A series of praseodymium added CeO2(ZrO2)/TiO2 catalysts separately prepared by methods of sol-gel and impregnation were tested for selective catalytic reduction of NO, and characterized by X-ray diffraction (XRD)...A series of praseodymium added CeO2(ZrO2)/TiO2 catalysts separately prepared by methods of sol-gel and impregnation were tested for selective catalytic reduction of NO, and characterized by X-ray diffraction (XRD), N2-brumauer-emmett-teller (N2-BET), NH3-temperature programmed desorption (NH3-TPD), H2-temperature programmed reduction (H2-TPR), PL spectra, Ra-man spectra, electron paramagnetic resonance (EPR) and X-ray photoelectron spectroscopy (XPS), respectively. Influence of prepara-tion method on catalytic performance was studied. Results showed that the influence of Pr addition on catalytic performance of the CeO2(ZrO2)/TiO2 catalysts was different between the sol-gel method and the impregnation method. The Pr addition tended to interact with TiO2 and formed the structure of Ti-O-Pr in the sol-gel method while it was more likely to interact with CeO2 forming the struc-ture of Ce-O-Pr in the impregnation method. The total acid amount and redox properties of the catalysts prepared by sol-gel method decreased with the addition of Pr element, which resulted in decrease of catalytic activity. In contrast, the Pr-added catalyst prepared by impregnation method was found to possess easier reducibility, more total acid amount and higher proportion of Ce3+ species, which was favourable for higher catalytic activity.展开更多
A series CeO2(ZrO2)/TiO2 catalysts were modified with Er using a sol-gel method.The catalytic activity of the obtained catalysts in the selective catalytic reduction(SCR) of NO with NH3 was investigated to determi...A series CeO2(ZrO2)/TiO2 catalysts were modified with Er using a sol-gel method.The catalytic activity of the obtained catalysts in the selective catalytic reduction(SCR) of NO with NH3 was investigated to determine the appropriate Er dosage.The catalysts were characterized using X-ray diffraction,N2 adsorption,NH3 temperature-programmed desorption,H2 temperature-programmed reduction,photoluminescence spectroscopy,electron paramagnetic resonance spectroscopy,and X-ray photoelectron spectroscopy.The results showed that the optimum Er/Ce molar ratio was 0.10;this catalyst had excellent resistance to catalyst poisoning caused by vapor and sulfur and gave more than 90% NO conversion at 220–395 ℃ and a gas hourly space velocity of 71 400 h^-1.Er incorporation increased the Ti^3+ concentrations,oxygen storage capacities,and oxygen vacancy concentrations of the catalysts,resulting in excellent catalytic performance.Er incorporation also decreased the acid strength and inhibited growth of TiO2 and CeO2 crystal particles,which increased the catalytic activity.The results show that high oxygen vacancy concentrations and oxygen storage capacities,large amounts of Ti^3+,and low acid strengths give excellent SCR activity.展开更多
采用共沉淀法制备了Zr0.5Ti0.5O2载体材料,将其掺杂在CeO2-Al2O3(CA)基催化剂中,并对其催化活性进行了超临界裂解测试,采用全自动吸附仪、X射线衍射(XRD)、透射电镜(TEM)、程序升温脱附(TPD)等方法对催化剂进行了表征.实验结果表明,催...采用共沉淀法制备了Zr0.5Ti0.5O2载体材料,将其掺杂在CeO2-Al2O3(CA)基催化剂中,并对其催化活性进行了超临界裂解测试,采用全自动吸附仪、X射线衍射(XRD)、透射电镜(TEM)、程序升温脱附(TPD)等方法对催化剂进行了表征.实验结果表明,催化剂能够明显降低裂解反应的温度,600°C CA基催化剂产气率是热裂解的2.8倍,掺杂Zr0.5Ti0.5O2载体材料的CA基催化剂是热裂解的4.0倍,650°C时,掺杂Zr0.5Ti0.5O2载体材料的CA基催化剂热沉提高了0.55 MJ kg 1.BET结果表明,掺杂Zr0.5Ti0.5O2载体后催化剂出现双孔结构,部分小孔的出现使得乙烯的选择性提高;NH3-TPD结果表明,掺杂Zr0.5Ti0.5O2载体材料后,催化剂强酸位的酸量增加了4.0倍,催化剂表现出更强的表面酸性和更集中的强酸酸中心密度,有利于裂解多产烯烃.展开更多
