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1.
Talanta ; 275: 126088, 2024 Aug 01.
Article in English | MEDLINE | ID: mdl-38636441

ABSTRACT

Three-dimensional sponge-architecture covalent organic frameworks (COFs)-aerogel was successfully designed and synthesized via a freeze-drying template approach, and utilized as an efficient sorbent in solid-phase extraction (SPE). A method for selective enrichment of pharmaceutical contaminants including tetracycline, chlortetracycline, methacycline and oxytetracycline in the environment and food samples was proposed by combining with high performance liquid chromatography (HPLC). To understand the adsorption mechanism, selectivity test and molecular dynamics (MD) simulated calculation were both carried out. The experimental and in-silico results demonstrated that the COFs-aerogel possessed high selectivity for contaminants with H bond acceptors/donors and good efficiency with maximum adsorption capacity up to 294.1 mg/g. The SPE-based HPLC method worked well in the range of 8-1000 ng/mL, with the need of little dose of adsorbent and sample volume while no need of spectrometer, outgoing the reported adsorbents. Under the optimized conditions, the intra-day and inter-day relative standard deviations (RSD) of repeatability were within 2.78-6.29 % and 2.44-8.42 % (n = 5). The results meet the current detection requirement for practical applications, and could be extended for further design of promising adsorbents.


Subject(s)
Anti-Bacterial Agents , Metal-Organic Frameworks , Solid Phase Extraction , Tetracyclines , Adsorption , Solid Phase Extraction/methods , Metal-Organic Frameworks/chemistry , Anti-Bacterial Agents/chemistry , Anti-Bacterial Agents/analysis , Tetracyclines/analysis , Tetracyclines/chemistry , Tetracyclines/isolation & purification , Chromatography, High Pressure Liquid/methods , Molecular Dynamics Simulation , Gels/chemistry , Tetracycline/analysis , Tetracycline/chemistry , Tetracycline/isolation & purification , Water Pollutants, Chemical/analysis , Water Pollutants, Chemical/chemistry , Food Contamination/analysis
2.
J Food Drug Anal ; 31(2): 371-380, 2023 06 15.
Article in English | MEDLINE | ID: mdl-37335166

ABSTRACT

Tetracycline (TC) is a broad-spectrum antibiotic and has been added to animal feeds to grow livestock under healthy conditions, making it important to have effective methods for rapidly detecting TC in complex samples. In this study, a novel method that uses lanthanide ions (i.e. Eu3+ and Gd3+) as magnetic and sensing probes for the detection of TC from aqueous samples is explored. When dissolving Gd3+ in tris(hydroxymethyl)aminomethane (Tris) buffer at pH 9, magnetic Gd3+-Tris conjugates can be readily generated. The magnetic Gd3+-Tris conjugates possess trapping capacity toward TC from sample solutions via the chelation of Gd3+ and TC. Eu3+ is used as the fluorescence sensing probe against TC on the Gd3+-TC conjugates via the antenna effect. The fluorescence response derived from Eu3+ is increased with the increase of TC trapped on the Gd3+-based probes. The linear dynamic range against TC ranges from 20 to 320 nM, whereas the limit of detection toward TC is ~2 nM. Furthermore, the developed sensing method can be employed for the visual assay of TC with a concentration above ~0.16 µM under UV light illumination in the dark. Furthermore, we have demonstrated the applicability of the developed method to quantify TC in a chicken broth sample with complex matrix. Our developed method offers several advantages, including high sensitivity and good selectivity, for the detection of TC in complex samples.


Subject(s)
Tetracycline , Hydrogen-Ion Concentration , Tetracycline/chemistry , Tetracycline/isolation & purification , Gadolinium/chemistry , Europium/chemistry , Cations/chemistry , Temperature , Magnetics , Fluorescent Dyes/chemistry , Anti-Bacterial Agents/chemistry , Anti-Bacterial Agents/pharmacology
3.
Carbohydr Polym ; 273: 118528, 2021 Dec 01.
Article in English | MEDLINE | ID: mdl-34560942

