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Study Of Catalytic Oxidation Of Cyclohexane Over Cu-based Catalysts

Posted on:2013-10-25Degree:MasterType:Thesis
Country:ChinaCandidate:X Q GuFull Text:PDF
GTID:2231330371485509Subject:Polymer Chemistry and Physics
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Cyclohexanone is an important organic chemical intermediate, many methods ofcatalyst preparation are not only complex but also time-consuming. Thus, a simplepreparation method of catalyst plays an important significance in cyclohexane oxidation tocyclohexanol and cyclohexanone.In this paper, two Cu-based catalysts were prepared, and which were applied toselective oxidation of cyclohexane with30%H2O2. The effects es of these catalystspreparation conditions and oxidation reaction parameters on their catalytic performanceswere investigated in cyclohexane oxidation to cyclohexanone and cyclohexanol with30%H2O2as the oxidant.Copper pyrophosphate catalyst was prepared by precipitation Method andcharacterized by XRD. The characterized experiment result indicated that at2θ=28.327,30.199,35.402,35.943which are copper pyrophosphate. The the optimum preparationcondition of copper pyrophosphate catalyst that Cu/P ratio is1.0, stir time is20h, andcalcined temperature is550℃. using10mL of acetonitrile,8mmol of cyclohexane,0.0300g of copper pyrophosphate catalyst,3.00mL of w (H2O2)=30%hydrogen peroxideat temperature of65℃for10h, the conversion of cyclohexane reached54.1%, the yieldof cyclohexanol reached21.3%, the yield of cyclohexanone reached32.8%. Theselectivity of cyclohexanol and cyclohexanone reached41.3%and58.7%, respectively.A catalyst comprising Cu/HZSM-5molecular sieves was prepared by ion exchangeand characterized by XRD, BET, ICP, FT-IR and TG/DTA. Crystallization of CuO occursbetween300and400℃. The presence of various ligand bonds between the support andthe copper species scattered in the molecular sieve matrix. Cu/HZSM-5with10%coppernitrate solution, ion exchange temperature80℃, ion exchange and calcinationtemperature of600℃exhibited the best performance. Using acetonitrile10mL,cyclohexane0.5mL, catalyst0.03g,4mL of w (H2O2)=30%hydrogen peroxide at65℃for6h, the cyclohexane conversion and the total selectivity to cyclohexanol andcyclohexanone were43.1%and95.7%, respectively.
Keywords/Search Tags:copper pyrophosphate, Cu/HZSM-5catalyst, cyclohexane, cyclohexanone, hydrogen peroxide, oxidation
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