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Dynamic silver speciation as studied with fluorous-phase ion-selective electrodes: Effect of natural organic matter on the toxicity and speciation of silver.

ABSTRACT: The widespread application of silver in consumer products and the resulting contamination of natural environments with silver raise questions about the toxicity of Ag(+) in the ecosystem. Natural organic matter, NOM, which is abundant in water supplies, soil, and sediments, can form stable complexes with Ag(+), altering its bioavailability and toxicity. Herein, the extent and kinetics of Ag(+) binding to NOM, matrix effects on Ag(+) binding to NOM, and the effect of NOM on Ag(+) toxicity to Shewanella oneidensis MR-1 (assessed by the BacLight viability assay) were quantitatively studied with fluorous-phase Ag(+) ion-selective electrodes (ISEs). Our findings show fast kinetics of Ag(+) and NOM binding, weak Ag(+) binding for Suwannee River humic acid, fulvic acid, and aquatic NOM, and stronger Ag(+) binding for Pony Lake fulvic acid and Pahokee Peat humic acid. We quantified the effects of matrix components and pH on Ag(+) binding to NOM, showing that the extent of binding greatly depends on the environmental conditions. The effect of NOM on the toxicity of Ag(+) does not correlate with the extent of Ag(+) binding to NOM, and other forms of silver, such as Ag(+) reduced by NOM, are critical for understanding the effect of NOM on Ag(+) toxicity. This work also shows that fluorous-phase Ag(+) ISEs are effective tools for studying Ag(+) binding to NOM because they can be used in a time-resolved manner to monitor the activity of Ag(+) in situ with high selectivity and without the need for extensive sample preparation.

SUBMITTER: Mousavi MP

PROVIDER: S-EPMC4643687 | biostudies-literature | 2015 Dec

REPOSITORIES: biostudies-literature

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Dynamic silver speciation as studied with fluorous-phase ion-selective electrodes: Effect of natural organic matter on the toxicity and speciation of silver.

Mousavi Maral P S MP Gunsolus Ian L IL Pérez De Jesús Carlos E CE Lancaster Mitchell M Hussein Kadir K Haynes Christy L CL Bühlmann Philippe P

The Science of the total environment 20150815

The widespread application of silver in consumer products and the resulting contamination of natural environments with silver raise questions about the toxicity of Ag(+) in the ecosystem. Natural organic matter, NOM, which is abundant in water supplies, soil, and sediments, can form stable complexes with Ag(+), altering its bioavailability and toxicity. Herein, the extent and kinetics of Ag(+) binding to NOM, matrix effects on Ag(+) binding to NOM, and the effect of NOM on Ag(+) toxicity to Shew ...[more]