ABSTRACT

Pollution by tetracyclines antibiotics has a great potential risk on human and animal health even at trace levels. Copper nanoparticles immobilized-ß-cyclodextrin functionalized reduced graphene oxide (Cu/ß-CD/rGO) were successfully prepared as an efficient extractor of tetracycline (TC), oxytetracycline (OTC) and doxycycline (DC) antibiotics from different environmental water samples. Tetracyclines (TCs) are strongly deposited in the matrix of Cu/ß-CD/rGO nanocomposite via surface complexation with the Cu-nanoparticles besides the formation of inclusion complexes with ß-cyclodextrin and π-π interaction of reduced graphene oxide. The novel nanocomposite was characterized by HRSEM, TEM, TGA, FT-IR, XPS, and XRD. The optimization of variables such as the pH, contact time, ionic strength and TC concentration were successfully analyzed. The maximum adsorption capacity (qm) of Cu/ß-CD/rGO calculated from the Langmuir isotherm was 403.2 mg.g-1 for TC, 476.2 mg.g-1 for OTC and 434.8 mg.g-1 for DC at 298 K. The removal efficiency was decreased by 3.7% after five adsorption-desorption cycles. The Cu/ß-CD/rGO nanocomposite was applied for removing TCs from tap water and the Nile River water samples. The novel nanocomposite demonstrated fast and highly efficient removing performance for different TCs with low levels and large sample volume.


Subject(s)
Copper/chemistry , Graphite/chemistry , Nanocomposites/chemistry , Tetracyclines/isolation & purification , Water Pollutants, Chemical/isolation & purification , beta-Cyclodextrins/chemistry , Adsorption , Animals , Anti-Bacterial Agents/isolation & purification , Biodegradation, Environmental , Doxycycline/isolation & purification , Humans , Nanoparticles/chemistry , Oxytetracycline/isolation & purification , Spectroscopy, Fourier Transform Infrared/methods , Tetracycline/isolation & purification , Water/chemistry , Water Purification/methods
4.
Carbohydr Polym ; 262: 117951, 2021 Jun 15.
Article in English | MEDLINE | ID: mdl-33838827

ABSTRACT

Magnetic nanoparticles that can be employed as Fenton-like catalysts Fenton-like catalysts are attractive materials for degrading antibiotics. In this study, we facilely prepared novel magnetic pullulan (MP) hydrogels by doping modified magnetic nanoparticles into pullulan matrices, which could enhance catalytic degradation performance and strengthen the stability of resulting hydrogels. This is the first time that MP hydrogels have been fabricated successfully and used as Fenton-like catalysts for tetracycline hydrochloride (TCH) degradation. MP hydrogels were characterized and their catalytic TCH degradation abilities were also investigated. The optimized conditions (pH value, Fe3O4 content, H2O2 content and TCH concentration) for TCH degradation were investigated. The optimized system showed excellent degradation efficiency for TCH. Further, the degradation mechanism was comprehensively studied. Finally, synthesized MP hydrogels showed impressive reusability and stability in the cycle experiment. Thus, our findings would open new possibilities to develop magnetic hydrogels in eliminating antibiotic contaminants.


Subject(s)
Anti-Bacterial Agents/isolation & purification , Glucans/chemistry , Hydrogels/chemistry , Magnetic Iron Oxide Nanoparticles/chemistry , Wastewater/chemistry , Anti-Bacterial Agents/metabolism , Catalysis , Hydrogen Peroxide/chemistry , Iron/chemistry , Tetracycline/isolation & purification , Tetracycline/metabolism , Waste Disposal, Fluid/methods , Water Purification/methods
5.
Carbohydr Polym ; 251: 117004, 2021 Jan 01.
Article in English | MEDLINE | ID: mdl-33142571

ABSTRACT

Pennisetum sinese Roxb is a kind of forage with high yield and high quality. However, because only the leaves are used as feed, most straw is discarded or burned, causing pollution and resources waste. In this study, a magnetic cellulose adsorbent produced by extracting cellulose from Pennisetum sinese Roxb straw was used to adsorb antibiotic tetracycline (TC) from water and can be easily separated. The physicochemical properties of the obtained cellulose samples were studied. The adsorption process was mediated by multiple mechanisms including intra-particle diffusion, chemical ion exchange, hydrogen bonding, and electrostatic interaction. We determined the optimal pH, contact time, initial TC concentration, and temperature before investigating the effects of humic acid and ionic strength on the adsorption process. Our results demonstrate that the magnetic cellulose is a promising adsorbent for the removal of TC from water and is worth to be studied further to develop real-world implementation strategies.


