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1.
Sci Total Environ ; 917: 170537, 2024 Mar 20.
Article En | MEDLINE | ID: mdl-38301792

Sulfonamide antibiotics (SAs) are widely used as a broad-spectrum antibiotic, leading to global concerns due to their potential soil accumulation and subsequent effects on ecosystems. SAs often exhibit remarkable environmental persistence, necessitating further investigation to uncover the ultimate destiny of these molecules. In this work, molecular dynamics simulations combined with complementary quantum chemistry calculations were employed to investigate the influence of pH on the behavior of sulfadiazine (SDZ, a typical SAs) in soil particle models (silica, one of the main components of soil). Meanwhile, the quantification of SDZ molecules aggregation potential onto silica was further extended. SDZ molecules tend to form a monolayer on the soil surface under acidic conditions while forming aggregated adsorption on the surface under neutral conditions. Due to the hydrophilicity of the silica, multiple hydration layers would form on its surface, hindering the further adsorption of SDZ molecules on its surface. The calculated soil-water partition coefficient (Psoil/water) of SDZ+ and SDZ were 9.01 and 7.02, respectively. The adsorption evaluation and mechanisms are useful in controlling the migration and transformation of SAs in the soil environment. These findings provide valuable insights into the interactions between SDZ and soil components, shedding light on its fate and transport in the environment.


Anti-Bacterial Agents , Soil Pollutants , Anti-Bacterial Agents/analysis , Sulfadiazine/analysis , Soil/chemistry , Ecosystem , Sulfonamides , Sulfanilamide , Soil Pollutants/analysis , Silicon Dioxide , Water , Hydrogen-Ion Concentration
2.
J Hazard Mater ; 467: 133667, 2024 Apr 05.
Article En | MEDLINE | ID: mdl-38325102

Activated sludge extracellular polymeric substances (ASEPSs) comprise most dissolved organic matters (DOMs) in the tail water. However, the understanding of the link between the photolysis of antibiotic and the photo-reactivity/photo-persistence of ASEPS components is limited. This study first investigated the photochemical behaviors of ASEPS's components (humic acids (HA), hydrophobic substances (HOS) and hydrophilic substances (HIS)) separated from municipal sludge's EPS (M-EPS) and nitrification sludge's EPS (N-EPS) in the photolysis of sulfadiazine (SDZ). The results showed that 60% of SDZ was removed by the M-EPS, but the effect in the separated components was weakened, and only 24% - 39% was degraded. However, 58% of SDZ was cleaned by HOS in N-EPS, which was 23% higher than full N-EPS. M-EPS components had lower steady-state concentrations of triplet intermediates (3EPS*), hydroxyl radicals (·OH) and singlet oxygen (1O2) than M-EPS, but N-EPS components had the highest concentrations (5.96 ×10-15, 8.44 ×10-18, 4.56 ×10-13 M, respectively). The changes of CO, C-O and O-CO groups in HA and HOS potentially correspond to reactive specie's generation. These groups change little in HIS, which may make it have radiation resistance. HCO-3 and NO-3 decreased the indirect photolysis of SDZ, and its by-product N-(2-Pyrimidinyl)1,4-benzenediamine presents high environmental risk.


Extracellular Polymeric Substance Matrix , Sewage , Sewage/chemistry , Extracellular Polymeric Substance Matrix/chemistry , Sulfadiazine/analysis , Anti-Bacterial Agents/analysis , Photolysis , Humic Substances/analysis
3.
Chemosphere ; 351: 141226, 2024 Mar.
Article En | MEDLINE | ID: mdl-38228193

In this work, an electric field-enhanced heterogeneous catalytic ozonation (EHCO) was systematically investigated using a prepared FeOx/PAC catalyst. The EHCO process exhibited high sulfadiazine (SDZ) and TOC removal efficiency compared with electrocatalysis (EC) and heterogeneous catalytic ozonation (HCO) process. Almost 100% of SDZ was removed within 2 min, and the TOC removal reached approximately 85% within 60 min. Quenching experiments and EPR analysis suggested that the prominent SDZ and TOC removal performance is supported by the enhanced ·OH generation ability. Further study proved that H2O2 formed by O2 electrochemical reduction, peroxone reaction and electrochemical reduction of ozone contributed to improving ·OH generation. Furthermore, the EHCO system showed satisfactory stability and recyclability compared to conventional HCO systems, and the SDZ and TOC removal rates were maintained at ≥95% and ≥70% in 16 consecutive recycles, respectively. Meanwhile, XPS analysis and Boehm's titration for the FeOx/PAC catalyst used in HCO and EHCO process confirmed that the external electron supply could restrain the oxidation of surface functional groups of PAC and maintain a balance of the Fe(II)/Fe(III) ratio, which proved the critical role of cathode reduction in catalyst in situ regeneration during long consecutive recycles. In addition, the EHCO system could achieve more than 80% SDZ removal within 2 min in different water matrices. These results confirmed that the EHCO process has a wide application perspective for refractory organics removal in actual wastewater.


