The composite oxides xAg/Co_(0.93)Ce_(0.07)(x=Ag/(Co+Ce) molar ratio),intended for use as high performance catalytic materials,were successfully prepared via citric acid complexation.The effects of silver on ...The composite oxides xAg/Co_(0.93)Ce_(0.07)(x=Ag/(Co+Ce) molar ratio),intended for use as high performance catalytic materials,were successfully prepared via citric acid complexation.The effects of silver on the performance of these substances during soot combustion were subsequently investigated.Under O_2,the 0.3Ag/Co_(0.93)Ce_(0.07) catalyst resulted in the lowest ignition temperature,T_(10),of197 ℃,while the minimum light-off temperature was obtained from both 0.2Ag/Co_(0.93)Ce_(0.07) and0.3Ag/Co_(0.93)Ce_(0.07) in the NO_x atmosphere.These materials were also characterized by various techniques,including H_2,soot and NO_x temperature programmed reduction,X-ray diffraction,and electron paramagnetic resonance,Raman,X-ray photoelectron,and Fourier transform infrared spectroscopic analyses.The results demonstrated that silver significantly alters the catalytic behavior under both O_2 and NO_x,even though the lattice structure of the mixed oxide is not affected.Surface silver oxides generated under the O_2 atmosphere favor soot combustion by participating in the redox cycles between soot and the silver oxide,whereas the AgNO_3 that forms in a NO_x-rich atmosphere facilitates soot abatement at a lower temperature.The inferior activity of AgNO_3 relative to that of Ag_2O results in the different catalytic performance in the presence of NO_x or O_2.展开更多
Co3O4 catalysts prepared with different precipitants(NH3·H2O,KOH,NH4HCO3,K2CO3 and KHCO3)were investigated for the oxidation of formaldehyde(HCHO).Among these,KHCO3-precipitated Co3O4(KHCO3-Co) was the most...Co3O4 catalysts prepared with different precipitants(NH3·H2O,KOH,NH4HCO3,K2CO3 and KHCO3)were investigated for the oxidation of formaldehyde(HCHO).Among these,KHCO3-precipitated Co3O4(KHCO3-Co) was the most active low-temperature catalyst,and was able to completely oxidize HCHO at the 100-ppm level to CO2 at 90℃.In situ diffuse reflectance infrared spectroscopy demonstrated that hydroxyl groups on the catalyst surface were regenerated by K~+ and CO3^(2-),thus promoting the oxidation of HCHO.Moreover,H2-temperature programmed reduction and X-ray photoelectron spectroscopy showed that employing KHCO3 as the precipitant increased the Co^3+/Co^2+molar ratio on the surface of the Co3O4 catalyst,thus further promoting oxidation.Structural characterization revealed that catalysts precipitated with carbonate or bicarbonate reagents exhibited greater specific surface areas and pore volumes.Overall,these data suggest that the high activity observed during the Co3O4 catalyzed oxidation of HCHO can be primarily attributed to the presence of K~+ and CO3^(2-) on the Co3O4 surface and the favorable Co^3+/Co^2+ ratio.展开更多
我们采用柠檬酸配合法制备了Ce基复合氧化物催化剂,分别在热重分析仪(TG)和管式反应器中测试了其氧化碳烟及同时脱除NOx的催化活性;并利用XRD、BET、H2-TPR、XPS表征手段考察其结构.其中,Co0.1/C e La0.05复合氧化物同时催化去除碳烟和...我们采用柠檬酸配合法制备了Ce基复合氧化物催化剂,分别在热重分析仪(TG)和管式反应器中测试了其氧化碳烟及同时脱除NOx的催化活性;并利用XRD、BET、H2-TPR、XPS表征手段考察其结构.其中,Co0.1/C e La0.05复合氧化物同时催化去除碳烟和NOx的性能最佳,碳烟脱除率为50%的反应温度为301℃,N2产率为41.4%.实验结果表明,Co主要以氧化物形式均匀分散在Ce-La固溶体表面,Co3+与Co2+价态共存,离子间的变价有利于提高催化剂的氧化还原性能,有效降低了碳烟的起燃温度.La的引入增大了催化剂的比表面积,抑制了Ce O2晶粒长大,进而提高了N2产率.部分La和Co形成了微量的La Co O3,形成了更多氧空位,有利于提高催化氧化碳烟的活性.展开更多
