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Molten-salt Preparation Of Pt/TiO2 Catalysts And Their Catalytic Performance For VOCs Removal

Posted on:2019-02-06Degree:MasterType:Thesis
Country:ChinaCandidate:S LiFull Text:PDF
GTID:2381330593450297Subject:Chemical Engineering and Technology
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Volatile organic compounds?VOCs?cause harmful effects on the atmospheric environment and human health.Therefore,effectively controlling and reducing the emission of VOCs has great significance.Catalytic oxidation technology has high purification efficiency,low energy consumption and no secondary pollution,and the core of this technology is the development of high-performance catalysts.Molten salt method is a method for preparing nanomaterials with simple operation and moderate reaction temperature.In this paper,we used in-situ molten salt method to prepare TiO2catalysts with low loadings of noble metal Pt and Ce-,V-,or W-doped 0.05 wt%Pt/TiO2 catalysts.The catalytic activities of toluene?or acetone?oxidation and other properties?stability,water resistance,sulfur resistance,etc.?were investigated.The main conclusions are as follows:different molten salt systems and calcination temperatures have an impact on the catalytic activity of the catalysts.When Ti?SO4?2was used as titanium precursor,the sample with the best catalytic activity of toluene oxidation was calcined at 300 oC in NaNO3 and NaF molten salt systems.Using H2PtCl6 as a platinum precursor,different Pt loading catalysts were prepared by varying the amount of solution.The obtained TiO2 was anatase structure of tetragonal phase.Its morphology was irregular and its size was about 200 nm.Pt particles were highly dispersed on the TiO2 support.Over the x wt%Pt/TiO2 catalysts,the reduction peaks ascribed to the reduction of lattice oxygen species of TiO2 shifted toward the low temperature.That is to say,the reactivity of surface lattice oxygen species was enhanced via the loading of Pt onto TiO2.Under the reaction conditions of acetone or toluene concentration=1000 ppm,acetone/oxygen or toluene/oxygen molar ratio=1/400,and space velocity?SV?=40000 mL/?g h?,the catalytic activity increased with a rise in the loading of Pt.The catalytic activity of 4.14 wt%Pt/TiO2 was the best,T50%and T90%?the reaction temperature required for 50%and 90%conversion of acetone?were 172 oC and 195 oC,respectively.While T50%and T90%over 0.05 wt%Pt/TiO2 were 236 oC and 274 oC,respectively.It should be noted that the addition of Ce?V,or W?into 0.05 wt%Pt/TiO2 could improve the catalytic activity.The catalytic activities of the Ce-doped 0.05 wt%Pt/TiO2 catalysts first increased with a rise in the amount of CeO2 from 0 to 0.57 wt%,and then decreased with a further increase from0.57 to 1.61 wt%.Compared to 0.54 wt%V2O5-0.05 wt%Pt/TiO2 and 0.55 wt%WO3-0.05 wt%Pt/TiO2,0.57 wt%CeO2-0.05 wt%Pt/TiO2 catalyst had high surface oxygen adsorbed species concentration.T50%and T90%over 0.57 wt%CeO2-0.05 wt%Pt/TiO2 were 212 oC and 245 oC,respectively.Water resistance,CO2 resistance and sulfur resistance had also been improved.After addition of 20 vol%water vapor,10vol%CO2,or 100 ppm SO2 into the reactant,more than 85%,70%,and 60%of acetone were eliminated,respectively.The improvement in SO2-tolerance was due to?i?Ce,V,or W-doping increased the amount of surface acid sites,and then inhibited the adsorption of acidic SO2;?ii?the generation of Ce2?SO4?3 or VOSO4 partially consumed SO2 and then inhibited the formation of Ti?SO4?2 or TiOSO4;and?iii?WO3modified catalyst inhibited SO2 oxidation activity.The complete oxidation of acetone over 0.57 wt%CeO2-0.05 wt%Pt/TiO2 involved the following procedures:gaseous acetone molecules were first adsorbed on the catalyst surface,and then partially decomposed to generate formate species at low temperature.With an increase in the reaction temperature,the formate species were changed to the carbonate species.Finally,the intermediates were totally oxidized to CO2 and H2O.
Keywords/Search Tags:volatile organic compounds, catalytic oxidation, supported Pt catalyst, molten-salt method, H2O,CO2,and SO2-resistance
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