Ozone , Water Pollutants, Chemical , Water Purification , Hydrogen Peroxide , Ferric Compounds , Sulfadiazine/analysis , Water Pollutants, Chemical/analysis , Water Purification/methods , Ozone/analysis , Catalysis
4.
Sci Total Environ ; 893: 164857, 2023 Oct 01.
Article En | MEDLINE | ID: mdl-37321499

Sulfonamide antibiotics (SAs) are ubiquitous in surface water and soil environments, raising considerable concerns about their risk and removal. However, the impacts of various bromide ion (Br-) concentrations on the phytotoxicity, uptake and fate of SAs in plant growth and physiological metabolism of plants have not been well understood. Our research demonstrated that low concentrations of Br- (0.1, 0.5 mM) promoted the uptake and degradation of sulfadiazine (SDZ) in wheat and attenuated the phytotoxicity of SDZ. Additionally, we proposed a degradation pathway and identified the brominated product of SDZ (SDZBr), which attenuated the dihydrofolate synthesis inhibition by SDZ. The primary mechanism was that Br- reduced the level of reactive oxygen radicals (ROS) and alleviated oxidative damage. The production of SDZBr and the high consumption of H2O2 suggest the potential generation of reactive bromine species, contributing to the degradation of the electron-rich SDZ and thus reducing its toxicity. Moreover, metabolome analysis of wheat roots indicated that low concentrations of Br- stimulated the production of indoleacetic acid under SDZ stress, promoting growth and enhancing the uptake and degradation of SDZ. Conversely, high Br- (1 mM) concentration produced a deleterious effect. These findings provide valuable insights into the mechanisms of antibiotic removal, suggesting a potentially novel approach to plant-based antibiotic remediation.


Bromides , Sulfadiazine , Sulfadiazine/analysis , Bromides/toxicity , Bromides/analysis , Hydrogen Peroxide/analysis , Anti-Bacterial Agents/toxicity , Anti-Bacterial Agents/metabolism , Soil , Sulfanilamide
5.
Biosensors (Basel) ; 13(6)2023 Jun 03.
Article En | MEDLINE | ID: mdl-37366978

The monitoring of sulfadiazine (SDZ) is of great significance for food safety, environmental protection, and human health. In this study, a fluorescent aptasensor based on MnO2 and FAM-labeled SDZ aptamer (FAM-SDZ30-1) was developed for the sensitive and selective detection of SDZ in food and environmental samples. MnO2 nanosheets adsorbed rapidly to the aptamer through its electrostatic interaction with the base, providing the basis for an ultrasensitive SDZ detection. Molecular dynamics was used to explain the combination of SMZ1S and SMZ. This fluorescent aptasensor exhibited high sensitivity and selectivity with a limit of detection of 3.25 ng/mL and a linear range of 5-40 ng/mL. The recoveries ranged from 87.19% to 109.26% and the coefficients of variation ranged from 3.13% to 13.14%. In addition, the results of the aptasensor showed an excellent correlation with high-performance liquid chromatography (HPLC). Therefore, this aptasensor based on MnO2 is a potentially useful methodology for highly sensitive and selective detection of SDZ in foods and environments.


