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Catalytic Remove Of Soot Over Cu,Ce Or Mn Metal Oxides Supported HZSM-5 Zeolite Catalysts

Posted on:2017-06-08Degree:MasterType:Thesis
Country:ChinaCandidate:L WangFull Text:PDF
GTID:2321330512480427Subject:Industrial Catalysis
Abstract/Summary:PDF Full Text Request
Continuous renewable trap?CRT?is the most effective technology to eliminate soot particles in diesel exhaust.Development of high-performance catalytic combustion catalyst is the key factor of this technology.In this paper,the Cu,Mn and Ce metal oxide catalysts supported by HZSM-5 zeolite were studied.The catalysts were characterized by XRD,BET,TEM,SEM,NH3-TPD,H2-TPR,XPS,NO2-TPD and in situ DRIFTS.The activities of the catalysts were investigated under different conditions.Moreover,the TOF values of the catalysts were calculated by isothermal anaerobic titration,and the apparent activation energys?Ea?of catalytic soot combustion on the catalysts were calculated by TG/DTA testing.The catalysts loaded with different types of Cu species over HZSM-5 zeolite were prepared by cuprammonium evaporation method,and the referential sample was prepared by incipient wetness impregnation method.The effect of different Cu species in the soot catalytic combustion was investigated.In the loose contact mode,the isolated Cu?II?inside the zeolite,as the main active sites,has the strong oxidation ability of NO to NO2.In the tight contact mode,because the CuO particles on the external surface of zeolite can cantact with soot,it can directly provide reactive oxygen species for soot combustion.Compared with the catalyst of SiO2 loading CuO,the catalyst 9.5Cu-Z shows the superior catalytic activity.On the one hand,the isolated Cu?II?inside the HZSM-5 has a strong oxidation ability of NO to NO2.On the other hand,the acidicity of HZSM-5 inhibits NO2 adsorption on the catalyst,leading to a preferential adsorption of NO2 on the surface of soot and providing more chances for NO2-soot reactions.Moreover,the storage pathways of NO2 and the NO2-soot reaction mechanisms were discussed by situ DRIFTS.Moreover,the Mn,Ce and Mn-Ce metal oxides loaded HZSM-5 catalysts were prepared by incipient wetness impregnation method.The results show that compared with MnOx,the tempertature of hydrogen reduction of MnOx-CeO2 shifts toward lower temperatures due to the interaction of MnOx and CeO2.It demonstrates that the mixture of the MnOx-CeO2 metal oxides possesses better oxidizability.Furthermore,the interaction of MnOx and CeO2 also increases the chemisorbed oxygen species on the surface of the catalyst,which is considered to conducive to soot combustion.Finally,by NaOH etching of HZSM-5 zeolite,the Cu/Ce metal oxides loaded catalyst?CuCe/DZ?with the mesoporous structure was prepared.Compared with the catalyst of Cu/Ce metal oxides loaded untreated HZSM-5 zeolite?CuCe/Z?,the CuCe/DZ catalyst with the mesoporous structure presents the higher catalytic activity for soot combustion.Its T50 value decreases from 401 °C to 390 °C.Because of the interaction between CuO and CeO2,the oxidation ability of the catalyst is enhanced.In addition,the catalyst with the mesoporous structure can increase the effective contact between soot and the catalyst and promote the mass transport?...
Keywords/Search Tags:Soot, Catalytic combustion, Diesel vehicles, HZSM-5 molecular sieve, Metal oxides, Synergistic effect
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