A series of PdCu bimetallic catalysts with low Cu and Pd loadings and different Cu:Pd atomic ratios were prepared by conventionally sequential impregnation(CSD)and modified sequential impregnation(MSI)of Cu and Pd for...A series of PdCu bimetallic catalysts with low Cu and Pd loadings and different Cu:Pd atomic ratios were prepared by conventionally sequential impregnation(CSD)and modified sequential impregnation(MSI)of Cu and Pd for selective hydrogenation of acetylene.Characterization indicates that the supported copper(I)nitrate in the PdCu bimetallic catalysts prepared by MSI can be directly reduced to Cu metal particles due to the hydrogen spillover from Pd to Cu(NO3)2 crystals.In addition,for the catalysts prepared by MSI,Pd atoms can form PdCu alloy on the surface of metal particles,however,for the catalysts prepared by CSI,Pd tends to migrate and exist below the surface layer of Cu.Reaction results indicate that compared with CSI,the MSI method enables samples to possess preferable stability as well as comparable reaction activity.This should be due to the MSI method in favor of the formation of PdCu alloy on the surface of metal particles.Moreover,even Pd loading is super low,<0.045 wt-%in this study,by through adjusting Cu loading to an appropriate value,attractive reactivity and selectivity still can be achieved.展开更多
Five hundred ppm Pd/CeO2 catalyst was prepared and evaluated in selective hydrogenation of acetylene in large excess of ethylene since ceria has been recently found to be a reasonable stand-alone catalyst for this rea...Five hundred ppm Pd/CeO2 catalyst was prepared and evaluated in selective hydrogenation of acetylene in large excess of ethylene since ceria has been recently found to be a reasonable stand-alone catalyst for this reaction.Pd/CeO2 catalyst could be activated in situ by the feed gas during reactions and the catalyst without reduction showed much better ethylene selectivity than the reduced one in the high temperature range due to the formation of oxygen vacancies by reduction.Excellent ethylene selectivity of〜100%was obtained in the whole reaction temperature range of 50℃-200℃ for samples calcined at temperatures of 600℃ and 800℃.This could be ascribed to the formation of PdX-Ce1-xO2-y or Pd-O-Ce surface species based on the X-ray diffiaction and X-ray photoelectron spectroscopy results,indicating the strong interaction between palladium and ceria.展开更多
基金support of the National Natural Science Foundation of China(Grant No.1263094)Welch Foundation(No.T-0014)+1 种基金Key Scientific and Technological Projcct of Henan province,China(No.182102410072)Shanxi International Cooperation Project(No.201703D421037)。
文摘A series of PdCu bimetallic catalysts with low Cu and Pd loadings and different Cu:Pd atomic ratios were prepared by conventionally sequential impregnation(CSD)and modified sequential impregnation(MSI)of Cu and Pd for selective hydrogenation of acetylene.Characterization indicates that the supported copper(I)nitrate in the PdCu bimetallic catalysts prepared by MSI can be directly reduced to Cu metal particles due to the hydrogen spillover from Pd to Cu(NO3)2 crystals.In addition,for the catalysts prepared by MSI,Pd atoms can form PdCu alloy on the surface of metal particles,however,for the catalysts prepared by CSI,Pd tends to migrate and exist below the surface layer of Cu.Reaction results indicate that compared with CSI,the MSI method enables samples to possess preferable stability as well as comparable reaction activity.This should be due to the MSI method in favor of the formation of PdCu alloy on the surface of metal particles.Moreover,even Pd loading is super low,<0.045 wt-%in this study,by through adjusting Cu loading to an appropriate value,attractive reactivity and selectivity still can be achieved.
基金Welch Foundation(#T-0014)and the CNMS user program of the Oak Ridge National LaboratoryAcknowledgment is made to the Donors of the American Chemical Society Petroleum Research Fund for partial support of this research,ACS PRF(#57596-UR5).
文摘Five hundred ppm Pd/CeO2 catalyst was prepared and evaluated in selective hydrogenation of acetylene in large excess of ethylene since ceria has been recently found to be a reasonable stand-alone catalyst for this reaction.Pd/CeO2 catalyst could be activated in situ by the feed gas during reactions and the catalyst without reduction showed much better ethylene selectivity than the reduced one in the high temperature range due to the formation of oxygen vacancies by reduction.Excellent ethylene selectivity of〜100%was obtained in the whole reaction temperature range of 50℃-200℃ for samples calcined at temperatures of 600℃ and 800℃.This could be ascribed to the formation of PdX-Ce1-xO2-y or Pd-O-Ce surface species based on the X-ray diffiaction and X-ray photoelectron spectroscopy results,indicating the strong interaction between palladium and ceria.