Subject(s)
Cellulose/chemistry , Pennisetum/chemistry , Tetracycline/isolation & purification , Water Pollutants, Chemical/isolation & purification , Adsorption , Animals , Anti-Bacterial Agents/isolation & purification , Cellulose/ultrastructure , Humans , Humic Substances , Hydrogen-Ion Concentration , Kinetics , Magnetics , Microscopy, Electron, Scanning , Osmolar Concentration , Thermodynamics , Wastewater/chemistry , Water Purification/methods , X-Ray Diffraction
6.
PLoS One ; 15(8): e0237389, 2020.
Article in English | MEDLINE | ID: mdl-32797116

ABSTRACT

In the present work, a series of magnetically separable Fe3O4/g-C3N4/MoO3 nanocomposite catalysts were prepared. The as-prepared catalysts were characterized by XRD, EDX, TEM, FT-IR, UV-Vis DRS, TGA, PL, BET and VSM. The photocatalytic activity of photocatalytic materials was evaluated by catalytic degradation of tetracycline solution under visible light irradiation. Furthermore, the influences of weight percent of MoO3 and scavengers of the reactive species on the degradation activity were investigated. The results showed that the Fe3O4/g-C3N4/MoO3 (30%) nanocomposites exhibited highest removal ability for TC, 94% TC was removed during the treatment. Photocatalytic activity of Fe3O4/g-C3N4/MoO3 (30%) was about 6.9, 5, and 19.9-fold higher than those of the MoO3, g-C3N4, and Fe3O4/g-C3N4 samples, respectively. The excellent photocatalytic performance was mainly attributed to the Z-scheme structure formed between MoO3 and g-C3N4, which enhanced the efficient separation of the electron-hole and sufficient utilization charge carriers for generating active radials. The highly improved activity was also partially beneficial from the increase in adsorption of the photocatalysts in visible range due to the combinaion of Fe3O4. Superoxide ions (·O2-) was the primary reactive species for the photocatalytic degradation of TC, as degradation rate were decreased to 6% in solution containing benzoquinone (BQ). Data indicate that the novel Fe3O4/g-C3N4/MoO3 was favorable for the degradation of high concentrations of tetracycline in water.


Subject(s)
Ferrosoferric Oxide/chemistry , Graphite/chemistry , Molybdenum/chemistry , Nanocomposites/chemistry , Nitrogen Compounds/chemistry , Oxides/chemistry , Photochemical Processes , Tetracycline/chemistry , Water/chemistry , Catalysis , Light , Magnets/chemistry , Tetracycline/isolation & purification , Water Pollutants, Chemical/chemistry , Water Pollutants, Chemical/isolation & purification
7.
Molecules ; 25(14)2020 Jul 17.
Article in English | MEDLINE | ID: mdl-32709030

ABSTRACT

Antibiotics are active substances frequently used to treat and prevent diseases in animal husbandry, especially in swine and poultry farms. The use of manure as a fertilizer may lead to the dispersion of antibiotic residue into the environment and consequently the development of antibiotic-resistant bacteria. Most pharmaceutical active ingredients are excreted after administration, in some cases up to 90% of the consumed dose can be found in the feces and/or urine as parent compound. Therefore, due to antibiotic metabolism their residues can be easily detected in manure. This article describes a method for simultaneous analysis of ciprofloxacin, chlortetracycline, doxycycline, enrofloxacin, lincomycin, oxytetracycline, tetracycline, tiamulin, trimethoprim and tylosin in feces, liquid manure and digestate. Antibiotics were extracted from the different matrices with McIlvaine-Na2EDTA buffer solution and the extract was purified by the use two techniques: d-SPE and SPE (Strata-X-CW cartridges) and final eluent was analyzed by LC-MS and LC-MS/MS. The European Commission Decision 2002/657/EC was followed to conduct the validation of the method. Recoveries obtained from spiked pig and poultry feces and liquid manures samples ranged from 63% to 93% depending on analytes. The analysis of 70 samples (feces, liquid manure and digestate) revealed that 18 samples were positive for the presence of doxycycline, oxytetracycline, tetracycline, chlortetracycline, enrofloxacin, tiamulin and lincomycin. The results obtained in the presented study demonstrated that animal feces can be used as a non-invasive method detection antibiotic usage in animal production.


Subject(s)
Anti-Bacterial Agents/isolation & purification , Feces/chemistry , Animals , Anti-Bacterial Agents/therapeutic use , Chlortetracycline/chemistry , Chlortetracycline/isolation & purification , Chlortetracycline/therapeutic use , Chromatography, Liquid , Doxycycline/chemistry , Doxycycline/isolation & purification , Doxycycline/therapeutic use , Livestock , Mass Spectrometry , Oxytetracycline/chemistry , Oxytetracycline/isolation & purification , Oxytetracycline/therapeutic use , Poultry , Swine , Tetracycline/chemistry , Tetracycline/isolation & purification , Tetracycline/therapeutic use , Tylosin/chemistry , Tylosin/isolation & purification , Tylosin/therapeutic use
8.
Bioprocess Biosyst Eng ; 43(11): 1951-1960, 2020 Nov.
Article in English | MEDLINE | ID: mdl-32500436

