The aging process of pure copper precursors and copper-zinc binary precursorswere studied by XRD, TG-DTG and TPR techniques. The catalytic activity and stability of CuO/ZnOwere tested using fixed-bed flow reactor, and...The aging process of pure copper precursors and copper-zinc binary precursorswere studied by XRD, TG-DTG and TPR techniques. The catalytic activity and stability of CuO/ZnOwere tested using fixed-bed flow reactor, and the physical properties of the catalysts and Cuspecies were characterized with N_2 adsorption and N_2O passivation method, respectively. For theCu-Zn binary system prepared at the precipitating condition of pH=8.0 and temperature=80℃, theinitial phase was a mixture of copper nitrate hydroxide Cu_2(NO_3)(OH)_3, georgeite and hydrozinciteZn_5(CO_3)_2(OH)_6. By increasing the duration of its aging time, the phase of Cu_2(NO_3)(OH)_2first transited to georgeite, and then interdiffused into Zn_5(CO_3)_2(OH)_6 and resulted in two newphases: rosasite (Cu,Zn)_2CO_3(OH)_2 and au-richalcite (Zn,Cu)_5(CO_3)_2(OH)_6. The former phasewas much easier to be formed than the latter one, while the latter phase was more responsible forthe activity of methanol synthesis than the former one. It is found that the composition andstructure of the precursors altered obviously after the colour transition point. The experimentalresults showed that methanol synthesis is a structure-sensitive catalytic reaction.展开更多
MnO_x/Al_2O_3 and MnO_x/ZrO_2-Al_2O_3 catalysts were prepared by incipientwetness impregnation of Mn(CH_3COO)_2 on the corresponding supports, followed by thecharacterization using X-ray diffraction (XRD), temperature...MnO_x/Al_2O_3 and MnO_x/ZrO_2-Al_2O_3 catalysts were prepared by incipientwetness impregnation of Mn(CH_3COO)_2 on the corresponding supports, followed by thecharacterization using X-ray diffraction (XRD), temperature programmed reduction (TPR) and BETsurface area techniques. The result shows the BET surface area of ZrO_2-Al_2O_3 is lower than thatof Al_2O_3 due to the loading of ZrO_2. However the resulted MnO_x/ZrO_2-Al_2O_3 catalyst exhibitshigher activity for methane combustion than MnO_x/Al_2O_3, because the addition of ZrO_2 ontoAl_2O_3 is beneficial for the dispersion of Mn species and the improvement of the lattice oxygenactivity in MnO_x, subsequently the activation of methane during combustion. The optimum loading ofZr in MnO_x/ZrO_2-Al_2O_3 is in the range of 5%-10% correlated with the calcination temperatures ofcatalyst supports.展开更多
A natural montmorillonite, produced from Laiyang of Shandong Province, was pillared by Tipolyeations to form Ti-pillared clay (Ti-PILC), and characterized by BET surface area, infrared spectra and thermal analysis. Th...A natural montmorillonite, produced from Laiyang of Shandong Province, was pillared by Tipolyeations to form Ti-pillared clay (Ti-PILC), and characterized by BET surface area, infrared spectra and thermal analysis. The characterization results show that Ti-PILC has a larger surface area and more hydroxyl groups than that of the natural clay, thus was used as the catalytic carriers to prepare supported Cu catalysts (Cu/Ti-PILC). The 20%Cu/Ti-PILC with 10mmol/g of Ti/clay shows a high catalytic performance of methane combustion in the temperature range of 400 500℃.展开更多
文摘The aging process of pure copper precursors and copper-zinc binary precursorswere studied by XRD, TG-DTG and TPR techniques. The catalytic activity and stability of CuO/ZnOwere tested using fixed-bed flow reactor, and the physical properties of the catalysts and Cuspecies were characterized with N_2 adsorption and N_2O passivation method, respectively. For theCu-Zn binary system prepared at the precipitating condition of pH=8.0 and temperature=80℃, theinitial phase was a mixture of copper nitrate hydroxide Cu_2(NO_3)(OH)_3, georgeite and hydrozinciteZn_5(CO_3)_2(OH)_6. By increasing the duration of its aging time, the phase of Cu_2(NO_3)(OH)_2first transited to georgeite, and then interdiffused into Zn_5(CO_3)_2(OH)_6 and resulted in two newphases: rosasite (Cu,Zn)_2CO_3(OH)_2 and au-richalcite (Zn,Cu)_5(CO_3)_2(OH)_6. The former phasewas much easier to be formed than the latter one, while the latter phase was more responsible forthe activity of methanol synthesis than the former one. It is found that the composition andstructure of the precursors altered obviously after the colour transition point. The experimentalresults showed that methanol synthesis is a structure-sensitive catalytic reaction.
基金This work was financially supported by Shandong Provincial Department of Science and Technology(project number:981206403)and the State Key Laboratory of Coal Conversion at Institute of Coal Chemistry of CAS(2002-2003)
文摘MnO_x/Al_2O_3 and MnO_x/ZrO_2-Al_2O_3 catalysts were prepared by incipientwetness impregnation of Mn(CH_3COO)_2 on the corresponding supports, followed by thecharacterization using X-ray diffraction (XRD), temperature programmed reduction (TPR) and BETsurface area techniques. The result shows the BET surface area of ZrO_2-Al_2O_3 is lower than thatof Al_2O_3 due to the loading of ZrO_2. However the resulted MnO_x/ZrO_2-Al_2O_3 catalyst exhibitshigher activity for methane combustion than MnO_x/Al_2O_3, because the addition of ZrO_2 ontoAl_2O_3 is beneficial for the dispersion of Mn species and the improvement of the lattice oxygenactivity in MnO_x, subsequently the activation of methane during combustion. The optimum loading ofZr in MnO_x/ZrO_2-Al_2O_3 is in the range of 5%-10% correlated with the calcination temperatures ofcatalyst supports.
基金This work was financially supported by the Scientific Research Found ationfor the Returned Overseas Chinese Scholars,State Education Ministry(2004-527)and the StateKey Laboratory of Coal Conversion at Institute of Coal Chemistry of CAS(04-603).
文摘A natural montmorillonite, produced from Laiyang of Shandong Province, was pillared by Tipolyeations to form Ti-pillared clay (Ti-PILC), and characterized by BET surface area, infrared spectra and thermal analysis. The characterization results show that Ti-PILC has a larger surface area and more hydroxyl groups than that of the natural clay, thus was used as the catalytic carriers to prepare supported Cu catalysts (Cu/Ti-PILC). The 20%Cu/Ti-PILC with 10mmol/g of Ti/clay shows a high catalytic performance of methane combustion in the temperature range of 400 500℃.