Aptamers, Nucleotide , Biosensing Techniques , Humans , Sulfadiazine/analysis , Manganese Compounds/chemistry , Oxides/chemistry , Fluorescent Dyes/chemistry , Aptamers, Nucleotide/chemistry , Limit of Detection , Biosensing Techniques/methods
6.
J Chromatogr A ; 1696: 463965, 2023 May 10.
Article En | MEDLINE | ID: mdl-37059046

In this study, on-line preconcentration and selective determination of the trace sulfadiazine (SDZ) existing in milk and hen egg white samples were realized by the capillary electrophoresis using molecularly imprinted polymer (MIP) coated capillary. The capillary coated with MIP was firstly prepared through the surface imprinted techniques, using SDZ as template molecule and dopamine as function monomer and crosslinker, and then amine-terminated poly(2-methyl-2-oxazoline) (PMOXA-NH2) was introduced onto polydopamine layer to reduce the non-specific adsorption. Successful preparation of SDZ-MIP-PMOXA coating was verified by zeta potential, as well as water contact angle. The SDZ-MIP-PMOXA coated capillary performed well on-line preconcentration of SDZ and the obtained peak area of SDZ was 46 times higher than that one obtained in bare capillary using the same procedure. Then the proposed on-line preconcentration method was fully validated and displayed good linear behavior in the concentration from 5.0 to 100.0 ng/mL, with the limit of detection was low to 1.5 ng/mL; and this method presented excellent accuracy and robustness. The prepared SDZ-MIP-PMOXA coated capillary also showed high selectivity with the imprinting factor of 5.85 and good repeatability during five consecutive runs with the relative standard deviation value of peak area was 1.6%. At last, the application of the prepared SDZ-MIP-PMOXA coated capillary in the detection of SDZ in spiked food samples was investigated, and good recoveries of 98.7-109.3% were obtained.


Molecular Imprinting , Sulfadiazine , Animals , Adsorption , Electrophoresis, Capillary/methods , Milk/chemistry , Molecular Imprinting/methods , Molecularly Imprinted Polymers , Sulfadiazine/analysis , Eggs/analysis
7.
Anal Chim Acta ; 1281: 341891, 2023 Nov 15.
Article En | MEDLINE | ID: mdl-38783737

BACKGROUND: Sulfadiazine (SDZ) is a broad-spectrum antibiotic widely used in aquaculture and animal husbandry and it is easy to remain in the water system to damage the human body. Therefore, detection and removal of sulfadiazine in water systems become critical. Nowadays, catalysts and visible light are used to degrade sulfadiazine into smaller molecules containing N and S to reduce toxicity. However, these small molecules are easily released into water and the atmosphere to be the acid rain. Therefore, it is urgent to design a sensor with the ability to detect and remove SDZ at the same time. (96) RESULTS: We designed a novel composite catalyst sensor (Sb6O13@LTA GCE) with the ability to simultaneously monitor and remove sulfadiazine. The catalyst is generated by introducing SbCl5 into the reactive gel of LTA (Linde Type A) structure zeolite. In the hydrothermal reaction, the corrosive SbCl5 is transferred into nanosized Sb6O13 nanoparticle which is highly dispersed in the opening nano-scaled windows of the zeolite through redox and self-assembled progress. In the selected electrochemical overpotential range, the Sb6O13@LTA composited modified electrode could complete adsorption and desorption of SDZ through the electron transfer from Sb3+ to Sb5+. As the catalyst is in high stability, the only loss in the whole process of recovering SDZ is a small amount of electric energy. The extra-low detection limit and the removal efficiency of Sb6O13@LTA GCE have been achieved 4.0 pM and 19.3 mg/20 mg (136) SIGNIFICANCE: The prepared novel sensor has low detection limit, high removal efficiency and high selectivity for sulfadiazine. The Sb6O13@LTA GCE sensor, which is low-cost and has a simple preparation method, exhibits good reproducibility in both seawater and cell fluid. This provides the possibility for wide application in detecting and removing SDZ in water system. (53).


Anti-Bacterial Agents , Antimony , Electrochemical Techniques , Oxidation-Reduction , Sulfadiazine , Sulfadiazine/analysis , Antimony/chemistry , Antimony/analysis , Anti-Bacterial Agents/analysis , Anti-Bacterial Agents/chemistry , Electrochemical Techniques/methods , Water Pollutants, Chemical/analysis , Limit of Detection , Electrodes , Catalysis , Oxides/chemistry
8.
J Agric Food Chem ; 70(51): 16106-16116, 2022 Dec 28.
Article En | MEDLINE | ID: mdl-36524955