ABSTRACT

In this study, the roles of extracellular polymeric substances (EPSs) excreted by Pandoraea sp. XY-2 in the removal of tetracycline (TC) were investigated. In the early stage, TC in the solution was mainly removed by the adsorption of EPSs, which accounted for 20% of TC. Thereafter, large amount of TC was transported into the intracellular and biodegraded. EPSs was extracted and the contents of polyprotein and polysaccharides reached their maximum values (30.84 mg/g and 11.15 mg/g) in the first four days. Fourier transform infrared spectroscopy analysis revealed that hydroxyl, methylidyne, methylene and amide I groups in EPSs participated in the adsorption of TC. Furthermore, three-dimensional excitation-emission matrix fluorescence spectroscopy analysis revealed that TC caused the quenching of EPSs fluorescent groups. The quenching mechanism was attributed to static quenching and protein-like substances in EPSs from Pandoraea sp. XY-2 dominated the TC adsorption process. Bioinformatic analysis of Pandoraea sp. XY-2 genome identified multiple genes involved in exopolysaccharide synthesis and EPSs formation. The insights gained in this study might provide a better understanding about the adsorption process of EPSs in tetracycline-contaminated environment.


Subject(s)
Burkholderiaceae/metabolism , Extracellular Polymeric Substance Matrix/chemistry , Polymers/chemistry , Polyproteins/chemistry , Polysaccharides/chemistry , Spectrometry, Fluorescence/methods , Tetracycline/chemistry , Tetracycline/isolation & purification , Water Pollutants, Chemical/isolation & purification , Adsorption , Anti-Bacterial Agents/chemistry , Biotechnology/methods , Methane/analogs & derivatives , Sewage/chemistry , Spectroscopy, Fourier Transform Infrared , Time Factors , Water Pollutants, Chemical/chemistry , Water Purification
9.
Food Chem ; 329: 127162, 2020 Nov 01.
Article in English | MEDLINE | ID: mdl-32492599

ABSTRACT

We report for the first time the use of biochar as a stabilizer for oil-in-water (o/w) Pickering emulsion. The emulsion is subsequently used to prepare tetracycline-imprinted biochar composite microspheres (MIPMs) with tailored sizes and good uniformity. The adsorption properties of tetracycline to the MIPMs were investigated using different adsorption experiments including adsorption kinetic experiment, equilibrium binding experiment, selectivity evaluation and competitive adsorption tests. The MIPMs were used as adsorbent for solid phase extraction (SPE) for the extraction of tetracycline present in drinking water, fish, and chicken samples. Under optimal conditions, the results showed good recovery yield ranging from ~73% to ~95% with a relative standard deviation (RSD) ranging from ~0.3% to ~8.4%, respectively.


Subject(s)
Charcoal/chemistry , Emulsions/chemistry , Food Contamination/analysis , Solid Phase Extraction/methods , Tetracycline/isolation & purification , Adsorption , Anti-Bacterial Agents/isolation & purification , Chromatography, High Pressure Liquid , Food Analysis/instrumentation , Food Analysis/methods , Microspheres , Molecular Imprinting/methods , Solid Phase Extraction/instrumentation , Water Pollutants, Chemical/isolation & purification
10.
Food Chem ; 326: 126969, 2020 Oct 01.
Article in English | MEDLINE | ID: mdl-32438229

ABSTRACT

Biocompatible magnetic molecularly imprinted polymers (BMMIPs) were prepared with Zein for the first time, and were used to enrich tetracycline compounds selectively. Innovative combination of BMMIPs and electrochemistry to obtain lower detection line to satisfy industrial detection demands. Using Zein as the crosslinking agent, the polymers were synthesized on the surface of Fe3O4 particles. The scanning electron microscope, transmission electron microscope and X-ray diffraction technologies were used to characterize BMMIPs. Through optimization, BMMIPs attained large adsorption capacity (236.40 mg/g) with fast kinetics (40 min) and followed the Langmuir isotherm and pseudo-second-order kinetic models. BMMIPs had good recognition ability, the selective factors of oxytetracycline, chlortetracycline, doxycycline were 4.78, 4.23, and 3.39, respectively. Excellent linearity was attained in the range of 0.025-500 µg/mL, with low detection limits and low quantitation limits of 0.025 and 0.083 µg/mL. According to our exploring, BMMIPs was ideal materials for enrichment of tetracycline in complex biological samples.


