Fate of the antibiotic sulfadiazine in natural soils: Experimental and numerical investigations (original) (raw)
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Dynamics of transformation of the veterinary antibiotic sulfadiazine in two soils
Chemosphere, 2014
We show transformation and sequestration of the antibiotic sulfadiazine in two soils. Transformation products were found in liquid phase and extracts from the sorbed phase. We used a compartment model including all species and did global optimization. Sorption and transformation are concentration dependent.
Journal of Contaminant Hydrology, 2009
Concerning the transport of the veterinary antibiotic sulfadiazine (SDZ) little is known about its possible degradation during transport. Also its sorption behaviour is not yet completely understood. We investigated the transport of SDZ in soil columns with a special emphasis on the detection of transformation products in the outflow of the soil columns and on modelling of the concentration distribution in the soil columns afterwards. We used disturbed soil columns near saturation, packed with a loamy sand and a silty loam. SDZ was applied as a 0.57 mg L − 1 solution at a constant flow rate of 0.25 cm h − 1 for 68 h. Breakthrough curves (BTC) of SDZ and its transformation products 4-(2-iminopyrimidin-1(2H)-yl)aniline and 4-hydroxy-SDZ were measured for both soils. For the silty loam we additionally measured a BTC for an unknown transformation product which we only detected in the outflow samples of this soil. After the leaching experiments the 14 C-concentration was quantified in different layers of the soil columns. The transformation rates were low with mean SDZ mass fractions in the outflow samples of 95% for the loamy sand compared to 97% for the silty loam. The formation of 4-(2-iminopyrimidin-1(2H)yl)aniline appears to be light dependent and did probably not occur in the soils, but afterwards. In the soil columns most of the 14 C was found near the soil surface. The BTCs in both soils were described well by a model with one reversible (kinetic) and one irreversible sorption site. Sorption kinetics played a more prominent role than sorption capacity. The prediction of the 14 C -concentration profiles was improved by applying two empirical models other than first order to predict irreversible sorption, but also these models were not able to describe the 14 C concentration profiles correctly. Irreversible sorption of sulfadiazine still is not well understood.
Sorption, Fate, and Mobility of Sulfonamides in Soils
Water, Air, & Soil Pollution, 2011
Sulfonamides (SAs) are one of the broadly used antibiotics in domestic animal operations and have a notable potential of entering the environment through animal manure management practices. In this study, sulfamethazine (SMZ) was used as a prototype to study the sorption, fate, and transport of SAs in soil-water systems using batch and miscibledisplacement experiments. Sulfamethazine was degraded to a polar metabolite (PM). The batch experiments indicated that the linear sorption partitioning coefficient (K d ) values for the PM ranged from 7.5 to 206.2 L kg −1 . Strong relationships between the sorption of PM and various soil fractions and organic matter were also observed. The miscibledisplacement experiments showed that 33-70% of SMZ was degraded within 6 h during transport in the soil columns. Also, 69-99.7% of SMZ and PM were recovered in the effluents suggesting their high mobility. Also, the simultaneous degradation, sorption, and transport of SMZ and PM were described using a two-site chemical nonequilibrium fate and transport model, using the K d values obtained from the batch experiments. The parameters of this model were uniquely estimated using a global optimization strategy, the stochastic ranking evolutionary strategy.
Analysis, fate and effects of the antibiotic sulfadiazine in soil ecosystems
TrAC Trends in Analytical Chemistry, 2009
This review summarizes current knowledge about the interplay between fate and effects of the antibiotic sulfadiazine in soil ecosystems. In applying manure from antibiotic-treated animals to arable soils, sulfadiazine can reach the environment, but fate and transformation processes and the consequences for soil microorganisms and soil functions have not been studied adequately. Since antibiotics are explicitly designed to affect microorganisms, they are likely to affect ''non-target'' microbes in the soil ecosystem. Recent papers provide new insights into the disappearance dynamics of sulfadiazine, its effects on distinct microbial communities and the development of antibiotic resistance. ª
The sorption and transport of a sulphonamide antibiotic in soil systems
Toxicology letters, 2002
Veterinary medicines are administered to animals to treat disease and protect their health. After administration, the substances can be metabolised and a mixture of the parent compound and metabolites may be excreted in the urine and faeces. For animals on pasture, the excreta will be released directly to soil whereas for intensively reared animals, the main route of entry will be through slurry and manure spreading. Whilst the behaviour of other classes of substance (e.g. pesticides and nutrients) that are applied to soil is well understood, limited information is available on the transport and fate of veterinary medicines applied to soils. Laboratory and field studies were, therefore, performed to investigate the sorption behaviour of the sulfonamide antibiotic, sulfachloropyridazine, in soil and to assess the potential for sulfachloropyridazine to move from soil to surface waters and groundwaters. Sorption coefficients (K D ) for the compound in soil and soil/slurry mixtures were low (ranging from 0.9 to 1.8 l kg − 1 ) and indicated that the substance would be highly mobile. Field studies on a clay field supported these observations and demonstrated that, after application, the compound was rapidly transported to surface waters, concentrations of up to 590 mg l − 1 being observed in drainage waters. Leaching studies at a sandy site indicated that the substance had a low potential to leach to groundwaters, concentrations in the soil pore water being below or close to analytical detection limits. An assessment of currently available models for predicting concentrations of veterinary medicines entering surface waters indicated that for sulfachloropyridazine, the methods provide reasonable estimates, predicted concentrations being within a factor of two of the maximum measured concentrations. The approaches may not, however, be appropriate for use on highly hydrophobic substances or for predicting groundwater concentrations.
