂CO_3(aq) and UO₂(CO₃)₂ ^2?, only existed as minor species. The pH value, alkalinity (CO₃ ^2?), and the main water inorganic constituents, specifically the Ca²⁺ concentration, showed a clear influence on uranium speciation. Speciation modeling was performed using the most recent thermodynamic data for aqueous complexes of uranium. The modeling results for the main uranium binding form in the investigated waters indicated a good agreement with the spectroscopy measurements.