Subject(s)
Biocompatible Materials/chemistry , Food Contamination/analysis , Milk/chemistry , Molecular Imprinting/methods , Tetracyclines/analysis , Adsorption , Animals , Anti-Bacterial Agents/analysis , Anti-Bacterial Agents/chemistry , Anti-Bacterial Agents/isolation & purification , Electrochemical Techniques , Food Analysis/methods , Limit of Detection , Magnetic Phenomena , Magnetite Nanoparticles/chemistry , Polymers/chemistry , Tetracycline/analysis , Tetracycline/chemistry , Tetracycline/isolation & purification , Tetracyclines/chemistry , Tetracyclines/isolation & purification , X-Ray Diffraction , Zein/chemistry
11.
J Colloid Interface Sci ; 573: 287-298, 2020 Aug 01.
Article in English | MEDLINE | ID: mdl-32283417

ABSTRACT

In this work, iron-manganese binary oxides (FMO) modified with different proportions of glucose addition (FMOCx) by co-precipitation method showed good activity in activating hydrogen peroxide (H2O2) for tetracycline degradation. The structure and surface characterizations of the FMO and FMOCx were measured by XRD, FTIR, TEM, BET and XPS. With increased glucose addition, FMOCx has more surface functional groups such as -OH and -COOH, particle size decreases, surface area gradually increases, and the ratio of high valence iron and manganese also increases. In addition, the glucose might be oxidized by KMnO4 to form amorphous carbon on the catalyst surface. Glucose modified iron-manganese binary oxides FMOC3 (with 0.003 mol glucose added) showed the highest efficiency removal capability for tetracycline up to 85%, which attribute to it has a larger surface area, more surface functional groups and higher surface active Mn(IV) site content. The results also demonstrated that FMOC3 could efficiently activate hydrogen peroxide. This study proves that glucose modified iron-manganese binary oxides (FMOCx) can offered a possibility of degradation of refractory organic pollutants as an environmentally friendly catalyst in the absence of H2O2 or not.


Subject(s)
Glucose/chemistry , Iron/chemistry , Manganese/chemistry , Oxides/chemistry , Tetracycline/isolation & purification , Hydrogen Peroxide/chemistry , Oxidation-Reduction , Particle Size , Surface Properties , Tetracycline/chemistry
12.
Int J Biol Macromol ; 155: 421-429, 2020 Jul 15.
Article in English | MEDLINE | ID: mdl-32224175

ABSTRACT

In the present study, novel ionic liquid-impregnated chitosan hydrogel beads (CS-TCMA) were fabricated via the reaction of tricaprylmethylammonium chloride (TCMA, Aliquat-336) with the chitosan's amino groups. They were used for the fast adsorption of Tetracycline (TC), as a pharmaceutical compound model, from aqueous solution. It was found that the impregnation of TCMA greatly improved the adsorption behaviour of chitosan toward TC. The optimum adsorbent was determined to be 3 mg/ L in a wide pH range of 5-11. It was a fast process, with a 90% removal efficiency in <45 min. The adsorption kinetic of TC on the CS-TCMA was well described by the pseudo-first-order model and intra-particle diffusion model. The adsorption also obeyed the Langmuir adsorption isotherm model and the maximum adsorption capacity obtained was 22.42 mg/g at 45 °C. The thermodynamic study also revealed the endothermic nature of the process. The adsorption mechanism was also studied.


Subject(s)
Anti-Bacterial Agents/isolation & purification , Chitosan/chemistry , Hydrogels/chemistry , Quaternary Ammonium Compounds/chemistry , Tetracycline/isolation & purification , Water Pollutants, Chemical/isolation & purification , Water Purification/methods , Adsorption , Anti-Bacterial Agents/analysis , Anti-Bacterial Agents/metabolism , Ionic Liquids/chemistry , Kinetics , Tetracycline/analysis , Tetracycline/metabolism , Thermodynamics , Water Pollutants, Chemical/analysis , Water Pollutants, Chemical/metabolism
13.
Molecules ; 25(6)2020 Mar 13.
Article in English | MEDLINE | ID: mdl-32183050

