Orderly mesoporous CuFe2O4spinel-type mixed oxide with high specific surface area was prepared successfully by a hard-template method in which KIT-6mesoporous silica was selected as the hard template.The KIT-6 hard te...Orderly mesoporous CuFe2O4spinel-type mixed oxide with high specific surface area was prepared successfully by a hard-template method in which KIT-6mesoporous silica was selected as the hard template.The KIT-6 hard template and CuFe2O4samples were characterized by X-ray diffraction,X-ray photoelectron spectroscopy,X-ray fluorescence,transmission electron microscopy,scanning electron microscopy,nitrogen physisorption,and hydrogen-temperature programmed reduction.The KIT-6 hard template had perfect crystallization and ordered mesoporous structure with a probable pore distribution of about 9.1 nm,large enough to be filled by the spinel precursor.The mesoporous CuFe2O4spinel oxide synthesized inside the KIT-6 mesopores had a relatively small pore size(4.3 nm),orderly arrangement,and high specific area(194 m2/g).The catalytic activity of the mesoporous CuFe2O4was tested for the selective oxidation of ammonia to nitrogen.The conversion of ammonia reached nearly 100%at 300°C with a nitrogen selectivity as high as 96%.The nitrogen selectivity remained high with increasing temperature and even maintained a value of80%at 600°C.展开更多
Chromium oxide and manganese oxide promoted ZrO2-CeO2 catalysts were prepared by a homogeneous precipitation method for the selective catalytic reduction of NOx with NH3. A series of characterization including X-ray d...Chromium oxide and manganese oxide promoted ZrO2-CeO2 catalysts were prepared by a homogeneous precipitation method for the selective catalytic reduction of NOx with NH3. A series of characterization including X-ray diffraction （XRD）, high-resolution transmission electron microscope （HR-TEM）, Bmnaue-Emmett-Teller （BET） surface area analysis, H2 temperature- programmed reduction （H2-TPR）, and X-ray photoelectron spectroscopy （XPS） were used to evaluate the influence of the physicochemical properties on NH3-SCR activity. Cr-Zr-Ce and Mn-Zr-Ce catalysts are much more active than ZrO2-CeO2 binary oxide for the low temperature NH3-SCR, mainly because of the high specific surface area, more surface oxygen species, improved reducibility derived from synergistic effect among different elements. Mn-Zr-Ce catalyst exhibited high tolerance to SO2 and H2O. Cr-Zr-Ce mixed oxide exhibited〉80% NO,. conversion at a wide temperature window of 100 ℃ 300℃. In situ DRIFT studies showed that the addition of Cr is beneficial to the formation of Bronsted acid sites and prevents the formation of stable nitrate species because of the presence ofCr6 ＋. The present mixed oxide can be a candidate for the low temperature abatement of NOx.展开更多
Sulfate adsorption is one of the factors that cause the poisoning of catalyst in the low-temperature NH_(3) selective catalytic reduction reaction(NH_(3)-SCR).In this paper,by controlling the co-adsorption time of SO_...Sulfate adsorption is one of the factors that cause the poisoning of catalyst in the low-temperature NH_(3) selective catalytic reduction reaction(NH_(3)-SCR).In this paper,by controlling the co-adsorption time of SO_(2) and O_(2) at 150℃,a range of sulfated MnCeOx catalysts with different contents of metal sulfate species were prepared to reveal the influence of metal sulfate species content on the catalytic performances and reaction mechanisms at low temperature.The catalytic activity below 250℃rapidly decreases with increasing metal sulfate species content.The results of characterizations shed light on the reduction of specific surface area,Mn^(4+)and Ce^(3+)content,and redox ability of MnCeOx owing to the formation of metal sulfate species.Further experiments reveal that metal sulfate species preferentially absorb on MnOx domains rather than on CeO_(2) domains,and the adsorbed metal sulfate species can suppress the Eley-Rideal and the Langmuir-Hinshelwood reaction mechanisms over the sulfated MnCeOx.All the above results are detrimental to the activity of sulfated MnCeOx in the low-temperature NH3-SCR reaction.展开更多
The sulfated CeO_(2)/Al_(2)O_(3) catalysts with different sizes of CeO_(2)nanoparticles were prepared by using pure H_2O or acetic acid solution as impregnation solvent, and the influence of sizes of CeO_(2) nanoparti...The sulfated CeO_(2)/Al_(2)O_(3) catalysts with different sizes of CeO_(2)nanoparticles were prepared by using pure H_2O or acetic acid solution as impregnation solvent, and the influence of sizes of CeO_(2) nanoparticles on the catalytic performances of the sulfated CeO_(2)/Al_(2)O_(3) catalyst was studied. The catalytic performance tests show that the sulfated CeO_(2)/Al_(2)O_(3) catalyst using acetic acid solution as impregnation solvent has better catalytic activity and the resistance to K+poisoning than the sulfated CeO_(2)/Al_(2)O_(3) catalyst using pure H_(2)O as impregnation solvent. The excellent catalytic performances can be ascribed to the smaller sizes of CeO_(2) nanoparticles in CeO_(2)/Al_(2)O_(3) catalyst using acetic acid solution, which results in larger amount of adsorbed sulfate species, surface acid sites, surface active oxygen species and excellent redox property. These features are helpful for improving the catalytic performances of sulfated CeO_(2)/Al_(2)O_(3) catalyst using smaller amount of CeO_(2) to cut the costs.展开更多
基金supported by the National High Technology Research and Development Program of China (2013AA065900)the National Natural Science Foundation of China (21177008,21121064)
文摘Orderly mesoporous CuFe2O4spinel-type mixed oxide with high specific surface area was prepared successfully by a hard-template method in which KIT-6mesoporous silica was selected as the hard template.The KIT-6 hard template and CuFe2O4samples were characterized by X-ray diffraction,X-ray photoelectron spectroscopy,X-ray fluorescence,transmission electron microscopy,scanning electron microscopy,nitrogen physisorption,and hydrogen-temperature programmed reduction.The KIT-6 hard template had perfect crystallization and ordered mesoporous structure with a probable pore distribution of about 9.1 nm,large enough to be filled by the spinel precursor.The mesoporous CuFe2O4spinel oxide synthesized inside the KIT-6 mesopores had a relatively small pore size(4.3 nm),orderly arrangement,and high specific area(194 m2/g).The catalytic activity of the mesoporous CuFe2O4was tested for the selective oxidation of ammonia to nitrogen.The conversion of ammonia reached nearly 100%at 300°C with a nitrogen selectivity as high as 96%.The nitrogen selectivity remained high with increasing temperature and even maintained a value of80%at 600°C.