The valorization of poultry byproducts, like feathers (processed to feather meal), in animal feed could contribute to the presence of veterinary drugs, including antibiotics. An animal study was carried out to study the fate of sulfadiazine, trimethoprim, and oxytetracycline in feathers, plasma, and droppings of broiler chickens. Cage and floor housing, different from current farm practices, were studied. Samples were analyzed by liquid chromatography-tandem mass spectrometry (LC-MS/MS). A longer presence of antibiotics was observed in feathers compared to plasma, with sulfadiazine being present the most. The internal presence (via blood) and the external presence (via droppings) of antibiotics in/on feathers were shown. Analysis of Escherichia coli populations, from droppings and feathers, highlighted that resistant bacteria could be transferred from droppings to feathers in floor-housed animals. The overall results suggest that feathers are a potential reservoir of antimicrobial residues and could contribute to the selection of antibiotic-resistant bacteria in the environment, animals, and humans.


Anti-Bacterial Agents , Oxytetracycline , Humans , Animals , Anti-Bacterial Agents/analysis , Oxytetracycline/analysis , Chickens , Feathers/chemistry , Sulfadiazine/pharmacology , Sulfadiazine/analysis , Trimethoprim/pharmacology , Trimethoprim/analysis , Chromatography, Liquid , Tandem Mass Spectrometry/methods
9.
Food Chem ; 394: 133540, 2022 Nov 15.
Article En | MEDLINE | ID: mdl-35763903

In this research, a green, selective and inexpensive switchable hydrophilicity solvent-based liquid phase microextraction (SHS-LPME) procedure has been optimized for the extraction and preconcentration of sulfadiazine (SDZ) in milk, honey and water samples prior to spectrophotometric analysis. Five variables affecting the SHS-LPME procedure were optimized using chemometric-based central composite design. For the SHS-LPME procedure, analytical parameters such as linearity, limit of detection, extraction recovery and enrichment factor were 15-300 µg L-1, 4.5 µg L-1, 96 ± 3% and 113, respectively. The precision of the method was investigated by repeatability and reproducibility studies. The relative standard deviation from these studies was found in the range of 2.4-4.5%. The recovery of the SDZ in the samples was in the range of 94 ± 4-99 ± 2%. Collected samples were analyzed by both the SHS-LPME procedure and the reference method using flow injection-flame atomic absorption technique, and the results were compared. There was no statistically significant difference between the two methods. This showed that the SHS-LPME procedure can be safely applied to the analysis of real samples.


Honey , Liquid Phase Microextraction , Animals , Chemometrics , Honey/analysis , Hydrophobic and Hydrophilic Interactions , Limit of Detection , Liquid Phase Microextraction/methods , Milk/chemistry , Reproducibility of Results , Solvents , Sulfadiazine/analysis , Water/analysis
10.
Article En | MEDLINE | ID: mdl-34854803

It is well-established that antibiotics stored individually at their optimal pH and in appropriate solvents are stable over time. However, limited information exists on the stability of antibiotics from multiple classes when prepared and stored as a mixture prior to multiresidue analysis by mass spectrometry. This study tested the stability of antibiotic standard mixtures from eight classes [amphenicols, tetracyclines, sulfonamides, quinolones, macrolides, ß-lactams, lincosamides and miscellaneous (i.e., trimethoprim)] in relation to the water:methanol ratio, presence of sodium hydroxide base (to solubilise quinolones), storage temperature, and container type including plain and silanized glass vials. Antibiotics were analysed by ultra-high-performance liquid chromatography coupled to tandem mass spectrometry. Several antibiotics, mainly quinolones, tetracyclines and macrolides, were unstable when stored as mixtures for one week regardless of the water:methanol ratio, storage temperature (4, -20 or -80 °C) and presence/absence of sodium hydroxide. Silanization of glassware improved the storage stability of quinolones and macrolides but reduced the stability of tetracyclines and other antibiotics including florfenicol amine, penicillin G, erythromycin and sulfadiazine. Our results show that several antibiotics in water:methanol are unstable when stored as a mixture and suggest a limited advantage of using base or silanized glass vials for the preparation and storage of antibiotic standards mixed together. Freshly prepared antibiotic standard mixtures are recommended for multi-residue quantitation of antibiotics.Abbreviations AMOX: amoxicillin; AMP: ampicillin; AZ: azithromycin; CAP: chloramphenicol; CE: collision energy; CTC: chlortetracycline; CIP: ciprofloxacin; DOX: doxycycline; ENO: enoxacin; ENRO: enrofloxacin; ERYTH: erythromycin; FF: florfenicol; FFA: florfenicol amine; FLU: flumequine; HDPE: high-density polyethylene; LC-MS/MS: liquid chromatography-tandem mass spectrometry; LIN: lincomycin; MRM: multiple reaction monitoring; NOR: norfloxacin; OFL-D3: ofloxacin-D3; OXO: oxolinic acid; OTC: oxytetracycline; PEN-G: penicillin G; PEN-V: penicillin V; ROX: roxithromycin; SDM: sulfadimethoxine; SDZ: sulfadiazine; SMX: sulfamethoxazole; SMZ-D4: sulfamethazine-D4; SSZ: sulfasalazine; TC: tetracycline; TAP: thiamphenicol; TILM: tilmicosin; TRIM: trimethoprim; TL: tolerance limit; VIRG: virginiamycin; UPLC-MS/MS: ultra-high pressure liquid chromatography-tandem mass spectrometry.


