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《Acta Physico-chimica Sinica》 1993-03
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DISPERSION STATE OF FERRIC OXIDE ON ZrO_2 AND ITS INFLUENCE ON THE CATALYTIC PERFORMANCE

Ji Weijie Shen Shikong Li Shuben Wang Hongli (State Key Laboratory of Oxo-Synthesis and Selective Oxidation,Lanzhou Institute of Chemical Physics,Chinese Academic of Sciences,Lanzhou 730000)  
Three methods,dipping of support into an excess of aqueous solution of(NH_4)_3[Fe(C_2O_4)_3].xH_2O,incipient wetness impregnation of Fe(NO_3)_3 solution and batchadsorption of Fe(AcAc)_3 in toluene were adopted to prepare supported ferric oxide onZrO_2.Extensive characterization has been done on the physico-chemical properties ofthe system.The results indicated that monolayer dispersion of the supported componentcan be realized using the dipping and adsorption methods.It is difficult to obtain afull coverage of FeO_x on ZrO_2.In order to get monolayer dispersion,it is import-ment that the adsorbed particles should be fully washed with pure toluene in adsorp-tion method or the remained solution on the support particles should be carefullyremoved in dipping method.The monolayer FeO_x,espically the “quasi-isolated” Fe——O polyhedrons are difficultly detected by FTIR-DRS,LRS as well as XRD.TEM andHEED techniques were adopted to further comfirm the observation.The monolayerdispersed Fe~(3+) is at high spin state and located in a site with distorted rhombicsymmetry.The monolayer FeO_x on ZrO_2 is easily reduced to ferrous state as comparedwith the unsupported bulk ferric oxide or even those monolayer FeO_x species onTiO_2(A)and γ-Al_2O_3.However,further reduction of ferrous ion is still difficult. The microcrystal of ferric oxide on ZrO_2 is reduced through an intermediate compoundduring the reduction process.The results of pulse reaction of 2-C_4H_8 with or withoutgas oxygen showed that even the monolayer “quasi-isolated” polyhedrons are stilleffective to catalyse the ODH of the reactant.Different from the bulk ferric oxide,the monolayer catalysts are sensitive to the presence of gas oxygen for the formationof surface residues and CO_(x).In addition,the monolayer FeO_x species are not activefor the methanation reaction.
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