文摘Chromium oxide and manganese oxide promoted ZrO2-CeO2 catalysts were prepared by a homogeneous precipitation method for the selective catalytic reduction of NOx with NH3. A series of characterization including X-ray diffraction （XRD）, high-resolution transmission electron microscope （HR-TEM）, Bmnaue-Emmett-Teller （BET） surface area analysis, H2 temperature- programmed reduction （H2-TPR）, and X-ray photoelectron spectroscopy （XPS） were used to evaluate the influence of the physicochemical properties on NH3-SCR activity. Cr-Zr-Ce and Mn-Zr-Ce catalysts are much more active than ZrO2-CeO2 binary oxide for the low temperature NH3-SCR, mainly because of the high specific surface area, more surface oxygen species, improved reducibility derived from synergistic effect among different elements. Mn-Zr-Ce catalyst exhibited high tolerance to SO2 and H2O. Cr-Zr-Ce mixed oxide exhibited〉80% NO,. conversion at a wide temperature window of 100 ℃ 300℃. In situ DRIFT studies showed that the addition of Cr is beneficial to the formation of Bronsted acid sites and prevents the formation of stable nitrate species because of the presence ofCr6 ＋. The present mixed oxide can be a candidate for the low temperature abatement of NOx.
基金Project supported by the National Natural Science Foundation of China(21607019)the Scientific andTechnological Research Program of Chongqing Municipal Education Commission(KJQN202101242,KJQN202001227)+2 种基金the Science andTechnology Project of Wanzhou(wzstc-2019034)the Open Project Program of Key Laboratory of Water Environment Evolution andPollution Control in the Three Gorges Reservoir(WEPKL2019ZD-04)the Project Program of Chongqing Postgraduate Research andInnovation(CYS21489)。
文摘Sulfate adsorption is one of the factors that cause the poisoning of catalyst in the low-temperature NH_(3) selective catalytic reduction reaction(NH_(3)-SCR).In this paper,by controlling the co-adsorption time of SO_(2) and O_(2) at 150℃,a range of sulfated MnCeOx catalysts with different contents of metal sulfate species were prepared to reveal the influence of metal sulfate species content on the catalytic performances and reaction mechanisms at low temperature.The catalytic activity below 250℃rapidly decreases with increasing metal sulfate species content.The results of characterizations shed light on the reduction of specific surface area,Mn^(4+)and Ce^(3+)content,and redox ability of MnCeOx owing to the formation of metal sulfate species.Further experiments reveal that metal sulfate species preferentially absorb on MnOx domains rather than on CeO_(2) domains,and the adsorbed metal sulfate species can suppress the Eley-Rideal and the Langmuir-Hinshelwood reaction mechanisms over the sulfated MnCeOx.All the above results are detrimental to the activity of sulfated MnCeOx in the low-temperature NH3-SCR reaction.
基金Project supported by the National Natural Science Foundation of China(21607019)the Scientific and Technological Research Program of Chongqing Municipal Education Commission(KJQN202101242,KJQN202001227)the Open Project Program of Key Laboratory of Water Environment Evolution and Pollution Control in the Three Gorges Reservoir(WEPKL2019ZD-04)。
文摘The sulfated CeO_(2)/Al_(2)O_(3) catalysts with different sizes of CeO_(2)nanoparticles were prepared by using pure H_2O or acetic acid solution as impregnation solvent, and the influence of sizes of CeO_(2) nanoparticles on the catalytic performances of the sulfated CeO_(2)/Al_(2)O_(3) catalyst was studied. The catalytic performance tests show that the sulfated CeO_(2)/Al_(2)O_(3) catalyst using acetic acid solution as impregnation solvent has better catalytic activity and the resistance to K+poisoning than the sulfated CeO_(2)/Al_(2)O_(3) catalyst using pure H_(2)O as impregnation solvent. The excellent catalytic performances can be ascribed to the smaller sizes of CeO_(2) nanoparticles in CeO_(2)/Al_(2)O_(3) catalyst using acetic acid solution, which results in larger amount of adsorbed sulfate species, surface acid sites, surface active oxygen species and excellent redox property. These features are helpful for improving the catalytic performances of sulfated CeO_(2)/Al_(2)O_(3) catalyst using smaller amount of CeO_(2) to cut the costs.
