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The Effect Of CeO2 Modification And Facet-tuned On Photo-oxidation Of Elemental Mercury

Posted on:2021-05-28Degree:MasterType:Thesis
Country:ChinaCandidate:M J LinFull Text:PDF
GTID:2381330611962453Subject:Environmental Engineering
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Elemental mercury?Hg0?is one of the most harmful environmental pollutants.It is another difficult problem in the field of air pollution control for how to efficiently control its emissions.Due to the high-efficiency and low-temperature catalytic performance,TiO2 is used for Hg0 removal.While its photocatalytic oxidation efficiency is significantly suppressed when the reaction temperature is too high?>100°C?.However,the catalytic efficiency can be effectively improved by changing the chemical composition of the catalyst surface and adjusting the crystal structure.Therefore,cerium dioxide?CeO2?with a narrow band gap width,high reactivity and excellent oxygen storage capacity was selected as a modifier.And CeO2/TiO2 were prepared by the sol-gel method,then explore the effects of energy band structure,types and number of surface free radicals,and their photocatalytic performance for mercury removal,clarify the mechanism of CeO2 modification to promote the photocatalytic oxidation of Hg0 by TiO2.Subsequently,the effect of facet-tuned TiO2 and CeO2modification on the photocatalytic performance of mercury removal was studied,and the synergistic effects of crystal plane effect and CeO2 modification on energy level structure,generation of strong oxidizing free radicals,and photocatalytic activity were studied.And clarify the photocatalytic reaction path.The main conclusions of this study are as follows:?1?Preparation of CeO2 modified TiO2 catalyst and its mercury removal performance.CeO2/TiO2 catalyst is granular,and the average particle diameter is 20-30 nm;TiO2 is an anatase type,and CeO2 with an amorphous structure,exists in the gap of the TiO2 lattice structure.?2?The reaction mechanism of CeO2/TiO2 catalyst in removing Hg0.The doping of CeO2 can reduce the band gap of TiO2,reduce the inherent ohmic resistance of TiO2and inhibit the recombination of electron-hole pairs and thereby improve the photocatalytic activity.In addition,4%CeO2/TiO2 has the best photocatalytic activity due to the the potential difference between its conduction band potential and O2/·O2-standard redox potential and its low inherent resistance.This is consistent with the characteristics of its band structure.The CeO2/TiO2 catalysts contribute to the formation of·O2-rather than·OH,which affects the photo-oxidation mechanism of Hg0.?3?Preparation of CeO2-TiO2 catalyst with different exposed crystal planes and Hg0 removal performance.TiO2{001}has a nano-plate morphology and an octahedral structure with a particle size of 50-200 nm.All five unsaturated coordination bonds on the crystal surface increase the adsorption sites.TiO2{101}and TiO2{001-101}are granular,with a particle size between 20-50 nm.The TiO2{101}crystal plane is a double-pyramid structure,and all of them have 6 saturated coordination bonds,and there are fewer adsorption sites.CeO2 supported by the dipping method is mainly dispersed on the surface of CeO2-TiO2{101},and does not change the morphology and structure of TiO2.?4?Study on the synergy effect of crystal plane effect and CeO2 loading.Due to the formation of new Ti-O-Ce bonds,new Ce 4f energy levels are introduced into the valence and conduction bands of TiO2,and CeO2 can reduce the band gap and reduce the electrochemical impedance of CeO2-TiO2 and promotes charge transfer.In addition,7%CeO2-TiO2{001}has the highest photocatalytic activity at 50-150? due to the formation of more surface Ti3+and superoxide radicals on its crystal plane;However,the surface Ti3+and superoxide free radicals are suppressed by high temperature.CeO2has high temperature stability and deposits most on{101}surface,which is helpful for photocatalytic oxidation to remove Hg0.Thus 7%CeTi{101}has the highest photocatalytic activity at 200-250?.
Keywords/Search Tags:TiO2, Photo catalysis, Elemental mercury(Hg~0), Band structure, CeO2, Crystal plane
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