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Exfoliation And Compound Of Layered Mg/Al LDHs And MnO2 And Their Adsorption Performance

Posted on:2016-03-07Degree:DoctorType:Dissertation
Country:ChinaCandidate:Y X YanFull Text:PDF
GTID:1311330542975970Subject:Materials science
Abstract/Summary:PDF Full Text Request
In recent year,2D nanomaterials has became research focus in the field of nanomaterials for their excellent performance in sensors,photocatalysis,capacitor,and adsorption etc.Now,nuclear energy has playing an increasingly important role in human life.Adsorption is recognized as a new,efficient and economical method for separation and enrichment of uranium.Adsorption has good prospects.In the process of adsorption,2D nanosheets has more exposure interface and adsorption sites compared to bulk materials.In this paper,three kinds of effective solution exfoliation Methods has proposed.Used thosethreemethods,wepreparedLDHsandMnO2nanosheetsuccessfully.SEM,TEM,XRD and other testing means,has used to confirm the morphology and formation mechanism of product.Compositing with Fe3O4,a series of magnetic materials,such as Fe3O4@E-LDHs and Fe3O4@E-MnO2 has prepared.The introduction of Fe3O4 magnetic particles makes the fast and efficient recovery of adsorbent.The uranium adsorption properties by as-prepared products are investigated.Mg/Al LDHs ultrathin nanosheetswere successfully prepared byMg/Al-CO32-LDHs as precursor,NH4NO3 as plate expander,formamide as agent.E-LDHs ultrathin nanosheets colloidal substance was completely transparent,with obvious Tyndall effect,the diamete of E-LDHs about hundreds of nanometer and the thickness is about 8.7 nm.We prepared E-LDHs film for methyl orange(MO)adsorption.The results show that LDHs layered structure maintaind well after the adsorption.In the interlayer,MO-ion in parallel to the LDHs plate.With Fe3O4 magnetic material as substrate,Fe3O4@E-LDHs composite material was successful prepared.Fe3O4@E-LDHssize is about 12μm,with uneven surface and severalFe3O4sphericalparticlescloselybondedtogetherby LDHs.Fe3O4@E-LDHs composite has good magnetic response,saturation magnetization is23.5 emu/g.Study found that Fe3O4@E-LDHs composite has good uranium adsorption properties.When Co=121.1 mg/L,Fe3O4@E-LDHs is 0.01 g,adsorption timeis 2h,adsorption temperature is 25℃and pH=5,the uranium adsorption capacity reached224.6mg/g.Kinetic studies showed that Fe3O4@E-LDHsadsorption of uranyl is homogeneous monolayer adsorption.Thermodynamics research shows that Fe3O4@E-LDHs on adsorption of uranium in different temperature are all showed:(35)G0<0,(35)H0>0,indicating that the adsorption is the endothermic process,adsorption reaction occur spontaneously.Suggesting that raise the temperature promote adsorption reaction.Using K-MnO2 as precursor,with the protonation exchanging and solution exfoliation steps,E-Birnessite nanosheets were prepared.Addition K-MnO2 to(NH42S2O8 solution can occur following changes:(001)peak changed from 12.967°to 12.300°,suggesting interlayer spacing increased from 0.6823 nm to 0.7198 nm,and the transformation of K-MnO2 structure to the H-MnO2 happened.With H-MnO2 as precursor,TMAOH as solvent,E-MnO2 ultrathin nanosheets can be prepared successfully,the nanosheet thickness is about 5.2nm,about 7 MnO2 layers.At the same time,the nano film has spontaneousstacking,crimpcharacteristics.StudiesshownH-Birnessite(001)and(002)peaks gradually shift to lower angles,(001)peaks were appeared in10.959°,9.480°and 7.351°,corresponding to layer spacing 0.8074 nm,0.9330 nm and1.2027 nm.Compared to K-MnO2,H-MnO2layer spacing of 0.7198 nm increased a lot,and layered structure from crystal structure change into a non crystal structure.With Fe3O4 magnetic material as substrate,Fe3O4@E-MnO2 composite material was successful prepared,Fe3O4@E-MnO2 size is about sevralμm,dozens of Fe3O4 spherical particles closely bonded together by MnO2.Those composite has good magnetic response,the saturation magnetization is 41.6 emu/g.Studies found that Fe3O4@MnO2composite has good adsorption properties for uranium.When Fe3O4@MnO2 is 0.01g,adsorption time is 6 h,C0=688.9 mg/g,T=45°C,the adsorption capacity reached1325.8mg/g.Kinetic studies showed that Fe3O4@E-MnO2 adsorption of uranyl ion in water is more in line with the pseudo-second-order kinetics with R2=0.9903.The Langmuir isothermal adsorption equation can describe the adsorption behavior of Fe3O4@E-MnO2.So,adsorption is homogeneous monolayer adsorption.H2O2as solvent,usingpropertyof H2O2exfoliatedLDHslayered materialsintoultrathinnanosheets.AlargenumberofO2generationwhen H2O2 decomposition and create a super high pressure environment.For violent movement of molecularoxygen,theLDHslayeredmaterialsexfoliatedintoultrathin nanosheets,realizating the LDHs layer prepation in one step.Changing H2O2 concentration to 0 wt%,10 wt%,20 wt%and 30 wt%,results show that with the increase of H2O2concentration,crystallization degree of LDHs decreased and the interlayer spacing increased.At the same time,the LDHs product is becoming more and more transparent,whenhydrogen peroxide content reached 30wt%,the product is translucent gelatinous material.the product is ultrathin nanosheets,with size of 50100nm,thickness is 1.4 nm(two LDHs layers).LDHs prepared by the method of strip products with high thermal stability.
Keywords/Search Tags:Uranium adsorption, LDHs, Manganese dioxide, Magnetic materials
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