A series of catalysts consisting of three‐dimensionally ordered macroporous(3DOM)x‐CeO2/Al2O3‐supported Au nanoparticles(x=2,10,20,and40wt%)were successfully synthesized using a reduction‐deposition method.These c...A series of catalysts consisting of three‐dimensionally ordered macroporous(3DOM)x‐CeO2/Al2O3‐supported Au nanoparticles(x=2,10,20,and40wt%)were successfully synthesized using a reduction‐deposition method.These catalysts were characterized using scanning electron microscopy,the Brunauer‐Emmett‐Teller method,X‐ray diffraction,transmission electron microscopy,ultraviolet‐visible spectroscopy,and temperature‐programmed reduction by H2.Au nanoparticles of mean particle size5nm were well dispersed and supported on the inner walls of uniform macropores.The3DOM structure improved the contact efficiency between soot and the catalyst.An Al‐Ce‐O solid solution was formed in the multilayer support,i.e.,x‐CeO2/Al2O3,by the incorporation of Al3+ions into the CeO2lattice,which resulted in the creation of extrinsic oxygen vacancies.Strong interactions between the metal(Au)and the support(Ce)increased the amount of active oxygen species,and this promoted soot oxidation.The catalytic performance in soot combustion was evaluated using a temperature‐programmed oxidation technique.The presence of CeO2nanolayers in the3DOM Au/x‐CeO2/Al2O3catalysts clearly improved the catalytic activities in soot oxidation.Among the prepared catalysts,3DOM Au/20%CeO2/Al2O3showed high catalytic activity and stability in diesel soot oxidation.展开更多
Ultrasonic treatment and hydrothermal method were applied in the traditional homogeneous precipitation for nano-TiO_2 preparation, which was used as carrier material for the production of honeycomb selective catalytic...Ultrasonic treatment and hydrothermal method were applied in the traditional homogeneous precipitation for nano-TiO_2 preparation, which was used as carrier material for the production of honeycomb selective catalytic reduction(SCR) catalyst. The influence rules of the two improved methods on characterization of TiO_2 samples, denitration activity and mechanical strength of honeycomb SCR catalyst samples were mainly focused on. The results indicate that the specific surface area, particle size and uniformity of TiO_2 samples are significantly improved by both of the ultrasonic and hydrothermal treatments compared with the traditional homogeneous precipitation. Also, the denitration activities of catalyst samples are enhanced by the two improved methods(the NO_x reduction ratio increases from 88.89% to 95.45% by ultrasonic homogeneous precipitation process, and to 94.12% by hydrothermal homogeneous precipitation process). On the other hand, because of good spherical shape and high particle distribution of TiO_2 sample from hydrothermal homogeneous precipitation process, the corresponding honeycomb catalyst samples get the best mechanical strength, which is even higher than that of the reference sample from commercial nano-TiO_2. So, it is concluded that the hydrothermal homogeneous precipitation can be a feasible and effective preparation method of TiO_2 carrier for the honeycomb SCR catalyst production.展开更多
The effect of a wide variety of metal oxide （MOx） supports has been discussed for CO oxidation on nanoparticulate gold catalysts. By using typical co‐precipitation and deposition–precipitation methods and under id...The effect of a wide variety of metal oxide （MOx） supports has been discussed for CO oxidation on nanoparticulate gold catalysts. By using typical co‐precipitation and deposition–precipitation methods and under identical calcination conditions, supported gold catalysts were prepared on a wide variety of MOx supports, and the temperature for 50%conversion was measured to qualita‐tively evaluate the catalytic activities of these simple MOx and supported Au catalysts. Furthermore, the difference in these temperatures for the simple MOx compared to the supported Au catalysts is plotted against the metal–oxygen binding energies of the support MOx. A clear volcano‐like correla‐tion between the temperature difference and the metal–oxygen binding energies is observed. This correlation suggests that the use of MOx with appropriate metal–oxygen binding energies （300–500 kJ/atom O） greatly improves the catalytic activity of MOx by the deposition of Au NPs.展开更多
In the intrinsic pathway of apoptosis, stresses of mitochondrial reactive oxygen species （mitoROS） might be sensed as more effective signals than those in cytosol, as mitochondria are the major sources of reactive o...In the intrinsic pathway of apoptosis, stresses of mitochondrial reactive oxygen species （mitoROS） might be sensed as more effective signals than those in cytosol, as mitochondria are the major sources of reactive oxygen species （ROS） and pivotal components during cell apoptosis. Mitochondrial superoxide dismutase （SOD2） takes the leading role in eliminating mitoROS, and inhibition of SOD2 might induce severe disturbances overwhelming the mitochondrial oxidative equilibrium, which would elevate the intracellular oxidative stresses and drive cells to death. Herein, we report a general strategy to kill cancer cells by targeted inhibition of SOD2 using 2-methoxyestradiol （2-ME, an inhibitor for the SOD family） via a robust mitochondria-targeted mesoporous silica nanocarrier （mtMSN）, with the expected elevation of mitoROS and activation of apoptosis in HeLa cells. Fe304@MSN was employed in the mitochondria-targeted drug delivery and selective inhibition of mitochondrial enzymes, and was shown to be stable with good biocompatibility and high loading capacity. Due to the selective inhibition of SOD2 by 2-ME/mtMSN, enhanced elevation of mitoROS （132% of that with free 2-ME） was obtained, coupled with higher efficiency in initiating cell apoptosis （395% of that with free 2-ME in 4 h）. Finally, the 2-ME/mtMSN exhibited powerful efficacy in targeted killing of HeLa cells by taking advantage of both biological recognition and magnetic guiding, causing 97.0% cell death with only 2 Dg/mL 2-ME/mtMSN, hinting at its great potential in cancer therapy through manipulation of the delicate mitochondrial oxidative balance.展开更多
