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1.
Anal Bioanal Chem ; 403(9): 2503-18, 2012 Jul.
Article in English | MEDLINE | ID: mdl-22543693

ABSTRACT

An overview is given of existing trace analytical methods for the determination of seven popular artificial sweeteners [acesulfame (ACE), aspartame, cyclamate (CYC), neotame, neohesperidine dihydrochalcone, saccharin (SAC), and sucralose (SUC)] from aqueous environmental samples. Liquid chromatography-electrospray ionization tandem mass spectrometry and liquid chromatography-electrospray ionization high-resolution mass spectrometry are the methods most widely applied, either directly or after solid-phase extraction. Limits of detection and limits of quantification down to the low nanogram per liter range can be achieved. ACE, CYC, SAC, and SUC were detected in wastewater treatment plants in high microgram per liter concentrations. Per capita loads of individual sweeteners can vary within a wide range depending on their use in different countries. Whereas CYC and SAC are usually degraded by more than 90% during wastewater treatment, ACE and SUC pass through wastewater treatment plants mainly unchanged. This suggests their use as virtually perfect markers for the study of the impact of wastewater on source waters and drinking waters. In finished water of drinking water treatment plants using surface-water-influenced source water, ACE and SUC were detected in concentrations up to 7 and 2.4 µg/L, respectively. ACE was identified as a precursor of oxidation byproducts during ozonation, resulting in an aldehyde intermediate and acetic acid. Although the concentrations of ACE and SUC are among the highest measured for anthropogenic trace pollutants found in surface water, groundwater, and drinking water, the levels are at least three orders of magnitude lower than organoleptic threshold values. However, ecotoxicology studies are scarce and have focused on SUC. Thus, further research is needed both on identification of transformation products and on the ecotoxicological impact of artificial sweeteners and their transformation products.


Subject(s)
Chromatography, Liquid/methods , Solid Phase Extraction/methods , Spectrometry, Mass, Electrospray Ionization/methods , Sweetening Agents/analysis , Water Pollutants, Chemical/analysis , Water Purification/methods , Drinking Water/analysis , Fresh Water/analysis , Groundwater/analysis , Sewage/analysis
2.
Water Res ; 44(12): 3573-84, 2010 Jun.
Article in English | MEDLINE | ID: mdl-20462625

ABSTRACT

Due to incomplete removal of artificial sweeteners in wastewater treatment plants some of these compounds end up in receiving surface waters, which are used for drinking water production. The sum of removal efficiency of single treatment steps in multi-barrier treatment systems affects the concentrations of these compounds in the provided drinking water. This is the first systematic study revealing the effectiveness of single treatment steps in laboratory experiments and in waterworks. Six full-scale waterworks using surface water influenced raw water were sampled up to ten times to study the fate of acesulfame, saccharin, cyclamate and sucralose. For the most important treatment technologies the results were confirmed by laboratory batch experiments. Saccharin and cyclamate proved to play a minor role for drinking water treatment plants as they were eliminated by nearly 100% in all waterworks with biologically active treatment units like river bank filtration (RBF) or artificial groundwater recharge. Acesulfame and sucralose were not biodegraded during RBF and their suitability as wastewater tracers under aerobic conditions was confirmed. Sucralose proved to be persistent against ozone and its transformation was < 20% in lab and field investigations. Remaining traces were completely removed by subsequent granular activated carbon (GAC) filters. Acesulfame readily reacts with ozone (pseudo first-order rate constant k = 1.3 x 10(-3) s(-1) at 1 mg L(-1) ozone concentration). However, the applied ozone concentrations and contact times under typical waterworks conditions only led to an incomplete removal (18-60%) in the ozonation step. Acesulfame was efficiently removed by subsequent GAC filters with a low throughput of less than 30 m(3) kg(-1), but removal strongly depended on the GAC preload. Thus, acesulfame was detected up to 0.76 microg L(-1) in finished water.


