A series of three‐dimensionally ordered macroporous(3DOM)SnO2‐based catalysts modified by the cations Ce4+,Mn3+,and Cu2+have been prepared by using a colloidal crystal templating method and tested for soot combustio...A series of three‐dimensionally ordered macroporous(3DOM)SnO2‐based catalysts modified by the cations Ce4+,Mn3+,and Cu2+have been prepared by using a colloidal crystal templating method and tested for soot combustion under loose contact condition.XRD and STEM mapping results confirm that all the secondary metal cations have entered the lattice matrix of tetragonal rutile SnO2 to form non‐continuous solid solutions,thus impeding crystallization and improving the surface areas and pore volumes of the modified catalysts.In comparison with regular SnO2 nanoparticles,the 3DOM SnO2 displays evidently improved activity,testifying that the formation of the 3DOM structure can anchor the soot particulates in the macro‐pores,which ensures that the contact of the soot particles with the active sites on the 3DOM skeleton is more easily formed,thus benefiting the target reaction.With the incorporation of the secondary metal cations,the activity of the catalyst can be further improved due to the formation of more abundant mobile oxygen species.In summary,these effects are believed to be the major factors responsible for the activity of the catalyst.展开更多
To understand the effect of the doping amount of Cu^2+ on the structure and reactivity of SnO2 in NOx-SCR with NH3, a series of Sn-Cu-O binary oxide catalysts with different Sn/Cu ratios have been prepared and thoroug...To understand the effect of the doping amount of Cu^2+ on the structure and reactivity of SnO2 in NOx-SCR with NH3, a series of Sn-Cu-O binary oxide catalysts with different Sn/Cu ratios have been prepared and thoroughly characterized. Using the XRD extrapolation method, the SnO2 lattice capacity for Cu^2+ cations is determined at 0.10 g Cu O per g of SnO2, equaling a Sn/Cu molar ratio of 84/16. Therefore, in a tetragonal rutile SnO2 lattice, only a maximum of 16% of the Sn4+ cations can be replaced by Cu^2+ to form a stable solid solution structure. If the Cu content is higher, Cu O will form on the catalyst surface, which has a negative effect on the reaction performance. For samples in a pure solid solution phase, the number of surface defects increase with increasing Cu content until it reaches the lattice capacity, as confirmed by Raman spectroscopy. As a result, the amounts of both active oxygen species and acidic sites on the surface, which critically determine the reaction performance, also increase and reach the maximum level for the catalyst with a Cu content close to the lattice capacity. A distinct lattice capacity threshold effect on the structure and reactivity of Sn-Cu binary oxide catalysts has been observed. A Sn-Cu catalyst with the best reaction performance can be obtained by doping the SnO2 matrix with the lattice capacity amount of Cu^2+.展开更多
基金the Natural Science Foundation of China(21567016,21503106)the Natural Science Foundation of Jiangxi Province(20171BAB213013)+3 种基金the Education Department Foundation of Jiangxi Province(KJLD14005)National Key Research and Development Program of China(2016YFC0209302)the Innovation Fund Designated for Graduate Students of Jiangxi Province(YC2015-B017)the Innovation Fund Designated for Undergraduate Students of China(201701035)~~
文摘A series of three‐dimensionally ordered macroporous(3DOM)SnO2‐based catalysts modified by the cations Ce4+,Mn3+,and Cu2+have been prepared by using a colloidal crystal templating method and tested for soot combustion under loose contact condition.XRD and STEM mapping results confirm that all the secondary metal cations have entered the lattice matrix of tetragonal rutile SnO2 to form non‐continuous solid solutions,thus impeding crystallization and improving the surface areas and pore volumes of the modified catalysts.In comparison with regular SnO2 nanoparticles,the 3DOM SnO2 displays evidently improved activity,testifying that the formation of the 3DOM structure can anchor the soot particulates in the macro‐pores,which ensures that the contact of the soot particles with the active sites on the 3DOM skeleton is more easily formed,thus benefiting the target reaction.With the incorporation of the secondary metal cations,the activity of the catalyst can be further improved due to the formation of more abundant mobile oxygen species.In summary,these effects are believed to be the major factors responsible for the activity of the catalyst.
文摘To understand the effect of the doping amount of Cu^2+ on the structure and reactivity of SnO2 in NOx-SCR with NH3, a series of Sn-Cu-O binary oxide catalysts with different Sn/Cu ratios have been prepared and thoroughly characterized. Using the XRD extrapolation method, the SnO2 lattice capacity for Cu^2+ cations is determined at 0.10 g Cu O per g of SnO2, equaling a Sn/Cu molar ratio of 84/16. Therefore, in a tetragonal rutile SnO2 lattice, only a maximum of 16% of the Sn4+ cations can be replaced by Cu^2+ to form a stable solid solution structure. If the Cu content is higher, Cu O will form on the catalyst surface, which has a negative effect on the reaction performance. For samples in a pure solid solution phase, the number of surface defects increase with increasing Cu content until it reaches the lattice capacity, as confirmed by Raman spectroscopy. As a result, the amounts of both active oxygen species and acidic sites on the surface, which critically determine the reaction performance, also increase and reach the maximum level for the catalyst with a Cu content close to the lattice capacity. A distinct lattice capacity threshold effect on the structure and reactivity of Sn-Cu binary oxide catalysts has been observed. A Sn-Cu catalyst with the best reaction performance can be obtained by doping the SnO2 matrix with the lattice capacity amount of Cu^2+.
