In this work,a series of Ce-Ti composite oxides with different Ti/Ce molar ratios was prepared by coprecipitation method,and investigated for the catalytic degradation of toluene and selective catalytic reduction of N...In this work,a series of Ce-Ti composite oxides with different Ti/Ce molar ratios was prepared by coprecipitation method,and investigated for the catalytic degradation of toluene and selective catalytic reduction of NO.The phase transition process between Ce species and Ti species is limited by modulating the interaction between Ce4+and Ti4+,while a completely amorphous composite is generated with an appropriate molar ratio of Ti/Ce(1.5/1).The catalyst CeTi1.5Oxexhibits the best catalytic performance,where the values of T90and T50for deep degradation of toluene are 297 and 330℃respectively at high weight hours space velocity(WHSV=120000 mL/(g·h)).Compared with CeO_(2),T90and T50decrease by48 and 34℃respectively while declining by 67 and 70℃compared to TiO_(2).For the SCR reaction,CeTi1.5Oxreaches 100%NO conversion at 250℃with WHSV=60000 mL/(g·h),reduced by 50℃compared to pure CeO_(2).The amorphous nanostructure with highly dispersed Ce and Ti species was confirmed by transmission electron microscopy(TEM)and X-ray diffraction(XRD)characterizations.The X-ray photoelectron spectroscopy(XPS)and Raman analyses show that a large number of active Ce-O-Ti species and surface oxygen vacancies are generated due to the strong interaction between Ti^(4+)and Ce^(4+)in CeTi_(1.5)O_(x).Additionally,H_(2)-TPR and O_(2)-TPD further confirm that the interaction promotes the low-temperature reducibility and mobility of surface-active oxygen species.Meanwhile,in-situ DRIFTS study reveals that CeTi1.5Oxwith amorphous nanostructure can dramatically enhance the dissociative and complete oxidation capacity for toluene.展开更多
We made precipitated nano-ceria(~5 nm) on the surface of the catalyst by heat treatment of Cesupersaturated amorphous CeTiOxto improve the oxygen storage properties of CeO_2. The catalysts were prepared by sol-gel met...We made precipitated nano-ceria(~5 nm) on the surface of the catalyst by heat treatment of Cesupersaturated amorphous CeTiOxto improve the oxygen storage properties of CeO_2. The catalysts were prepared by sol-gel methods and TiO_2 nanoparticles were preferentially generated as a core material to form selective Ce-supersaturated structure on the catalyst surface. Reaction temperature and amount of doping element are optimized to induce selective crystallization of CeO_2. Cee Ce(2 nd shell)bond around 0.38 nm of Ce L3-edge extended X-ray absorption fine structure is reduced and nanostructure of precipitated ceria on the surface is observed by HREM. The catalyst is present as amorphous with precipitated nano-CeO_2 on the surface. The de-NOxefficiency of the catalyst, which has precipitated CeO_2, improves by ~50% owing to the simultaneous reactions of the nano CeO_2 and the amorphous CeTiO_x.展开更多
基金Project supported by the National Natural Science Foundation of China(22072096,22108184)。
文摘In this work,a series of Ce-Ti composite oxides with different Ti/Ce molar ratios was prepared by coprecipitation method,and investigated for the catalytic degradation of toluene and selective catalytic reduction of NO.The phase transition process between Ce species and Ti species is limited by modulating the interaction between Ce4+and Ti4+,while a completely amorphous composite is generated with an appropriate molar ratio of Ti/Ce(1.5/1).The catalyst CeTi1.5Oxexhibits the best catalytic performance,where the values of T90and T50for deep degradation of toluene are 297 and 330℃respectively at high weight hours space velocity(WHSV=120000 mL/(g·h)).Compared with CeO_(2),T90and T50decrease by48 and 34℃respectively while declining by 67 and 70℃compared to TiO_(2).For the SCR reaction,CeTi1.5Oxreaches 100%NO conversion at 250℃with WHSV=60000 mL/(g·h),reduced by 50℃compared to pure CeO_(2).The amorphous nanostructure with highly dispersed Ce and Ti species was confirmed by transmission electron microscopy(TEM)and X-ray diffraction(XRD)characterizations.The X-ray photoelectron spectroscopy(XPS)and Raman analyses show that a large number of active Ce-O-Ti species and surface oxygen vacancies are generated due to the strong interaction between Ti^(4+)and Ce^(4+)in CeTi_(1.5)O_(x).Additionally,H_(2)-TPR and O_(2)-TPD further confirm that the interaction promotes the low-temperature reducibility and mobility of surface-active oxygen species.Meanwhile,in-situ DRIFTS study reveals that CeTi1.5Oxwith amorphous nanostructure can dramatically enhance the dissociative and complete oxidation capacity for toluene.
基金Project supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)through GCRC-SOP(2011-0030013)
文摘We made precipitated nano-ceria(~5 nm) on the surface of the catalyst by heat treatment of Cesupersaturated amorphous CeTiOxto improve the oxygen storage properties of CeO_2. The catalysts were prepared by sol-gel methods and TiO_2 nanoparticles were preferentially generated as a core material to form selective Ce-supersaturated structure on the catalyst surface. Reaction temperature and amount of doping element are optimized to induce selective crystallization of CeO_2. Cee Ce(2 nd shell)bond around 0.38 nm of Ce L3-edge extended X-ray absorption fine structure is reduced and nanostructure of precipitated ceria on the surface is observed by HREM. The catalyst is present as amorphous with precipitated nano-CeO_2 on the surface. The de-NOxefficiency of the catalyst, which has precipitated CeO_2, improves by ~50% owing to the simultaneous reactions of the nano CeO_2 and the amorphous CeTiO_x.
基金supported by the National Natural Science Foundation of China (21277060 and 21107030)the Development Program of the Science and Technology of Shandong Province (2011GSF11702)+3 种基金the Foundation for Outstanding Young Scientist in Shandong Province (BS2011HZ002)the Natural Science Foundation of Shandong Province (ZR2013BQ003)the Open Project from Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control of Nanjing University of Information Science and Technology (KHK1116)Jiangsu Province Innovation Platform for Superiority Subject of Environmental Science and Engineering~~
