Nickel Speciation and Complexation Kinetics in Freshwater by Ligand Exchange and DPCSV
A technique of ligand exchange with DMG (dimethylglyoxime) and DPCSV was applied to determine Ni speciation in lake, river, and groundwater samples. The working conditions related to ligand-exchange equilibrium were optimized, and the ligand-exchange kinetics were examined. The observed pseudo-first...
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Published in | Environmental science & technology Vol. 35; no. 3; pp. 539 - 546 |
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Main Authors | , , , |
Format | Journal Article |
Language | English |
Published |
Washington, DC
American Chemical Society
01.02.2001
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Abstract | A technique of ligand exchange with DMG (dimethylglyoxime) and DPCSV was applied to determine Ni speciation in lake, river, and groundwater samples. The working conditions related to ligand-exchange equilibrium were optimized, and the ligand-exchange kinetics were examined. The observed pseudo-first-order rate, k obsd, was about 3 × 10-5 (s-1) for Ni(DMG)2 complex formation with an excess of DMG (μM) over Ni (nM) at pH 7.1−7.7. The second-order exchange kinetic constants, k exch, were between 1.2 × 102 and 5.7 × 103 s-1 M-1 for ligand exchange of NiEDTA with DMG and between 5 × 102 and 7 × 103 s-1 M-1 for exchange of natural ligands with DMG in the freshwater samples under similar conditions. Ni ligand exchange between natural ligands and DMG occurred over days with half-lifes of 5−95 h. Total dissolved Ni concentrations in samples from various freshwater systems in Switzerland ranged from 4 nM in an oligotrophic lake to 30 nM in a small river affected by inputs from sewage effluents and agriculture. Free ionic Ni2+ concentrations were determined in the range of 10-13−10-15 M (pNi =12.2−14.7), indicating that more than 99.9% of dissolved Ni was bound by organic ligands with strong affinity (log K 12.1−14.9) and low concentrations (13−100 nM) at pH 7.2−8.2. Because of slow ligand-exchange kinetics, Ni speciation in natural waters may in many cases not reach equilibrium. |
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AbstractList | A technique of ligand exchange with DMG (dimethylglyoxime) and DPCSV was applied to determine Ni speciation in lake, river, and groundwater samples. The working conditions related to ligand-exchange equilibrium were optimized, and the ligand-exchange kinetics were examined. The observed pseudo-first-order rate, kobsd, was about 3 x 10-5 (s-1) for Ni(DMG)2 complex formation with an excess of DMG (M) over Ni (nM) at pH 7.1-7.7. The second-order exchange kinetic constants, kexch, were between 1.2 x 102 and 5.7 x 103 s-1 M-1 for ligand exchange of NiEDTA with DMG and between 5 x 102 and 7 x 103 s-1 M-1 for exchange of natural ligands with DMG in the freshwater samples under similar conditions. Ni ligand exchange between natural ligands and DMG occurred over days with half-lifes of 5-95 h. Total dissolved Ni concentrations in samples from various freshwater systems in Switzerland ranged from 4 nM in an oligotrophic lake to 30 nM in a small river affected by inputs from sewage effluents and agriculture. Free ionic Ni2 concentrations were determined in the range of 10-13-10-15 M (pNi =12.2-14.7), indicating that more than 99.9␘f dissolved Ni was bound by organic ligands with strong affinity (log K 12.1-14.9) and low concentrations (13-100 nM) at pH 7.2-8.2. Because of slow ligand-exchange kinetics, Ni speciation in natural waters may in many cases not reach equilibrium A technique of ligand exchange with DMG (dimethylglyoxime) and DPCSV was applied to determine Ni speciation in lake, river, and groundwater samples. The working conditions related to ligand-exchange equilibrium were optimized, and the ligand-exchange kinetics were examined. The observed pseudo-first-order rate, k sub(obsd), was about 3 x 10 super(-5) (s super(-1)) for Ni(DMG) sub(2) complex formation with an excess of DMG ( mu M) over Ni (nM) at pH 7.1-7.7. The second-order exchange kinetic constants, k sub(exch), were between 1.2 x 10 super(2) and 5.7 x 10 super(3) s super(-1) M super(-1) for ligand exchange of NiEDTA with DMG and between 5 x 10 super(2) and 7 x 10 super(3) s super(-1) M super(-1) for exchange of natural ligands with DMG in the freshwater samples under similar conditions. Ni ligand exchange between natural ligands and DMG occurred over days with half-lifes of 5-95 h. Total dissolved Ni concentrations in samples from various freshwater systems in Switzerland ranged from 4 nM in an oligotrophic lake to 30 nM in a small river affected by inputs from sewage effluents and agriculture. Free