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Synergetic Photocatalytic Activity And Visible Light Response:Consolidation Of Reactive Oxygen Species By Composites

Posted on:2020-06-18Degree:DoctorType:Dissertation
Country:ChinaCandidate:Haroon Ur RasheedFull Text:PDF
GTID:1361330596996748Subject:Environmental Science and Engineering
Abstract/Summary:PDF Full Text Request
Today's world,tetracycline hydrochloride?TC?considered as a Compounds of Emerging Concern?CECs?.Recently,metal-organic frameworks MOFs with a microporous structure and holding larger pores indicating potential applications in the fields of environmental purification.Carbon aerogel?CA?has also aroused great interest due to its larger specific surface area,low density,thermal stability,and non-toxicity.The synthesis of relevant catalysts was carried out around the synthesis of MOFs and CA materials,and the study on the photocatalytic degradation of tetracycline hydrochloride was carried out.Herein,MIL-100?Fe?was synthesized under low temperature and combined with Fe3O4 and CA,respectively.The obtained MIL-100?Fe?,MIL-100?Fe?@Fe3O4,MIL-100?Fe?@CA and MIL-100?Fe?@Fe3O4/CA investigated as a photocatalyst for removal of TC from the water.The results indicated that the MIL-100?Fe?@Fe3O4/CA degrade TC up to 85%,which is much higher than MIL-100?Fe?@Fe3O4?c.a.42%?,due to its high surface area 389 m2g-1,smaller pore size and pore volume 2.4 nm and 0.319 m3g-1,high separation of electron and hole,and lower band gap of1.76 eV.The coupling of CA with MIL-100?Fe?@Fe3O4 considerably accelerate the transfer of photo-generated charge carriers and enhanced 1.6 times the performance of MIL-100?Fe?@Fe3O4.Furthermore,the stability and recyclability were improved due to the addition of Fe3O4,facilitating the environmentally friendly water purification processes.The use of heterostructure photocatalysts becomes a more promising method for decontamination.In this work,synthesis of?-Fe2O3 done without using NH3.H2O and achieved the composite??-Fe2O3@CN?doped with CN?graphitic carbon nitride?,without calcination involved.The characterization of the composite was done by XRD,FT-IR,SEM,DRS,XPS,PL,and EIS to confirm the bandgap,functional groups,spherical structure of the?-Fe2O3,ability to absorb the visible light,detection of elements?Fe,O,C and N?,and the better charge separation.Results indicated the proper ratio of?-Fe2O3 and CN to enhance the bandgap and to speed-up the photodegradation of the TC.As compared with pure?-Fe2O3 and CN,the composite?-Fe2O3@CN exhibited more effective photocatalytic TC degradation under the visible-light spectrum.An obvious enhancement is observed when?-Fe2O3 is coupled onto CN,with a proper loading rate,i.e.,?-Fe2O3@1.5 CN,has highest removal efficiency due to better distribution of?-Fe2O3 on CN nano-sheets,which leads to the production of the Reactive Oxygen Species?O2-and?OH radical?and limit the electron and hole recombination,synergies the photodegradation of TC,suggesting the potential environmental application.The composite?-Fe2O3@1.5 exhibited 3.25-and 2.18-times better degradation as compared to CN and?-Fe2O3 respectively.Results also compared different loading rates of?-Fe2O3 and CN,indicating that the degradation of?-Fe2O3@1.5 CN is 2.45-and 1.63-times better than?-Fe2O3@0.75 CN and?-Fe2O3@3.0 CN respectively.The stability of the photocatalyst was investigated through the cyclic process.The results showed that after washing five times,there was no significant change observed in the rate of degradation.Herein,ZnO@CN nanocomposites synthesized by facile thermal decomposition strategy with loading certain concentrations of ZnO and CN.The as-prepared photocatalyst was used to examine the photodegradation studies against antibiotic tetracycline hydrochloride?TC?as an environmental pollutant most commonly used in the pharmaceutical industry and investigate their degradation through ZnO@CN.The characterization of ZnO@CN was done by different analytical techniques such as XRD,FT-IR,SEM,DRS,XPS,PL and EIS which indicated that the composite has a narrow bandgap,hexagonal-shaped nanobolts structure,high stability,maximum ability to absorb visible light spectrum,high adsorption ability,and excellent charge separation.In this research,it was observed that a balanced ratio of ZnO and CN play a vital role in charge separation and provide standard bandgap which participates to boost-up photocatalytic degradation under visible light spectrum.As compared with pure CN and ZnO,the composites ZnO@CN-2showed more efficient photocatalytic activity for TC degradation under the visible-light spectrum.The most advantageous CN amount in ZnO@CN-2 nanocomposite exhibited 2.77-and 1.51-times faster photodegradation as compared to CN and ZnO respectively.The ZnO@CN-2 showed better photodegradation for the oxidation of TC under visible light irradiation,as compared to the other composites with different ZnO to CN ratio.The cyclic process investigated the stability of the photocatalyst.The results showed that after washing five times,there was no significant change observed in the rate of degradation.Moreover,the coupling of CN with ZnO facilitates the photodegradation phenomena by providing active sites,producing rich oxygen species and limiting the electron and hole recombination,which lead to better degradation of tetracycline hydrochloride under the solar irradiation spectrum.
Keywords/Search Tags:Tetracycline hydrochloride, Photocatalysis, MIL-100?Fe?@Fe3O4, CN, ?-Fe2O3, ZnO
PDF Full Text Request
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