PMID: 26284896

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Project description:Vegetation fires are known to have broad geochemical effects on carbon (C) cycles in the Earth system, yet limited information is available for nitrogen (N). In this study, we evaluated how charring organic matter (OM) to pyrogenic OM (PyOM) altered the N molecular structure and affected subsequent C and N mineralization. Nitrogen near-edge X-ray absorption fine structure (NEXAFS) of uncharred OM, PyOM, PyOM toluene extract, and PyOM after toluene extraction were used to predict PyOM-C and -N mineralization potentials. PyOM was produced from three different plants (e.g. Maize-Zea mays L.; Ryegrass-Lollium perenne L.; and Willow-Salix viminalix L.) each with varying initial N contents at three pyrolysis temperatures (350, 500 and 700?°C). Mineralization of C and N was measured from incubations of uncharred OM and PyOM in a sand matrix for 256?days at 30?°C. As pyrolysis temperature increased from 350 to 700?°C, aromatic C[bond, double bond]N in 6-membered rings (putative) increased threefold. Aromatic C[bond, double bond]N in 6-membered oxygenated ring increased sevenfold, and quaternary aromatic N doubled. Initial uncharred OM-N content was positively correlated with the proportion of heterocyclic aromatic N in PyOM (R2?=?0.44; P?<?0.0001; n?=?42). A 55% increase of aromatic N heterocycles at high OM-N content, when compared to low OM-N content, suggests that higher concentrations of N favor the incorporation of N atoms into aromatic structures by overcoming the energy barrier associated with the electronic and atomic configuration of the C structure. A ten-fold increase of aromatic C[bond, double bond]N in 6-membered rings (putative) in PyOM (as proportion of all PyOM-N) decreased C mineralization by 87%, whereas total N contents and C:N ratios of PyOM had no effects on C mineralization of PyOM-C for both pyrolysis temperatures (for PyOM-350?°C, R2?=?0.15; P?<?0.27; for PyOM-700?°C, R2?=?0.22; P?<?0.21). Oxidized aromatic N in PyOM toluene extracts correlated with higher C mineralization, whereas aromatic N in 6-membered heterocycles correlated with reduced C mineralization (R2?=?0.56; P?=?0.001; n?=?100). Similarly, aromatic N in 6-membered heterocycles in PyOM remaining after toluene extraction reduced PyOM-C mineralization (R2?=?0.49; P?=?0.0006; n?=?100). PyOM-C mineralization increased when N atoms were located at the edge of the C network in the form of oxidized N functionalities or when more N was found in PyOM toluene extracts and was more accessible to microbial oxidation. These results confirm the hypothesis that C persistence of fire-derived OM is significantly affected by its molecular N structure and the presented quantitative structure-activity relationship can be utilized for predictive modeling purposes.

Project description:The determination of copper (Cu) speciation and its bioavailability in natural waters is an important issue due to its specific role as an essential micronutrient but also a toxic element at elevated concentrations. Here, we report an improved anodic stripping voltammetry (ASV) method for organic Cu speciation, intended to eliminate the important problem of surface-active substances (SAS) interference on the voltammetric signal, hindering measurements in samples with high organic matter concentration. The method relies on the addition of nonionic surfactant Triton-X-100 (T-X-100) at a concentration of 1 mg L-1. T-X-100 competitively inhibits the adsorption of SAS on the Hg electrode, consequently 1) diminishing SAS influence during the deposition step and 2) strongly improving the shape of the stripping Cu peak by eliminating the high background current due to the adsorbed SAS, making the extraction of Cu peak intensities much more convenient. Performed tests revealed that the addition of T-X-100, in the concentration used here, does not have any influence on the determination of Cu complexation parameters and thus is considered "interference-free." The method was tested using fulvic acid as a model of natural organic matter and applied for the determination of Cu speciation in samples collected in the Arno River estuary (Italy) (in spring and summer), characterized by a high dissolved organic carbon (DOC) concentration (up to 5.2 mgC L-1) and anthropogenic Cu input during the tourist season (up to 48 nM of total dissolved Cu). In all the samples, two classes of ligands (denoted as L1 and L2) were determined in concentrations ranging from 3.5 ± 2.9 to 63 ± 4 nM eq Cu for L1 and 17 ± 4 to 104 ± 7 nM eq Cu for L2, with stability constants logK Cu,1 = 9.6 ± 0.2-10.8 ± 0.6 and logK Cu,2 = 8.2 ± 0.3-9.0 ± 0.3. Different linear relationships between DOC and total ligand concentrations between the two seasons suggest a higher abundance of organic ligands in the DOM pool in spring, which is linked to a higher input of terrestrial humic substances into the estuary. This implies that terrestrial humic substances represent a significant pool of Cu-binding ligands in the Arno River estuary.

Dataset Information

Dynamic silver speciation as studied with fluorous-phase ion-selective electrodes: Effect of natural organic matter on the toxicity and speciation of silver.

Publications

Dynamic silver speciation as studied with fluorous-phase ion-selective electrodes: Effect of natural organic matter on the toxicity and speciation of silver.

Similar Datasets

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