Anti-Bacterial Agents/analysis , Chromatography, High Pressure Liquid , Fluoroquinolones/analysis , Hydrogen-Ion Concentration , Macrolides/analysis , Methanol , Sulfadiazine/analysis , Tandem Mass Spectrometry , Temperature , Tetracyclines/analysis , Trimethoprim/analysis , Water , beta-Lactams/analysis
11.
Talanta ; 232: 122449, 2021 Sep 01.
Article En | MEDLINE | ID: mdl-34074433

Antibiotics, such as sulfadiazine and sulfathiazole, are widely used in veterinary applications which can result in remains in edible animal products. Therefore, there is an immense need for a reliable, selective, sensitive, and simple analytical technique for monitoring the concentration of sulfadiazine (SDZ) and sulfathiazole (STZ) in edible animal products. In this regard, we developed a magnetic dual template molecularly imprinted polymer (MMIP) to determine the SDZ and STZ in milk samples. For the sensitive and selective extraction and determination of target analytes, MMIPs have been combined with the syringe-to-syringe magnetic solid-phase microextraction (SS-MSPME) method. In addition, we used central composite design (CCD) for the extraction of SDZ and STZ. With optimum conditions, an efficient, rapid, and convenient technique for the preconcentration and determination of SDZ and STZ in milk samples by SS-MSPME coupling with HPLC-UV was developed. Using our combined approach, the limits of detection are 0.9 and 1.3 ng mL-1 for SDZ and STZ, respectively, along with good linearity and determination coefficients higher than 0.98. Our method demonstrates a practical approach for the deduction of antibiotics in milk samples with high recoveries and selectivity.


Molecular Imprinting , Sulfadiazine , Animals , Chromatography, High Pressure Liquid , Magnetic Phenomena , Milk/chemistry , Molecularly Imprinted Polymers , Solid Phase Extraction , Sulfadiazine/analysis , Sulfathiazoles , Syringes
12.
J Chromatogr A ; 1649: 462186, 2021 Jul 19.
Article En | MEDLINE | ID: mdl-34034102

Covalent organic frameworks (COFs) have showed expected potential in chromatographic separation due to unique structure and excellent performance. Nowadays, COF materials applied as chromatographic stationary phases is still in its infancy. Here, we modified COF materials on silica using benzene-1,4,5-tetracarboxylic dianhydride (PMDA) and 1,3,5-tris-(4-aminophenyl)triazine (TAPT) monomers by one-pot synthetic method for performing mixed-mode function, named as SiO2@COF. Five characterization methods including thermogravimetric analysis (TGA), scanning electron microscopy (SEM), Fourier transform infrared spectrometry (FT-IR), elemental analysis (EA) and powder X-ray diffraction (XRD) verified the morphology, structure characteristics and physicochemical properties of the materials. SiO2@COF for performing the separation of polar and nonpolar analytes on high performance liquid chromatography (HPLC) achieved the desired results. Retention mechanisms of the constructed SiO2@COF were researched via observing the effects of mobile phase with retention times. Results exhibited that the prepared stationary phase can provide various interaction modes, including hydrophobic, hydrophilic, hydrogen bonding and π-π interactions. In conclusion, the prepared SiO2@COF stationary phase can execute mixed-mode separation abilities and show potential for complex samples analysis.


