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Preparation,Characterization And Related Properties Of The Functional Composites Materials Used For Industrial Wastewater Treatment

Posted on:2018-05-15Degree:DoctorType:Dissertation
Country:ChinaCandidate:Z C YuanFull Text:PDF
GTID:1311330533455520Subject:Materials Science and Engineering
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With the development of the environmental conservation and the sustainable development concepts,water resource related problem attracts more and more attention in recent years.Many efforts have been focused on the environmental-friendly wastewater treatment to realize the protection and recycling of the water resource.In recent years,with the further research,many new treatment methods havev been continuously developed.However,the demands of the wastewater treatment also increase at the same time.Therefore,it is necessary to continuously improve the wastewater treatment methods.In this paper,Fe3O4 was introduced onto the surface of attapulgite(AT)by ultrasound-deposition method to prepare a series of the magnetic attapulgite functional nanocomposites materials(AT/Fe3O4)for the dyes wastewater treatment.This nanocomposites materials showed excellent adsorption capability and worked out the recycling problem of the AT by using magnetic separation technique.On the basis of this research,Fe-octacarboxylic acid phthalocyanine(Fe OCAP),which possessed high photocatalytic activity property,was utilized to prepare novel AT/Fe3O4-FeOCAP functional nanocomposites materials.The photocatalytic degradation property of the nanocomposites materials for dyes wastewater was investigated.To meet the smart requirement for the wastewater treatment materials,the multiple stimulus-responsive nanocomposites hydrogels were applied to remove dyes from wastewater.The treatment process could be controlled by the various smart responsive properties of the hydrogels.Besides,the surface molecular imprinting functional nanocomposites materials were investiged to selective recognize the specific target from heavy metal wastewater.The main contents were as follows:(1)The AT/Fe3O4 magnetic nanocomposites were prepared by ultrasound-deposition method.Fourier transform infrared spectroscopy(FTIR),X-ray diffraction analysis(XRD),field emission scanning electron microscopy(FESEM),BET specific surface area measurements and vibrating sample magnetometry(VSM)were used to characterize the AT/Fe3O4 nanocomposites.The results indicated that Fe3O4 nanoparticles were well dispersed on the surface of AT and the AT/Fe3O4 nanocomposites showed excellent absorption capability and magnetic property.The removal percentage of Rhodamine B(RhB)dyes could reach above 90% in a short time,which could be well described by the pseudo-second order kinetic model.With the pH value increasing,the removal percentage of the cationic dyes obviously improved.These nanocomposites could be effectively separated from aqueous and recollected by simply applying an external magnetic field.After four recycles,the removal percentage of dyes could still reach above 60%.The application potential of the AT/Fe3O4 in real industrial wastewater treatment was invistaged by simulation the dynamic adsorption process experiment.(2)Novel nanocomposites photocatalysts(AT/Fe3O4-FeOCAP)were successfully prepared from Fe-octacarboxylic acid phthalocyanine(Fe OCAP)and AT/Fe3O4 by an ultrasonic method.FTIR,UV-Vis,XPS and photocatalytic degradation experiment were used to characterize the nanocomposites photocatalysts.The results showed that the FeOCAP was successfully introduced onto the surface of the AT/Fe3O4 nanocomposites.The face-to-face macrocycles aggregation of the FeOCAP could be eliminated by using AT/Fe3O4 as the matrix,which implied that the photocatalytic activity had been improved.The band gap and Fermi level analysis proved that the photocatalytic activity could improve with the content of FeOCAP increasing.The as-prepared photocatalysts had excellent RhB photodegradation property and could prevent the maximum adsorption and complicated reused process problem of the traditional adsorption materials.The kinetic data was well fitted by the Langmuir-Hinshelwood kinetic model.(3)The multiple stimulus-responsive organic/inorganic hybrid hydrogels by combining poly(2-(2-methoxyethoxy)ethyl methacrylate-co-oligo(ethylene glycol)methacrylate-co-acrylic acid)(PMOA)hydrogel with AT/Fe3O4 nanocomposites were prepared to meet the smart process demands for the dyes wastewater treatment.The dyes adsorption experiment was carried out to analyze the properties of the hydrogels.The hydrogels had excellent adsorption capability of Rh B dyes.The pseudo-second order kinetic model and Langmuir isotherm model could be used to describe this adsorption process,which indicated that the adsorption process was preferred to the heterogeneous adsorption system.The hydrogels still possessed temperature,pH and magnetic-field sensitivity during the adsorption process,and thus the adsorption could be controlled by the responsive properties of the hydrogels.Utilization those responsive properties,the hydrogels could be simply reused four times and still show high removal percentage of the RhB dyes.(4)The Fe OCAP/MAT-PMOA photocatalyst hydrogels was successfully synthesized by the introduction of the excellent photocatalytic AT/Fe3O4-FeOCAP nanocomposites into PMOA matrix.FTIR result showed that there were hydrogen bond interactions between AT/Fe3O4-Fe OCAP and PMOA matrix,which acted as the crosslink points in the hydrogels network.Therefore,those hydrogen bond interactions could stabilize the AT/Fe3O4-FeOCAP in hydrogels network without phase separation to improve the photocatalytic property.Photocatalytic degradation studies confirmed that the RhB removal percentage by the as-prepared nanocomposites hydrogels could nearly reach 100% and the kinetics of photocatalytic degradation reaction could be also described by the Langmuir-Hinshelwood kinetic model.The recycle experiment showed that the stabilization of FeOCAP was improved and the leaking process to the aqueous was prevented by the introduction of the hydrogels matrix.The hydrogels could be reused more than 5 times without losing any photocatalytic degradation capability.With the external environment changing,this hydrogels still showed various smart responsive properties and removal percentage of Rh B dyes.(5)The pH responsive Cu(II)-imprinted smart hydrogels was prepared by surface molecular imprinting technique using attapulgite as the matrix material,Cu(II)as the target,which could be used to selective recognition target in the heavy metal wastewater treatment.The FTIR results showed that the copper ion could be removed by using aqueous 1.0M HNO3 to form imprinted sites which could be used in the next selective recognization process.In the selection recognition experiment,the as-prepared imprinted hydrogels showed a higher affinity for Cu2+,and the adsorption equilibrium data fitted Freundlich isotherm model well.The hydrogels could be reused five times without obviously losing selective recognization property and adsorption capability.In addition,Cu(II)-imprinted hydrogels still had pH responsive property,which could be used to control the various selective recognization properties.
Keywords/Search Tags:attapulgite, Fe-octacarboxylic acid phthalocyanine, smart hydrogels, photocatalytic degradation, magnetic separation and recollection, molecular imprinting, industrial wastewater treatment
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