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Study On The NOx Storage And Reduction Performance Of The CuO/K2CO3/MgAl2O4 Catalyst At High Temperatures

Posted on:2018-07-23Degree:MasterType:Thesis
Country:ChinaCandidate:Y Y LiuFull Text:PDF
GTID:2321330542457085Subject:Industrial Catalysis
Abstract/Summary:PDF Full Text Request
High NOx removal efficiency has been achieved over the Pt/BaO/Al2O3 catalyst within a narrow temperature window of 300-400?.When the operating temperature exceeds 400?,Pt sintering and the low thermal stability of nitrates hamper the declines its application at high operating temperatures.To solve this problem,herein,we employ CuO to substitude of expensive Pt as the NOx oxidation and reduction center,potassium as the NOx storage element and MgAl2O4 as the support material,designing a new CuO/K2CO3/MgAl2O4 NSR catalyst operating at the high temperatures?350-550??.The CuO/K2CO3/Al2O3 catalyst was also prepared as a comparison.we characterized the catalysts by the X-ray diffraction?XRD?,X-ray absorption near-edge structures?XANES?,X-Ray photoelectron spectroscopy?XPS?,scanning electron microscopy?SEM?,high-resolution transmission electron microscopy?HR-TEM?,fourier-transforminginfraredspectra?FT-IR?,H2temperature-programmed reduction?H2-TPR?,temperature-programmed desorption of CO2?CO2-TPD?and temperature-programmed desorption of NOx?NOx-TPD?.The NOx reduction percentage?NRP?of the CuO/K2CO3/MgAl2O4 catalyst remains above90%over a wide temperature range?400-550??,and reaches the highest NRP of99.9%at 450? with the N2 selectivity of 99.7%.Based on our study,the CuO/K2CO3/MgAl2O4 catalyst can improve the NOx storage capacity of K2CO3 and the redox ability of CuO on it.Furthermore,CuO/K2CO3/MgAl2O4 catalyst can enhance the thermal stability of nitrate formed on it in the NOx storage stage.Therefore,the CuO/K2CO3/MgAl2O4 catalyst exhibits the high NSR performance at high operating temperatures.In this study,the effect of potassium loading on the NOx storage and reduction performance of the catalyst was also studied.In the catalyst,the K2CO3 exists as highly dispersed K2CO3 and bulk K2CO3.In the lean-burn period,the nitrates formed on the bulk K2CO3 have high thermal stability at high operating temperature,while the thermal stability of the nitrates formed on the highly dispersed K2CO3 is low.When the K loading is low,the K2CO3 mainly exists as highly dispersed K2CO3,the limited NOx storage capacity and the low thermal stability of the nitrates result in the low NSR activity at high temperature.While too much K2CO3 loaded on the catalyst can decrease the redox ability of CuO by covering it,which will decrease the NSR activity of the catalysts.When the K loading is 10%,the best NSR activity is obtained with the highest NOx reduction percentage at 450?.
Keywords/Search Tags:NO_xstorage reduction, Copper oxide, High temperature, MgAl2O4, Potassium loading
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