Chromatography, High Pressure Liquid/methods , Metal-Organic Frameworks/chemistry , Silicon Dioxide/chemistry , Hydrophobic and Hydrophilic Interactions , Metal-Organic Frameworks/chemical synthesis , Spectroscopy, Fourier Transform Infrared , Sulfadiazine/analysis , X-Ray Diffraction
13.
Ecotoxicol Environ Saf ; 208: 111516, 2021 Jan 15.
Article En | MEDLINE | ID: mdl-33120260

Rapid-monitoring of drugs has attracted tremendous consideration owing to robust global demand for cost-effective and high effectiveness. Binary metal oxides with various morphology have been reported as electrodes for electrochemical sensor to fulfilling the clinical and enviromental requirements. In this study, strontium tungstate (SrWO4) nanoflakes have been successfully prepared via the facile sonochemical method for the first time. The characteristics of as-prepared SrWO4 are systematically measured by various analytical and spectroscopic methods. The SrWO4 nanoflakes are utilized to modify the electrochemical electrode for the sulfadiazine (SDZ) determination. The SrWO4 modified electrode possesses excellent electrocatalytic activity and high recognition capability for the electrochemical detection of SDZ. Impressively, the as-fabricated SrWO4 modified electrode attainted lowest oxidation peak at +0.93 V (vs Ag/AgCl2) with the limit of detection of 0.009 µM, the sensitivity of 0.123 µA µM-1 cm2 and linear detection range of 0.05-235 µM. The enhanced performance of proposed SrWO4-based sensors could be attributed to the catalytic effect, large surface area, good electrical conductivity and physicochemical nature. Notably, the electrocatalytic performances of the SDZ sensors are good as compared to the previous literature, indicating the significance of the newly designed SrWO4 modified electrode. The real-sample diagnosis by the SDZ detection in environmental sample demonstrates the proposed SrWO4-based sensors with good recovery range.


Environmental Monitoring/methods , Environmental Pollutants/analysis , Sulfadiazine/analysis , Tungsten Compounds/chemistry , Catalysis , Electrochemical Techniques/methods , Electrodes , Oxidation-Reduction , Oxides/chemistry , Strontium
14.
Sci Rep ; 10(1): 14088, 2020 08 24.
Article En | MEDLINE | ID: mdl-32839521

River deltas are frequently facing salinity intrusion, thus challenging agricultural production in these areas. One adaption strategy to increasing salinity is shrimp production, which however, heavily relies on antibiotic usage. This study was performed to evaluate the effect of increasing salinity on the dissipation rates of antibiotics in tropical flooded soil systems. For this purpose, paddy top soil from a coastal Vietnamese delta was spiked with selected frequently used antibiotics (sulfadiazine, sulfamethazine, sulfamethoxazole, trimethoprim) and incubated with flood water of different salt concentrations (0, 10, 20 g L-1). Antibiotic concentrations were monitored in water and soil phases over a period of 112 days using liquid chromatography and tandem mass spectrometry. We found that sulfamethazine was the most persistent antibiotic in the flooded soil system (DT50 = 77 days), followed by sulfadiazine (DT50 = 53 days), trimethoprim (DT50 = 3 days) and sulfamethoxazole (DT50 = 1 days). With the exception of sulfamethoxazole, the apparent distribution coefficient increased significantly (p < 0.05) for all antibiotics in course of the incubation, which indicates an accumulation of antibiotics in soil. On a whole system basis, including soil and water into the assessment, there was no overall salinity effect on the dissipation rates of antibiotics, suggesting that common e-fate models remain valid under varying salinity.


Anti-Bacterial Agents/analysis , Environmental Monitoring/methods , Geologic Sediments/chemistry , Salinity , Soil Pollutants/analysis , Animals , Floods , Penaeidae/growth & development , Shellfish , Soil/chemistry , Sulfadiazine/analysis , Sulfamethazine/analysis , Sulfamethoxazole/analysis , Trimethoprim/analysis , Tropical Climate
15.
J Nat Prod ; 83(4): 1305-1308, 2020 04 24.
Article En | MEDLINE | ID: mdl-32208615

The structure of 2,4-(4'-aminobenzenamine)pyrimidine (1), a pyrimidine alkaloid previously isolated from the bulbs of Scilla madeirensis (Asparagaceae, synonym Autonoë madeirensis), has been revised. These conclusions were met via comparison of reported NMR and EIMS data with those obtained from synthetic standards. The corrected structure is the antibiotic sulfadiazine (2), which has likely been isolated as a contaminant from the site of collection. The reported bioactivity of 1 as an α1-adrenoceptor antagonist should instead be ascribed to sulfadiazine. Our findings appear to show another example of an anthropogenic contaminant being identified as a natural product and emphasize the importance of considering the biosynthetic origins of isolated compounds within a phylogenetic context.