ABSTRACT

Serious environmental and human health problems caused by the abuse of antibiotics have attracted worldwide concern. Recently, metal-organic frameworks (MOFs) with high porosity have drawn wide attention for their effects in the adsorption and removal of pollutants from complex matrices. Herein, a high-stable metal organic framework (MOF), i.e., ((ZnCl2)3(L)2·DMF)n, where L=1,3,5-tris((pyridin-4-ylthio)methyl)benzene), MOF 1, was applied to adsorb and remove tetracycline from sewage and dairy products. The results showed that MOF 1 exhibited a strong performance in the adsorption of tetracycline. The effects of initial pH values, adsorbent dose, contact time and ionic strength of the adsorption performance of MOF 1 were investigated. The adsorption kinetics best fit the pseudo-second order model, and the adsorption isotherms matched the Langmuir adsorption model well. It was indicated that both chemical adsorption and physical adsorption play an important role in the adsorption process, and the adsorption of tetracycline was homogeneous and occurred on a monolayer on the surface of MOF 1. Additionally, the stability of MOF 1 and the details of the adsorption mechanism were also investigated. Thus, this study provides a new candidate for the application of MOFs-based adsorbents in the removal of antibiotics from sewage and dairy products.


Subject(s)
Dairy Products/analysis , Metal-Organic Frameworks/chemistry , Sewage/chemistry , Tetracycline/isolation & purification , Adsorption , Hydrogen-Ion Concentration , Kinetics , Osmolar Concentration , Temperature , Tetracycline/chemistry , Time Factors , X-Ray Diffraction
14.
Sci Rep ; 10(1): 2960, 2020 02 19.
Article in English | MEDLINE | ID: mdl-32076056

ABSTRACT

In this study, a novel, sustainable and efficient ceramsite substrate of constructed wetlands (CWs) were prepared for tetracycline (TC) removal by employing bentonite (Ben) and red mud (Rm) as the main materials and pine sawdust (Ps) as the additive. The optimal parameters for Ben/Rm/Ps ceramsite preparation were obtained via orthogonal and one-factor experimental designs, and the optimal parameters were presented as follows: mass ratio of Ben: Rm: Ps = 4:1:0.9, preheating temperature = 240 °C, preheating time = 20 min, calcining temperature = 1150 °C, and calcining time = 14 min. The properties of Ben/Rm/Ps-op ceramsite (obtained at the optimal condition) were first analyzed, including XRD and SEM, and demonstrated a microporous structure with some crystal strength components. Neutral condition and higher temperature were indicated conducive to improve the TC removal efficiency, while coexisting ions (Na+ or Ca2+) showed adverse effect for TC adsorption by Ben/Rm/Ps-op. In addition, adsorption kinetics and isotherm could be well described by the second-order kinetics and linear isothermal model, respectively, which suggested chemisorption and multilayer adsorption thickness increased infinitely. The theoretical maximum TC adsorption capacity of Ben/Rm/Ps-op at 20 °C reached up to 2.5602 mg/g. In addition, Ben/Rm/Ps-op could effectively remove TC as the CWs substrate under a dynamic flow condition. Further, Ben/Rm/Ps-op exhibited high reusability capability and stability for TC removal, and the adsorption amount still remained for 2.13 mg/g (C0 = 80 mg/L) after three consecutive cycles.


Subject(s)
Complex Mixtures/chemistry , Green Chemistry Technology/methods , Tetracycline/isolation & purification , Water Pollutants, Chemical/isolation & purification , Water Purification/methods , Adsorption , Bentonite/chemistry , Sewage/chemistry , Tetracycline/chemistry , Water Pollutants, Chemical/chemistry
15.
Analyst ; 145(6): 2398-2404, 2020 Mar 16.
Article in English | MEDLINE | ID: mdl-32039409

ABSTRACT

The metal-organic framework (MOF-74) series has the most open metal sites. The metal ions have different bonding strengths with the ligand in MOF-74 and the bond of the ligand can be successively broken to obtain highly active heteroparticles by controlling the temperature, which is difficult to achieve using traditional methods. Magnetic NiCo/Fe3O4-MOF-74, which is fabricated using trimetallic NiCoFe-MOF-74 as a precursor, is simple and rational in comparison with the traditional magnetic core and tunable MOF shell hybrid composites that are formed using a step-by-step assembly strategy. After thermal treatment under a specific atmosphere, NiCo/Fe3O4-MOF-74 shows higher stability, strong magnetism and more active metal sites compared to the original MOF. NiCo/Fe3O4-MOF-74 shows excellent enrichment capability for the removal of tetracycline, with a high removal efficiency that reached 94.1% within 5 min, which is much higher than that of NiCoFe-MOF-74. The main interaction between the adsorbent and analyte is most likely attributed to the open metal sites that can form a stable metal-ligand with the antibiotic molecules. Furthermore, the material can be reused five times without considerable loss. The prepared material has potential applications for removing antibiotics with high efficiency at low cost. Therefore, the experiments described in this study provide a route to a broad class of MOF-based materials for detecting organic contaminants.