Subject(s)
Sweetening Agents/isolation & purification , Water Purification/methods , Water Purification/standards , Water Supply/analysis , Biodegradation, Environmental/drug effects , Bioreactors , Charcoal/chemistry , Filtration , Flocculation/drug effects , Germany , Halogenation/drug effects , Laboratories , Ozone/pharmacology
3.
Anal Bioanal Chem ; 394(6): 1585-94, 2009 Jul.
Article in English | MEDLINE | ID: mdl-19533103

ABSTRACT

A method for the simultaneous determination of seven commonly used artificial sweeteners in water is presented. The analytes were extracted by solid phase extraction using Bakerbond SDB 1 cartridges at pH 3 and analyzed by liquid chromatography electrospray ionization tandem mass spectrometry in negative ionization mode. Ionization was enhanced by post-column addition of the alkaline modifier Tris(hydroxymethyl)amino methane. Except for aspartame and neohesperidin dihydrochalcone, recoveries were higher than 75% in potable water with comparable results for surface water. Matrix effects due to reduced extraction yields in undiluted waste water were negligible for aspartame and neotame but considerable for the other compounds. The widespread distribution of acesulfame, saccharin, cyclamate, and sucralose in the aquatic environment could be proven. Concentrations in two influents of German sewage treatment plants (STPs) were up to 190 microg/L for cyclamate, about 40 microg/L for acesulfame and saccharin, and less than 1 microg/L for sucralose. Removal in the STPs was limited for acesulfame and sucralose and >94% for saccharin and cyclamate. The persistence of some artificial sweeteners during soil aquifer treatment was demonstrated and confirmed their environmental relevance. The use of sucralose and acesulfame as tracers for anthropogenic contamination is conceivable. In German surface waters, acesulfame was the predominant artificial sweetener with concentrations exceeding 2 microg/L. Other sweeteners were detected up to several hundred nanograms per liter in the order saccharin approximately cyclamate > sucralose.


Subject(s)
Fresh Water/chemistry , Sweetening Agents/analysis , Waste Disposal, Fluid , Water Pollutants, Chemical/analysis , Water Purification , Chromatography, Liquid , Germany , Molecular Structure , Sewage/chemistry , Soil , Sweetening Agents/chemistry , Tandem Mass Spectrometry
4.
Environ Sci Technol ; 39(6): 1523-31, 2005 Mar 15.
Article in English | MEDLINE | ID: mdl-15819205

ABSTRACT

Sulfonated naphthalene-formaldehyde condensates (SNFC) are high production volume chemicals used in a variety of applications, for example, as concrete plasticizers, tanning agents, or dye dispersants. They enter the aquatic environment primarily by the wastewater path. The occurrence and fate of the monomers, which are different isomers of mono- and disulfonated naphthalene, was intensively investigated in previous studies. However, the environmental fate of the persistent higher molecular SNFC is so far widely unknown. This paper describes an ultrasonic extraction under alkaline conditions, followed by ion-pair HPLC with fluorescence detection for the analysis of SNFC oligomers from solid environmental matrixes such as sewage sludge, suspended solids, and river sediments. Limits of quantification of about 0.1 mg kg-1 d.m. were well below the measured concentrations in environmental samples. SNFC were adsorbed to suspended solids and river sediments in three major German rivers (Rhine, Neckar, and Danube) in concentrations typically up to several mg kg(-1) d.m. A total content of about 4 g kg(-1) d.m. was measured in a sewage sludge of a municipal wastewater treatment plant, which receives wastewater from a textile dyeing plant. Furthermore, the first quantitative field data on the partition of SNFC and their monomers between the aqueous phase and solid environmental compartments are presented. Solid-liquid partition coefficients (Kd) of oligomers with a chain-length ranging from three to six naphthalenesulfonate units were derived from the analysis of corresponding wastewater and sewage sludge samples and from suspended solids and river water samples, respectively. Determined Kd values were in the range from 10(2) to 10(4) L kg(-1).


Subject(s)
Disinfectants/chemistry , Formaldehyde/chemistry , Models, Theoretical , Naphthalenesulfonates/chemistry , Water Pollutants, Chemical/analysis , Chromatography, High Pressure Liquid , Solubility , Waste Disposal, Fluid
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