Biological Products/pharmacology , Pyrimidines/pharmacology , Scilla/chemistry , Sulfadiazine/chemistry , Sulfadiazine/pharmacology , Biological Products/analysis , Biological Products/chemistry , Biological Products/isolation & purification , Magnetic Resonance Spectroscopy , Molecular Structure , Phylogeny , Plant Roots/chemistry , Pyrimidines/chemistry , Pyrimidines/isolation & purification , Sulfadiazine/analysis , Sulfadiazine/isolation & purification
16.
Chemosphere ; 252: 126472, 2020 Aug.
Article En | MEDLINE | ID: mdl-32200179

Sulfadiazine (SDZ) is widely used in clinical treatment, livestock husbandry and aquaculture as an antibacterial agent, resulting in environmental risks. In this work, batch experiments were conducted to investigate the characteristics of SDZ biodegradation and reaction mechanisms in a nitrate anaerobic denitrifying system for the first time. The results showed that 98.52% of the SDZ, which had an initial concentration of 50 mg L-1, was degraded after 70 h, indicating that the removal efficiency of SDZ in anaerobic denitrifying system was 55.27% higher than that in anaerobic system. Furthermore, LC-MS-MS analysis confirmed that SDZ could be degraded into 16 byproducts via 3 main degradation pathways that contained 6 different reactions. After analyzing the microbial communities of the reactor, the denitrifying bacteria and desulfurizing bacteria Desulforhabdus, Ignavibacterium, SBR1031_norank, Nocardioides, etc. were highly associated with the removal of SDZ in the system. The biological toxicity test of the effluent indicated that the remaining organic matter and inorganic matter of the effluent could provide nutrients for E. coli and promote its growth. In other words, anaerobic denitrifying systems are highly efficient, simple and environmentally friendly, and have an impressive prospect in the biodegradation of sulfonamide antibiotics.


Anti-Bacterial Agents/metabolism , Biodegradation, Environmental , Microbiota , Sulfadiazine/metabolism , Anaerobiosis , Bacteria/metabolism , Bioreactors , Denitrification , Escherichia coli/metabolism , Sulfadiazine/analysis , Sulfonamides
17.
J Hazard Mater ; 386: 121955, 2020 03 15.
Article En | MEDLINE | ID: mdl-31887563

Micropollution such as pharmaceutical residuals potentially compromises water quality and jeopardizes human health. This study evaluated the photo-Fenton ceramic membrane filtration toward the removal of sulfadiazine (SDZ) as a common antibiotic chemical. The batch experiments verified that the photo-Fenton reactions with as Goethite (α-FeOOH) as the photo-Fenton catalyst achieved the degradation rates of 100% within 60 min with an initial SDZ concentration of 12 mg·L-1. Meanwhile, a mineralization rate of over 80% was obtained. In continuous filtration, a negligible removal rate (e.g., 4%) of SDZ was obtained when only filtering the feed solution with uncoated or catalyst-coated membranes. However, under Ultraviolet (UV) irradiation, both the removal rates of SDZ were significantly increased to 70% (no H2O2) and 99% (with H2O2), respectively, confirming the active degradation by the photo-Fenton reactions. The highest apparent quantum yield (AQY) reached up to approximately 25% when the UV254 intensity was 100 µW·cm-2 and H2O2 was 10 mmol·L-1. Moreover, the photo-Fenton reaction was shown to effectively mitigate fouling and prevent flux decline. This study demonstrated synchronization of photo-Fenton reactions and membrane filtration to enhance micropollutant degradation. The findings are also important for rationale design and operation of photo-Fenton or photocatalytic membrane filtration systems.