采用溶液燃烧法和盐助溶液燃烧法制备铜铁矿结构(ABO2)的钴酸锂(Li Co O2)系列催化剂,通过XRD、BET、ICP、XPS、H2-TPR、程序升温反应等手段对其进行了结构表征与性能评价.研究了溶液燃烧法中燃料尿素以及助剂无机盐Na Cl的用量对所制...采用溶液燃烧法和盐助溶液燃烧法制备铜铁矿结构(ABO2)的钴酸锂(Li Co O2)系列催化剂,通过XRD、BET、ICP、XPS、H2-TPR、程序升温反应等手段对其进行了结构表征与性能评价.研究了溶液燃烧法中燃料尿素以及助剂无机盐Na Cl的用量对所制备的催化剂性能影响.实验结果表明,在尿素过量100%时所制备的催化剂结晶程度及催化氧化性能较好,起燃温度达到270℃,N2的转化率达到36.9%.适量助剂Na Cl的引入显著地提高了催化剂比表面积,增加了催化剂表面活性物种,增强了催化剂的氧化还原能力,进而提升催化剂的活性.其中50%质量分数的Na Cl添加量制备的催化剂具有最低的碳烟起燃温度(246℃),但添加Na Cl对NOx的转化率影响不大.展开更多
基金supported by the National Natural Science Foundation of China(21577088)~~
文摘The composite oxides xAg/Co_(0.93)Ce_(0.07)(x=Ag/(Co+Ce) molar ratio),intended for use as high performance catalytic materials,were successfully prepared via citric acid complexation.The effects of silver on the performance of these substances during soot combustion were subsequently investigated.Under O_2,the 0.3Ag/Co_(0.93)Ce_(0.07) catalyst resulted in the lowest ignition temperature,T_(10),of197 ℃,while the minimum light-off temperature was obtained from both 0.2Ag/Co_(0.93)Ce_(0.07) and0.3Ag/Co_(0.93)Ce_(0.07) in the NO_x atmosphere.These materials were also characterized by various techniques,including H_2,soot and NO_x temperature programmed reduction,X-ray diffraction,and electron paramagnetic resonance,Raman,X-ray photoelectron,and Fourier transform infrared spectroscopic analyses.The results demonstrated that silver significantly alters the catalytic behavior under both O_2 and NO_x,even though the lattice structure of the mixed oxide is not affected.Surface silver oxides generated under the O_2 atmosphere favor soot combustion by participating in the redox cycles between soot and the silver oxide,whereas the AgNO_3 that forms in a NO_x-rich atmosphere facilitates soot abatement at a lower temperature.The inferior activity of AgNO_3 relative to that of Ag_2O results in the different catalytic performance in the presence of NO_x or O_2.
基金supported by the National Natural Science Foundation of China(21577088)~~
文摘Co3O4 catalysts prepared with different precipitants(NH3·H2O,KOH,NH4HCO3,K2CO3 and KHCO3)were investigated for the oxidation of formaldehyde(HCHO).Among these,KHCO3-precipitated Co3O4(KHCO3-Co) was the most active low-temperature catalyst,and was able to completely oxidize HCHO at the 100-ppm level to CO2 at 90℃.In situ diffuse reflectance infrared spectroscopy demonstrated that hydroxyl groups on the catalyst surface were regenerated by K~+ and CO3^(2-),thus promoting the oxidation of HCHO.Moreover,H2-temperature programmed reduction and X-ray photoelectron spectroscopy showed that employing KHCO3 as the precipitant increased the Co^3+/Co^2+molar ratio on the surface of the Co3O4 catalyst,thus further promoting oxidation.Structural characterization revealed that catalysts precipitated with carbonate or bicarbonate reagents exhibited greater specific surface areas and pore volumes.Overall,these data suggest that the high activity observed during the Co3O4 catalyzed oxidation of HCHO can be primarily attributed to the presence of K~+ and CO3^(2-) on the Co3O4 surface and the favorable Co^3+/Co^2+ ratio.
文摘我们采用柠檬酸配合法制备了Ce基复合氧化物催化剂,分别在热重分析仪(TG)和管式反应器中测试了其氧化碳烟及同时脱除NOx的催化活性;并利用XRD、BET、H2-TPR、XPS表征手段考察其结构.其中,Co0.1/C e La0.05复合氧化物同时催化去除碳烟和NOx的性能最佳,碳烟脱除率为50%的反应温度为301℃,N2产率为41.4%.实验结果表明,Co主要以氧化物形式均匀分散在Ce-La固溶体表面,Co3+与Co2+价态共存,离子间的变价有利于提高催化剂的氧化还原性能,有效降低了碳烟的起燃温度.La的引入增大了催化剂的比表面积,抑制了Ce O2晶粒长大,进而提高了N2产率.部分La和Co形成了微量的La Co O3,形成了更多氧空位,有利于提高催化氧化碳烟的活性.