基金supported by the National High Technology Research and Development Program of China(863 Program,2015AA034603)the National Natural Science Foundation of China(21477146,21673142 and 21303263)+2 种基金the Beijing Nova Program(Z141109001814072)the Specialized Research Fund for the Doctoral Program of Higher Education(20130007120011)the Science Foundation of China University of Petroleum-Beijing(YJRC-2013-13,2462013BJRC003)~~
文摘A series of catalysts consisting of three‐dimensionally ordered macroporous(3DOM)x‐CeO2/Al2O3‐supported Au nanoparticles(x=2,10,20,and40wt%)were successfully synthesized using a reduction‐deposition method.These catalysts were characterized using scanning electron microscopy,the Brunauer‐Emmett‐Teller method,X‐ray diffraction,transmission electron microscopy,ultraviolet‐visible spectroscopy,and temperature‐programmed reduction by H2.Au nanoparticles of mean particle size5nm were well dispersed and supported on the inner walls of uniform macropores.The3DOM structure improved the contact efficiency between soot and the catalyst.An Al‐Ce‐O solid solution was formed in the multilayer support,i.e.,x‐CeO2/Al2O3,by the incorporation of Al3+ions into the CeO2lattice,which resulted in the creation of extrinsic oxygen vacancies.Strong interactions between the metal(Au)and the support(Ce)increased the amount of active oxygen species,and this promoted soot oxidation.The catalytic performance in soot combustion was evaluated using a temperature‐programmed oxidation technique.The presence of CeO2nanolayers in the3DOM Au/x‐CeO2/Al2O3catalysts clearly improved the catalytic activities in soot oxidation.Among the prepared catalysts,3DOM Au/20%CeO2/Al2O3showed high catalytic activity and stability in diesel soot oxidation.
基金Project(201031)supported by the Environmental Protection Scientific Research of Jiangsu Province,ChinaProject(BE2010184)supported by the Technology Support Program of Jiangsu Province-Industrial Parts,China
文摘Ultrasonic treatment and hydrothermal method were applied in the traditional homogeneous precipitation for nano-TiO_2 preparation, which was used as carrier material for the production of honeycomb selective catalytic reduction(SCR) catalyst. The influence rules of the two improved methods on characterization of TiO_2 samples, denitration activity and mechanical strength of honeycomb SCR catalyst samples were mainly focused on. The results indicate that the specific surface area, particle size and uniformity of TiO_2 samples are significantly improved by both of the ultrasonic and hydrothermal treatments compared with the traditional homogeneous precipitation. Also, the denitration activities of catalyst samples are enhanced by the two improved methods(the NO_x reduction ratio increases from 88.89% to 95.45% by ultrasonic homogeneous precipitation process, and to 94.12% by hydrothermal homogeneous precipitation process). On the other hand, because of good spherical shape and high particle distribution of TiO_2 sample from hydrothermal homogeneous precipitation process, the corresponding honeycomb catalyst samples get the best mechanical strength, which is even higher than that of the reference sample from commercial nano-TiO_2. So, it is concluded that the hydrothermal homogeneous precipitation can be a feasible and effective preparation method of TiO_2 carrier for the honeycomb SCR catalyst production.
文摘The effect of a wide variety of metal oxide （MOx） supports has been discussed for CO oxidation on nanoparticulate gold catalysts. By using typical co‐precipitation and deposition–precipitation methods and under identical calcination conditions, supported gold catalysts were prepared on a wide variety of MOx supports, and the temperature for 50%conversion was measured to qualita‐tively evaluate the catalytic activities of these simple MOx and supported Au catalysts. Furthermore, the difference in these temperatures for the simple MOx compared to the supported Au catalysts is plotted against the metal–oxygen binding energies of the support MOx. A clear volcano‐like correla‐tion between the temperature difference and the metal–oxygen binding energies is observed. This correlation suggests that the use of MOx with appropriate metal–oxygen binding energies （300–500 kJ/atom O） greatly improves the catalytic activity of MOx by the deposition of Au NPs.
文摘In the intrinsic pathway of apoptosis, stresses of mitochondrial reactive oxygen species （mitoROS） might be sensed as more effective signals than those in cytosol, as mitochondria are the major sources of reactive oxygen species （ROS） and pivotal components during cell apoptosis. Mitochondrial superoxide dismutase （SOD2） takes the leading role in eliminating mitoROS, and inhibition of SOD2 might induce severe disturbances overwhelming the mitochondrial oxidative equilibrium, which would elevate the intracellular oxidative stresses and drive cells to death. Herein, we report a general strategy to kill cancer cells by targeted inhibition of SOD2 using 2-methoxyestradiol （2-ME, an inhibitor for the SOD family） via a robust mitochondria-targeted mesoporous silica nanocarrier （mtMSN）, with the expected elevation of mitoROS and activation of apoptosis in HeLa cells. Fe304@MSN was employed in the mitochondria-targeted drug delivery and selective inhibition of mitochondrial enzymes, and was shown to be stable with good biocompatibility and high loading capacity. Due to the selective inhibition of SOD2 by 2-ME/mtMSN, enhanced elevation of mitoROS （132% of that with free 2-ME） was obtained, coupled with higher efficiency in initiating cell apoptosis （395% of that with free 2-ME in 4 h）. Finally, the 2-ME/mtMSN exhibited powerful efficacy in targeted killing of HeLa cells by taking advantage of both biological recognition and magnetic guiding, causing 97.0% cell death with only 2 Dg/mL 2-ME/mtMSN, hinting at its great potential in cancer therapy through manipulation of the delicate mitochondrial oxidative balance.