基金supported by National Key Research and Development Program of China(2016YFC0205500)National Natural Science Foundation of China(51272105)+1 种基金Jiangsu Provincial Science and Technology Supporting Program(BE2013718)the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)
摘要A series of praseodymium added CeO2(ZrO2)/TiO2 catalysts separately prepared by methods of sol-gel and impregnation were tested for selective catalytic reduction of NO, and characterized by X-ray diffraction (XRD), N2-brumauer-emmett-teller (N2-BET), NH3-temperature programmed desorption (NH3-TPD), H2-temperature programmed reduction (H2-TPR), PL spectra, Ra-man spectra, electron paramagnetic resonance (EPR) and X-ray photoelectron spectroscopy (XPS), respectively. Influence of prepara-tion method on catalytic performance was studied. Results showed that the influence of Pr addition on catalytic performance of the CeO2(ZrO2)/TiO2 catalysts was different between the sol-gel method and the impregnation method. The Pr addition tended to interact with TiO2 and formed the structure of Ti-O-Pr in the sol-gel method while it was more likely to interact with CeO2 forming the struc-ture of Ce-O-Pr in the impregnation method. The total acid amount and redox properties of the catalysts prepared by sol-gel method decreased with the addition of Pr element, which resulted in decrease of catalytic activity. In contrast, the Pr-added catalyst prepared by impregnation method was found to possess easier reducibility, more total acid amount and higher proportion of Ce3+ species, which was favourable for higher catalytic activity.
基金supported by the National Natural Science Foundation of China(51272105)Jiangsu Provincial Science and Technology Supporting Program(BE2013718)+1 种基金Research Subject of Environmental Protection Department of Jiangsu Province of China(2013006)Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)~~
摘要A series CeO2(ZrO2)/TiO2 catalysts were modified with Er using a sol-gel method.The catalytic activity of the obtained catalysts in the selective catalytic reduction(SCR) of NO with NH3 was investigated to determine the appropriate Er dosage.The catalysts were characterized using X-ray diffraction,N2 adsorption,NH3 temperature-programmed desorption,H2 temperature-programmed reduction,photoluminescence spectroscopy,electron paramagnetic resonance spectroscopy,and X-ray photoelectron spectroscopy.The results showed that the optimum Er/Ce molar ratio was 0.10;this catalyst had excellent resistance to catalyst poisoning caused by vapor and sulfur and gave more than 90% NO conversion at 220–395 ℃ and a gas hourly space velocity of 71 400 h^-1.Er incorporation increased the Ti^3+ concentrations,oxygen storage capacities,and oxygen vacancy concentrations of the catalysts,resulting in excellent catalytic performance.Er incorporation also decreased the acid strength and inhibited growth of TiO2 and CeO2 crystal particles,which increased the catalytic activity.The results show that high oxygen vacancy concentrations and oxygen storage capacities,large amounts of Ti^3+,and low acid strengths give excellent SCR activity.
摘要采用共沉淀法制备了Zr0.5Ti0.5O2载体材料,将其掺杂在CeO2-Al2O3(CA)基催化剂中,并对其催化活性进行了超临界裂解测试,采用全自动吸附仪、X射线衍射(XRD)、透射电镜(TEM)、程序升温脱附(TPD)等方法对催化剂进行了表征.实验结果表明,催化剂能够明显降低裂解反应的温度,600°C CA基催化剂产气率是热裂解的2.8倍,掺杂Zr0.5Ti0.5O2载体材料的CA基催化剂是热裂解的4.0倍,650°C时,掺杂Zr0.5Ti0.5O2载体材料的CA基催化剂热沉提高了0.55 MJ kg 1.BET结果表明,掺杂Zr0.5Ti0.5O2载体后催化剂出现双孔结构,部分小孔的出现使得乙烯的选择性提高;NH3-TPD结果表明,掺杂Zr0.5Ti0.5O2载体材料后,催化剂强酸位的酸量增加了4.0倍,催化剂表现出更强的表面酸性和更集中的强酸酸中心密度,有利于裂解多产烯烃.