Anti-Bacterial Agents/analysis , Anti-Bacterial Agents/radiation effects , Ceramics/chemistry , Iron Compounds/chemistry , Membranes, Artificial , Minerals/chemistry , Sulfadiazine/analysis , Water Pollutants, Chemical/analysis , Water Purification/methods , Catalysis , Filtration , Hydrogen Peroxide/chemistry , Models, Theoretical , Oxidation-Reduction , Photolysis , Sulfadiazine/radiation effects , Ultraviolet Rays , Water Pollutants, Chemical/radiation effects
18.
Mikrochim Acta ; 187(1): 54, 2019 12 17.
Article En | MEDLINE | ID: mdl-31848725

A sensitive fluorometric assay is described for the direct determination of the antibiotic sulfadiazine. Silver nanoparticles placed on graphene quantum dots (Ag NP-GQDs) were synthesized by reduction of AgNO3 with sodium borohydride in the presence of GQDs. The growth of Ag NPs on the surface of the GQDs causes quenching of the blue fluorescence of the GQDs with an emission maximum at 470 nm by surface-enhanced energy transfer. If sulfadiazine is added, it interacts with Ag NPs and fluorescence is restored. Under optimal conditions, the fluorescence increases linearly in the sulfadiazine concentration range of 0.04-22.0 µM. The detection limit is 10 nM with relative standard deviations of 2.3 and 4.2 (at 10 µM of sulfadiazine; for n = 6) for intra- and inter-day assays. Graphical abstractSchematic representation of sulfadiazine determination using Ag NP-GQDs as a fluorescent nanoprobe.


Anti-Bacterial Agents/analysis , Fluorometry , Metal Nanoparticles/chemistry , Quantum Dots/chemistry , Silver/chemistry , Sulfadiazine/analysis , Graphite/chemistry , Particle Size , Surface Properties
19.
Ecotoxicol Environ Saf ; 184: 109656, 2019 Nov 30.
Article En | MEDLINE | ID: mdl-31526920

The existing form of ionizable organic contaminants (IOCs) could affect their adsorption characteristics to soil and biochar. In this study, 2 IOCs, namely, sulfadiazine and imazalil, were selected to study their adsorption by rice straw-derived biochar-amended soils, as well as the effect of pH and gallic acid on their adsorption. The results showed that the soil adsorption isotherms of the two ionizable organic contaminants could be fitted well by a linear equation and the Freundlich equation, and r2 was more than 0.80. The adsorption coefficient (Kd) in the three kinds of soil ranged from 0.262 to 4.07 L kg-1 for sulfadiazine and from 3.11 to 96.5 L kg-1 for imazalil. After the addition of biochar, the adsorption of sulfadiazine and imazalil in the soil increased. The adsorption of sulfadiazine by biochar gradually decreased with the increase in pH; the adsorption of imazalil increased when the pH increased from 2 to 5 and then gradually decreased with increasing pH. Gallic acid enhanced the adsorption of the two IOCs to pure soil and biochar-amended soil.


Charcoal/chemistry , Gallic Acid/chemistry , Oryza/chemistry , Soil Pollutants/analysis , Soil/chemistry , Adsorption , Hydrogen-Ion Concentration , Imidazoles/analysis , Sulfadiazine/analysis
20.
Anal Chim Acta ; 1086: 55-65, 2019 Dec 04.
Article En | MEDLINE | ID: mdl-31561794

Benefiting from the rich redox chemistry, high electrical conductivity and synergistic effect from two metal ions, the binary metal sulphides received tremendous attention in various applications. As a result, the MoS2-RuS2 nanomaterial was synthesized through the simple one-pot hydrothermal technique. The electrocatalytic activity of the as-synthesized nanomaterial was exploited towards the electrochemical detection of antibiotic drug sulphadiazine (SDZ). The electrocatalytic oxidation of the SDZ exhibited lowest anodic peak potential and ehanced anodic peak current rather than other modified electrodes. Notably, an excellent electrochemical performance with very lowest limit of detection (LOD) of 0.004 µM, appreciable linear range from 0.01 µM to 598.7 µM and high sensitivity (2.333 µA µM-1 cm-2) was obtained at MoS2-RuS2 modified electrode. Moreover, well anti-interfering property, good operational stability, repeatability and reproducibility was achieved. Facinatingly, the practicability of the modified electrode demonstrated in milk and human serum samples.


Anti-Bacterial Agents/analysis , Disulfides/chemistry , Electrochemical Techniques , Molybdenum/chemistry , Ruthenium/chemistry , Sulfadiazine/analysis , Sulfides/chemistry , Catalysis , Electrodes
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