Impacts of Global Climate Change, 2005
Veterinary antibiotics used in livestock operations have been identified as one of the major sources of antibiotics in the environment. Antibiotics, such as sulfonamides, used in feedlots are excreted in a partially metabolized form in the urine and fecal material of livestock animals. The current practice of land application of untreated lagoon waste from livestock operations has a serious potential to contaminate groundwater. This paper intends to elucidate some of the key aspects of the mobility of sulfonamides, such as sulfachloropyridazine (SCPD) and sulfamerazine (SMRZ), in the environment. To achieve this objective, column studies were performed for SCPD and SMRZ in three soils: Missouri loam, North Carolina loamy sand, and Iowa sandy loam. A pulse containing a suite of eight antibiotics was injected instantaneously and the filtrate was analyzed for antibiotics concentrations. In all three soils, based on the initial soil pH, both SCPD and SMRZ were observed to be highly mobile at high pH value; however, significant retardation was observed at lower pH. Enhanced mobility of these compounds observed at high pH was due to the cumulative effect of the anionic form of antibiotics, the polar nature of soil material, and the increased solubility observed at high pH value. Conversely, severe attenuation of these compounds observed at lower pH values was due to the increased interaction of cationic and neutral forms of antibiotics with soil material. The recoveries and the sorption experiment performed for SCPD and Iowa sandy loam indicated that the mobility of sulfonamides, in general, is contingent upon the alkalinity of the soil. Considerable decrease in the sorption coefficient was observed at high pH value.
Long-Term Sorption and Desorption of Sulfadiazine in Soil: Experiments and Modeling
Journal of Environmental Quality, 2010
Antibiotics, such as sulfadiazine (SDZ), may enter arable soil by spreading of manure of medicated husbandry or directly by the excrement of grazing animals. Knowledge of the fate of antibiotics in soils is crucial for assessing the environmental risk of these compounds, including possible transport to ground water. Kinetic sorption of 14 C-labeled SDZ (4-amino-N-pyrimidin-2-yl-benzenesulfonamide) was investigated using the batch technique. Th e batch sorption-desorption experiments were conducted at various concentration levels (0.044-13 mg L −1 initial solute concentration) and time scales (0.75-272 d). Sorption of 14 C-SDZ in the investigated silty loam was time dependent and strongly nonlinear in the solution phase concentration. Th e time to reach an apparent sorption equilibrium was about 20 d. However, desorption was very slow, and 41 d were insuffi cient to reach the desorption equilibrium. An inverse modeling technique was used to identify relevant sorption processes of 14 C-SDZ during the batch experiments. Among the investigated two-and three-domain sorption models, adsorption and desorption of 14 C-SDZ were best described with a new model defi ning two sorption domains and four parameters. Whereas sorption in the fi rst sorption domain was nonlinear and instantaneous, solute uptake in the second sorption domain was rate limited following fi rst-order kinetics. Desorption followed the same rate law until an equilibrium distribution was reached. After that, desorption was assumed to be impossible due to partly irreversible sorption. Although the proposed model needs further validation, it contributes to the discussion on complex sorption processes of organic chemicals in soils.
Sulfadiazine dissipation in acidic tropical soils
Environmental Science and Pollution Research, 2020
Sulfadiazine (SDZ) residues have been detected in manured soils as well as their adjacent water resources, but its behavior is still poorly understood in acidic tropical soils. This research aimed to evaluate sorption, leaching, and biodegradation of 14 C-SDZ in four acidic soils from Brazil, using OECD guidelines. Except for the sand soil (K d = 2.6 L kg −1), SDZ sorption tended to be higher (K d > 8.4 L kg −1) and more hysteretic (ΔH >> 1) in acidic soils. When freshly applied, SDZ leaching was low (< 0.11% of applied radioactivity (AR)) and could not always be predicted by K d values; but leaching was restricted when SDZ was aged for 62 days. SDZ mineralization was low (< 3%) but its dissipation was fast (DT 50 < 2.3 days and DT 90 < 6.3 days) due to fast initial degradation (an unknown metabolite was immediately formed, likely 4-hydroxysulfadiazine) and mainly to fast formation of non-extractable residues (NER) (> 78% of AR up to 7 days). For certain acidic soils, the abrupt breakdown of the SDZ suggests that degradation should be initially chemical and then followed by enzymatically driven reactions. The fast formation of NERs was attributed mostly to chemical bounding to soil humic substances (Type II-NER), but SDZ sequestration cannot be ruled out (Type I-NER). NERs represent a long-term environmental reservoir of SDZ that may cause deleterious effects on non-target organisms as well as promote antibiotic resistance to soil microbes.
