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1.
Environ Pollut ; 255(Pt 2): 113226, 2019 Dec.
Article in English | MEDLINE | ID: mdl-31546075

ABSTRACT

In this paper, Fe3O4@MIL-68 (Al), a magnetic aluminum-based metal organic framework, was synthesized by a simple method and used as a novel and effective adsorbent for the removal of minocycline (MC) from aqueous solutions. The material was thoroughly characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), Fourier-transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), thermogravimetric analysis (TGA) and N2 adsorption isotherms. The characterization results showed that the original structure of MIL-68(Al) was unchanged by the addition of Fe3O4 nanoparticles, and that the obtained material had a strong magnetic response which also promoted its adsorption. Batch adsorption experiments were conducted by the varying the adsorption time, temperature, initial MC concentration and pH. The maximum adsorption amount of MC onto Fe3O4@MIL-68 (Al) was 248.05 mg g-1 (t = 160 min, pH = 6, Co = 60 mg L-1), and the adsorption kinetics followed a pseudo-second-order model, and the adsorption isotherms conformed to the Freundlich equation. The adsorption mechanism of the magnetic metal organic framework materials were determined to involve complex interactions, including Al-N and Fe-N covalent bonds, hydrogen bonding, electrostatic adsorption, and π-π stacking. Combined the results indicate that Fe3O4@MIL-68 (Al) is an outstanding adsorbent for the removal of MC from water.


Subject(s)
Minocycline/analysis , Water Pollutants, Chemical/analysis , Water Purification/methods , Adsorption , Aluminum/chemistry , Hydrogen Bonding , Hydrogen-Ion Concentration , Kinetics , Magnetic Phenomena , Magnetics , Metal-Organic Frameworks , Microscopy, Electron, Scanning , Water/chemistry , Water Pollutants, Chemical/chemistry , X-Ray Diffraction
2.
Environ Sci Pollut Res Int ; 26(4): 3685-3696, 2019 Feb.
Article in English | MEDLINE | ID: mdl-30535742

ABSTRACT

The presence of tetracycline antibiotics (TCS) in the water and wastewater has raised growing concern due to its potential environmental impacts; thus, their removal is of high importance. In this study, a novel aluminum-based MOF/graphite oxide (Al-MOF/GO) granule was prepared as an adsorbent for the removal of TCS including oxytetracycline (OTC) and chlortetracycline (CTC). The adsorbent was characterized via XRD, FTIR, BET, SEM, and XPS methods. The granules exhibited similar crystal structure and some new mesopores appearing compared to the parent Al-MOF/GO powder. In addition, the adsorption behavior of OTC and CTC on samples was explored as a function of initial concentration, contact time, pH, and ionic strength by means of batch experiments. The adsorption capacity reached to 224.60 and 240.13 mg·L-1 for OTC and CTC, at C0 = 60 mg·L-1 as well as ambient temperature respectively. Moreover, the adsorption process of OTC and CTC on Al-MOF/GO samples can be better delineated by pseudo-second-order kinetics and Freundlich isotherm models. Besides, the adsorption mechanism over Al-MOF/GO granules was proposed, which could be ascribed to π-π interaction, cation-π bonding, and hydrogen bond. Finally, the great water stability, separation performance, and regeneration efficiency of these novel granules indicated their potential application in the OTC and CTC removals from aqueous solution.


Subject(s)
Chlortetracycline/isolation & purification , Metal-Organic Frameworks/chemistry , Oxytetracycline/isolation & purification , Water Pollutants, Chemical/isolation & purification , Adsorption , Aluminum/chemistry , Anti-Bacterial Agents/chemistry , Anti-Bacterial Agents/isolation & purification , Chlortetracycline/chemistry , Graphite/chemistry , Hydrogen Bonding , Kinetics , Microscopy, Electron, Scanning , Osmolar Concentration , Oxytetracycline/chemistry , Solutions , Spectroscopy, Fourier Transform Infrared , Wastewater/chemistry , Water Pollutants, Chemical/chemistry , Water Purification/methods , X-Ray Diffraction
3.
Ecotoxicol Environ Saf ; 164: 289-296, 2018 Nov 30.
Article in English | MEDLINE | ID: mdl-30125775

ABSTRACT

Tetracycline (TC) as a typical antibiotic has been used extensively and detected in soil, surface water, ground water and drinking water, which results in toxic effect and bacterial resistance. In this study, aluminum-based metal organic framework/graphite oxide (MIL-68(Al)/GO) pellets were prepared through the addition of sodium alginate (SA), a natural crosslinking agent, and applied as a novel adsorbent for aqueous TC removal. The adsorption materials were characterized by scanning electron microscope (SEM), X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), N2 adsorption-desorption analysis and X-ray photoelectron spectroscopy (XPS). Results demonstrated that the pellets maintained similar chemical structure with parent MIL-68(Al)/GO powder. It is noted that the surface area and total volume of the pellets decreased obviously due to the disappearance of micropores. Besides, the efficiency of MIL-68(Al)/GO pellets for TC removal was evaluated by adsorption properties compared with parent powder, including key influential parameters, and adsorption isotherms, kinetics and mechanisms. It is found that the adsorption process was conformed to pseudo-first-order kinetics model and more suitably described through Langmuir isotherm model, with 228 mg g-1 of the maximum adsorption capacity. Moreover, these pellets which were separated easily and quickly presented high adsorption capacity and good stability in a wide pH range. The adsorption mechanism of the pellets may be ascribed to the complex interactions of hydrogen bonding, π-π stacking as well as Al-N covalent bonding. Overall, the MIL-68(Al)/GO pellets might be a promising adsorbent and show great potential for the removal of aqueous TC.


Subject(s)
Anti-Bacterial Agents/chemistry , Oxides/chemistry , Tetracycline/isolation & purification , Water Pollutants, Chemical/chemistry , Water Pollutants/analysis , Water Purification/methods , Adsorption , Graphite/chemistry , Groundwater , Hydrogen-Ion Concentration , Ions , Kinetics , Powders , Wastewater/chemistry , Water , X-Ray Diffraction
4.
Water Sci Technol ; 75(12): 2800-2810, 2017 Jun.
Article in English | MEDLINE | ID: mdl-28659520

ABSTRACT

MIL-68(Al), a powdered aluminum-based metal organic framework (MOF), was synthesized and used to explore its adsorption behavior toward methyl orange (MO). The adsorption isotherm, thermodynamics, kinetics, and some key operating factors as well as changes in the material's structure were investigated. The adsorption isotherm conformed to the Langmuir isotherm model and the maximum equilibrium adsorption capacity was 341.30 mg g-1. Thermodynamic data demonstrated that the adsorption process was spontaneous, endothermic and showed positive entropy. For kinetics, the process of MO adsorption onto MIL-68(Al) was more suitably described by a pseudo-second-order model. Electrostatic and hydrogen-bonding interactions contributed to dye adsorption, with electrostatic interactions considered to be the principal binding force between adsorbent and adsorbate. Furthermore, MIL-68(Al) maintained a stable structure after adsorption. From these results, MIL-68(Al) was suggested here to be a stable MOF adsorbent for removing MO from aqueous solution.


Subject(s)
Aluminum , Azo Compounds , Metal-Organic Frameworks , Models, Chemical , Water Pollutants, Chemical , Adsorption , Aluminum/chemistry , Azo Compounds/chemistry , Hydrogen-Ion Concentration , Kinetics , Thermodynamics , Water Pollutants, Chemical/chemistry
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