ionic Ni super(2+) concentrations were determined in the range of 10 super(-13)-10 super(-15) M (pNi =12.2-14.7), indicating that more than 99.9% of dissolved Ni was bound by organic ligands with strong affinity (log K 12.1-14.9) and low concentrations (13-100 nM) at pH 7.2-8.2. Because of slow ligand-exchange kinetics, Ni speciation in natural waters may in many cases not reach equilibrium. A technique of ligand exchange with DMG (dimethylglyoxime) and DPCSV was applied to determine Ni speciation in lake, river, and groundwater samples. The working conditions related to ligand-exchange equilibrium were optimized, and the ligand-exchange kinetics were examined. The observed pseudo-first-order rate, k obsd, was about 3 × 10-5 (s-1) for Ni(DMG)2 complex formation with an excess of DMG (μM) over Ni (nM) at pH 7.1−7.7. The second-order exchange kinetic constants, k exch, were between 1.2 × 102 and 5.7 × 103 s-1 M-1 for ligand exchange of NiEDTA with DMG and between 5 × 102 and 7 × 103 s-1 M-1 for exchange of natural ligands with DMG in the freshwater samples under similar conditions. Ni ligand exchange between natural ligands and DMG occurred over days with half-lifes of 5−95 h. Total dissolved Ni concentrations in samples from various freshwater systems in Switzerland ranged from 4 nM in an oligotrophic lake to 30 nM in a small river affected by inputs from sewage effluents and agriculture. Free ionic Ni2+ concentrations were determined in the range of 10-13−10-15 M (pNi =12.2−14.7), indicating that more than 99.9% of dissolved Ni was bound by organic ligands with strong affinity (log K 12.1−14.9) and low concentrations (13−100 nM) at pH 7.2−8.2. Because of slow ligand-exchange kinetics, Ni speciation in natural waters may in many cases not reach equilibrium. A technique of ligand exchange with DMG (dimethylglyoxime) and DPCSV was applied to determine Ni speciation in lake, river, and groundwater samples. The working conditions related to ligand-exchange equilibrium were optimized, and the ligand-exchange kinetics were examined. A technique of ligand exchange with DMG (dimethylglyoxime) and DPCSV was applied to determine Ni speciation in lake, river, and groundwater samples. The working conditions related to ligand-exchange equilibrium were optimized, and the ligand-exchange kinetics were examined. The observed pseudo-first-order rate, kobsd, was about 3 x 10(-5) (s-1) for Ni(DMG)2 complex formation with an excess of DMG (microM) over Ni (nM) at pH 7.1-7.7. The second-order exchange kinetic constants, kexch, were between 1.2 x 10(2) and 5.7 x 10(3) s-1 M-1 for ligand exchange of NiEDTA with DMG and between 5 x 10(2) and 7 x 10(3) s-1 M-1 for exchange of natural ligands with DMG in the freshwater samples under similar conditions. Ni ligand exchange between natural ligands and DMG occurred over days with half-lifes of 5-95 h. Total dissolved Ni concentrations in samples from various freshwater systems in Switzerland ranged from 4 nM in an oligotrophic lake to 30 nM in a small river affected by inputs from sewage effluents and agriculture. Free ionic Ni2+ concentrations were determined in the range of 10(-13)-10(-15) M (pNi = 12.2-14.7), indicating that more than 99.9% of dissolved Ni was bound by organic ligands with strong affinity (log K 12.1-14.9) and low concentrations (13-100 nM) at pH 7.2-8.2. Because of slow ligand-exchange kinetics, Ni speciation in natural waters may in many cases not reach equilibrium. |
Author | Jansen, Stefan Sigg, Laura Xue, Han Bin Prasch, Andreas |
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Keywords | Complexation Organic matter Pollutant behavior Geochemistry Oxime Stability constant Nickel Water pollution Experimental study Chemical reaction kinetics Speciation Heavy metal |
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Snippet | A technique of ligand exchange with DMG (dimethylglyoxime) and DPCSV was applied to determine Ni speciation in lake, river, and groundwater samples. The... |
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SubjectTerms | Applied sciences Biological and physicochemical phenomena Earth sciences Earth, ocean, space Engineering and environment geology. Geothermics Environmental impact Exact sciences and technology Kinetics Laboratorium voor Fysische chemie en Kolloïdkunde Ligands Metals Models, Theoretical Natural water pollution Nickel - chemistry Oximes Physical Chemistry and Colloid Science Pollution Pollution, environment geology Sewage Soils Switzerland Water Pollutants - analysis Water pollution Water treatment and pollution WIMEK |
Title | Nickel Speciation and Complexation Kinetics in Freshwater by Ligand Exchange and DPCSV |
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