Sorption of Sulfonamide Pharmaceutical Antibiotics on Whole Soils and Particle-Size Fractions
Journal of Environment Quality, 2004
Sørensen, 2000). Consequently, residues of potentially harmful pharmaceutical antibiotics are found in soils Residues of pharmaceutical antibiotics are found in the environand adjacent environmental compartments (Hirsch et ment, whose fate and effects are governed by sorption. Thus, the extent and mechanisms of the soil sorption of p-aminobenzoic acid and al., 1999; Hamscher et al., 2002). Numerous pharmaceufive sulfonamide antibiotics (sulfanilamide, sulfadimidine, sulfadia-tical antibiotics are persistent in the environment (Gazine, sulfadimethoxine, and sulfapyridine) were investigated using topvalchin and Katz, 1994; Hamscher et al., 2002). Hence, soils of fertilized and unfertilized Chernozem and their organic-minthey can enter the food chain via uptake by plants or eral particle-size fractions. Freundlich adsorption coefficients (K f) translocation into ground water (Migliore et al., 1995; ranged from 0.5 to 6.5. Adsorption increased with aromaticity and Boxall et al., 2002). In addition, antibiotics can provoke electronegativity of functional groups attached to the sulfonyl-phenylthe formation of resistant microorganisms (Huysman et amine core. Adsorption to soil and particle-size fractions increased al., 1993; Gavalchin and Katz, 1994). The translocation in the sequence: coarse silt Ͻ whole soil Ͻ medium silt Ͻ sand Ͻ and bioactivity of antibiotics are influenced by soil sorpclay Ͻ fine silt and was influenced by pH. Sorption nonlinearity (1/n Յ tion, governing the distribution and transfer between 0.76) indicated specific interactions with functional groups of soil organic matter (SOM). Phenolic and carboxylic groups, N-hetero-phases and thus the resulting mobile and bioavailable cyclic compounds, and lignin decomposition products were tentatively fractions of the antibiotics. However, knowledge about assigned as preferred binding sites using statistical analysis of pyrolythe extent and mechanisms of antibiotic sorption in soils sis-mass spectra and adsorption coefficients. Adsorption of sulfonis still scarce (Thiele-Bruhn, 2003). amides to mineral soil colloids was weaker and resulted in a stronger As is with many other pharmaceuticals, sulfonamides desorption from clay-size fractions. Moreover, steric accessibility of are both fairly water-soluble and polar compounds, which organic-mineral complexes in clay-size fractions was significantly reionize depending on the pH of the matrix. In addition duced. With a quantitative structure-property relationship (QSPR) to hydrophobic partitioning, these compounds may sorb model, combining the organic carbon concentration, the sulfonamides' to soils via cation exchange, cation bridging, surface chromatographic capacity factor (k), and nondissociated species concentration (CF a), distribution coefficients (K d) were estimated with a complexes, and hydrogen bonding (Tolls, 2001). Accordcross-validated regression coefficient Q 2 ϭ 0.71. Modeling and molecingly, sorption of sulfonamides, such as sulfapyridine, ular mechanics calculations of antibiotic-SOM complexes showed varies between soils and is affected by the quantity, compreferred site-specific sorption via hydrogen bonds and van der Waals position, and structure of soil colloids (Thiele, 2000). The interactions. Distinct chemical structural properties, such as aromaticeffects of the variation in quantity and quality of soil ity and van der Waals volumes, correlated with the sorption data. components can be elucidated in sorption experiments using particle-size fractions obtained from physical separation of whole-soil samples. These fractions contain A ntibiotic pharmaceuticals are widely used for the mineral colloids and soil organic matter (SOM) of differ
The Science of the total environment, 2014
Adsorption and desorption are important processes that influence the transport, transformation and bioavailability of antimicrobials in soils. The adsorption-desorption characteristics of sulfadimethoxine, sulfaquinoxaline and sulfamethazine in Brazilian soils (sandy, sandy-clay and clay) were evaluated using the batch equilibrium method. The sulfonamides were quantified in the soil solutions by a previously in house validated HPLC-PAD method. The adsorption/desorption data for the sulfonamides in soils fit the Freundlich isotherms well in the logarithmic form. The Freundlich adsorption coefficients ranged from 1.4 to 19.0 μg(1-1/n)(cm(3))(1/n)g(-1), suggesting that all of the sulfonamides weakly adsorbed on the evaluated soils. The Freundlich desorption coefficients ranged from 0.85 to 24.8 μg(1-1/n)(cm(3))(1/n)g(-1), indicating that the sulfonamides tend to be leached from soils with high sand and low organic carbon contents, suggesting that there is high potential for surface and...