The performance of catalysts used in after-treatment systems is the key factor for the removal of diesel soot,which is an important component of atmosphericfine particle emissions.Herein,three-dimensionally ordered ma...The performance of catalysts used in after-treatment systems is the key factor for the removal of diesel soot,which is an important component of atmosphericfine particle emissions.Herein,three-dimensionally ordered macroporous–mesoporous Ti_(x)Si+(1-x)O_(2)(3DOM-m Ti_(x)Si+(1-x)O_(2)) and its supported MnO_(x)catalysts doped with different alkali/alkaline-earth metals (AMnO_(x)/3 DOM-m Ti_(0.7)Si_(0.3)O_(2)(A:Li,Na,K,Ru,Cs,Mg,Ca,Sr,Ba)) were prepared by mesoporous template (P123)-assisted colloidal crystal template (CCT) and incipient wetness impregnation methods,respectively.Physicochemical characterizations of the catalysts were performed using scanning electron microscopy,X-ray diffraction,N_(2)adsorption–desorption,H_(2)temperature-programmed reduction,O_(2)temperature-programmed desorption,NO temperature-programmed oxidation,and Raman spectroscopy techniques;then,we evaluated their catalytic performances for the removal of diesel soot particles.The results show that the 3DOM-m Ti_(0.7)Si_(0.3)O_(2)supports exhibited a well-defined 3DOM-m nanostructure,and AMnO_(x)nanoparticles with 10–50 nm were evenly dispersed on the inner walls of the uniform macropores.In addition,the as-prepared catalysts exhibited good catalytic performance for soot combustion.Among the prepared catalysts,CsMnO_(x)/3DOM-m Ti_(0.7)Si_(0.3)O_(2)had the highest catalytic activity for soot combustion,with T10,T50,and T90(the temperatures corresponding to soot conversion rates of 10%,50%,and 90%) values of 285,355,and 393℃,respectively.The high catalytic activity of the CsMnO_(x)/3 DOM-m Ti_(0.7)Si_(0.3)O_(2)catalysts was attributed to their excellent low-temperature reducibility and homogeneous macroporous–mesoporous structure,as well as to the synergistic effects between Cs and Mn species and between CsMnO_(x)and the Ti_(0.7)Si_(0.3)O_(2)support.展开更多
基金supported by Key Research and Development Program of Ministry of Science and Technology of the People’s Republic of China (MOST) (No. 2017YFE0131200) for collaboration between China and PolandNational Nature Science Foundation of China (NSFC) (Nos. 22072095, U1908204, 21761162016)+3 种基金General Projects of Liaoning Province Natural Fund (No. 2019-MS-284)National Engineering Laboratory for Mobile Source Emission Control Technology (No. NELMS2018A04)University level innovation team of Shenyang Normal University, Major Incubation Program of Shenyang Normal University (No. ZD201901)supported by the Research Grants Council (RGC) of Hong Kong through NSFC/RGC Joint Research Scheme (No. N_CUHK451/17)。
文摘The performance of catalysts used in after-treatment systems is the key factor for the removal of diesel soot,which is an important component of atmosphericfine particle emissions.Herein,three-dimensionally ordered macroporous–mesoporous Ti_(x)Si+(1-x)O_(2)(3DOM-m Ti_(x)Si+(1-x)O_(2)) and its supported MnO_(x)catalysts doped with different alkali/alkaline-earth metals (AMnO_(x)/3 DOM-m Ti_(0.7)Si_(0.3)O_(2)(A:Li,Na,K,Ru,Cs,Mg,Ca,Sr,Ba)) were prepared by mesoporous template (P123)-assisted colloidal crystal template (CCT) and incipient wetness impregnation methods,respectively.Physicochemical characterizations of the catalysts were performed using scanning electron microscopy,X-ray diffraction,N_(2)adsorption–desorption,H_(2)temperature-programmed reduction,O_(2)temperature-programmed desorption,NO temperature-programmed oxidation,and Raman spectroscopy techniques;then,we evaluated their catalytic performances for the removal of diesel soot particles.The results show that the 3DOM-m Ti_(0.7)Si_(0.3)O_(2)supports exhibited a well-defined 3DOM-m nanostructure,and AMnO_(x)nanoparticles with 10–50 nm were evenly dispersed on the inner walls of the uniform macropores.In addition,the as-prepared catalysts exhibited good catalytic performance for soot combustion.Among the prepared catalysts,CsMnO_(x)/3DOM-m Ti_(0.7)Si_(0.3)O_(2)had the highest catalytic activity for soot combustion,with T10,T50,and T90(the temperatures corresponding to soot conversion rates of 10%,50%,and 90%) values of 285,355,and 393℃,respectively.The high catalytic activity of the CsMnO_(x)/3 DOM-m Ti_(0.7)Si_(0.3)O_(2)catalysts was attributed to their excellent low-temperature reducibility and homogeneous macroporous–mesoporous structure,as well as to the synergistic effects between Cs and Mn species and between CsMnO_(x)and the Ti_(0.7)Si_(0.3)O_(2)support.