Subject(s)
Ferrosoferric Oxide/chemistry , Metal-Organic Frameworks/chemistry , Solid Phase Extraction/methods , Tetracycline/isolation & purification , Adsorption , Magnetic Phenomena , Tetracycline/chemistry , Water/chemistry
16.
Environ Res ; 183: 109195, 2020 04.
Article in English | MEDLINE | ID: mdl-32044570

ABSTRACT

Biochar (BC) derived from Chinese herbal medicine residues has been investigated for its performance as a potential adsorbent in tetracycline (TC) removal. In the present study, a chemical co-precipitation method was carried out to prepare manganese dioxide modified biochar (Mn-BC) to increase its sorption capacity. The properties of the modified biochar were characterized for further enhancing TC removal from an aqueous solution. Mn-BC was successfully synthesized and resulted in a much higher specific surface area, total pore volume and pore diameter. The sorption kinetics of TC on Mn-BC was described by the pseudo-second-order model. The sorption data of Mn-BC were fitted by Langmuir and Freundlich models. The study findings revealed a maximum adsorption capacity of Mn-BC (1:10) to TC was up to 131.49 mg/g. The adsorption process was endothermic and spontaneous. The degradation of TC was further enhanced by MnO2 acting as an oxidizer on Mn-BC. Overall, the modified biochar derived from Chinese herbal medicine residues is a superior alternative for the removal of TC from an aqueous solution.


Subject(s)
Drugs, Chinese Herbal , Tetracycline , Water Pollutants, Chemical , Water Purification , Adsorption , Charcoal , Kinetics , Manganese Compounds , Oxides , Tetracycline/isolation & purification
17.
J Hazard Mater ; 387: 121949, 2020 04 05.
Article in English | MEDLINE | ID: mdl-31927352

ABSTRACT

In this work, two multifunctional conjugated microporous polymers (CMP-LS7-8) were obtained via the Pd-catalyzed Suzuki coupling reactions of 2,4,6-tris(4-bromophenyl)pyridine with two aromatic borates. The Brunauer-Emmett-Teller (BET) surface areas of CMP-LS7-8 were calculated to be 507 and 2028 m2 g-1. CMP-LS7-8 exhibit excellent volatile iodine adsorption about 2.77 and 5.29 g g-1, respectively, and outstanding reversible adsorption. High adsorption capacity should be attributed to an integrated effect by excellent porous characteristics, effective sorption sites, and expanded π-conjugated network. In addition, this platform integrated two functions of sensing and adsorption of tetracycline (TC) into one material. The excellent luminescence of CMP-LS7-8 can be effectively quenched by TC, which demonstrates they can be acted as new sensitive and selective fluorescence probes toward TC. Simultaneously, CMP-LS7-8 also display high adsorption ability of TC. The adsorption kinetics of TC suggested that the process of adsorption followed a pseudo-second-order model, and the adsorption behaviour of these polymers fitted with the Langmuir model. These results suggest that CMP-LS7-8 posess high volatile iodine capture and exceptional TC detection and removal performance, which can be promising candidates for environmental remediation.


Subject(s)
Fluorescent Dyes/chemistry , Iodine/isolation & purification , Polymers/chemistry , Pyridines/chemistry , Tetracycline/isolation & purification , Water Pollutants, Chemical/isolation & purification , Adsorption , Fluorescent Dyes/chemical synthesis , Iodine/chemistry , Kinetics , Limit of Detection , Polymers/chemical synthesis , Porosity , Pyridines/chemical synthesis , Spectrometry, Fluorescence/methods , Tetracycline/analysis , Tetracycline/chemistry , Water Pollutants, Chemical/chemistry , Water Purification/methods
18.
Int J Biol Macromol ; 147: 258-267, 2020 Mar 15.
Article in English | MEDLINE | ID: mdl-31917217

ABSTRACT

In the present study, the magnetic nanocomposite is fabricated using chitosan, thiobarbituric acid, malondialdehyde and Fe3O4 nanoparticles (CTM@Fe3O4). The fabricated nanocomposite (CTM@Fe3O4) is characterized using FTIR, TGA, BET, XRD, Raman, XPS, FESEM, and HRTEM techniques. The results of BET analysis confirmed that the nanocomposite has a mesoporous structure with high surface area of 376 m2 g-1 and high pore volume 0.3828 cm3 g-1. The adsorption of tetracycline (TC) onto CTM@Fe3O4 adsorbent is carried out using batch technique by changing several factors such as pH, concentration, contact time, and temperature. Langmuir and pseudo-second-order nonlinear models were found to be the best-fit models to predict isotherms and kinetics of adsorption, respectively. The highest adsorption capacity of 215.31mg/g was achieved at the optimum conditions of 0.05g adsorbent dosage, 60mg/L TC concentration. Overall, results demonstrated that CTM@Fe3O4 nanocomposite was an excellent adsorbent material with superparamagnetic properties, which allowed the separation as well as recovery of the adsorbent from aqueous solution using external magnet for effective industrial applications.


Subject(s)
Chitosan/chemistry , Magnetic Phenomena , Nanocomposites/chemistry , Tetracycline/isolation & purification , Adsorption , Ferric Compounds/chemistry , Hydrogen-Ion Concentration , Kinetics , Malondialdehyde/chemistry , Nitrogen/chemistry , Photoelectron Spectroscopy , Spectroscopy, Fourier Transform Infrared , Spectrum Analysis, Raman , Thermodynamics , Thiobarbituric Acid Reactive Substances/chemistry , Time Factors , X-Ray Diffraction
19.
Chemosphere ; 239: 124831, 2020 Jan.
Article in English | MEDLINE | ID: mdl-31526986

ABSTRACT

The overuse of antibiotics, including tetracycline hydrochloride (TC), seriously threatens human health and ecosystems. In this work, magnetic carbon-coated cobalt oxide nanoparticles (CoO@C) were prepared by one-step annealing method and used as an adsorbent for efficient removal of TC from aqueous solution. The characteristic of the materials was studied by SEM, TEM, and XRD, revealing CoO nanoparticles (≤10 nm) were coated by carbon layer. Several influencial parameters, such as annealing temperature and pH on adsorption of TC, were explored, and found that the maximum adsorption capacity of CoO@C on TC reached as high as 769.43 mg g-1. Furthermore, CoO@C displayed excellent stability and reusability. After four repeated use of the adsorbent, the adsorption capacity still remained at 90% of the initial capacity. The pseudo-second order model and Temkin model proved that it was an exothermic chemical adsorption process. Furthermore, after analysis of FT-IR, Zeta-potential, XPS, the positive charge on the surface of CoO@C forms a strong electrostatic interaction with TC, and in addition, a surface bond is formed between the adsorbent and the TC molecule. This work provides a novel and efficient adsorbent for the purification of TC-containing wastewater.


Subject(s)
Cobalt/chemistry , Nanoparticles/chemistry , Oxides/chemistry , Tetracycline/chemistry , Water Pollutants, Chemical/isolation & purification , Adsorption , Anti-Bacterial Agents/chemistry , Carbon , Magnetics , Recycling , Tetracycline/isolation & purification , Wastewater/chemistry , Water Pollutants, Chemical/analysis , Water Purification/methods
20.
J Hazard Mater ; 384: 121320, 2020 02 15.
Article in English | MEDLINE | ID: mdl-31610346

ABSTRACT

Water pollution due to emerging contaminants (especially pharmaceuticals) is a major environmental threat which results in the development of antibiotic-resistant bacteria/resistance genes in the aquatic environment. Therefore, robust and cost-effective methods are required to address this problem. In this study, thermal activation was opted for the modification of natural bentonite clay (BC) and utilized to investigate the adsorptive removal of tetracycline (TC) from aqueous solution. The physicochemical surface properties of the raw and modified bentonite samples were also investigated. The BET analysis revealed that the thermally activated bentonite (TB) has better properties than BC. The surface area of TB was found to be more than two-fold higher compared to that of BC. The FTIR spectra exhibited the existence of AlOH, SiO and SiOSi functional groups in the samples, confirming the presence of hydrated aluminosilicate in the clay. The effects of various operating parameters were analyzed via optimization studies. The maximum monolayer adsorption capacity estimated by Langmuir model was found to be 156.7 and 388.1 mg g-1 for BC and TB, respectively. Furthermore, fixed-bed column studies were performed to get insights into the adsorption behavior of TB in a dynamic system. The mechanism of TC adsorption by TB was successfully explored.


Subject(s)
Anti-Bacterial Agents/isolation & purification , Bentonite/chemistry , Solutions/chemistry , Tetracycline/isolation & purification , Water Pollutants, Chemical/isolation & purification , Adsorption , Aluminum Silicates/chemistry , Thermodynamics , Water , Water Purification , X-Ray Diffraction
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