The three-dimensional ordered macroporous CeO2:Yb,Er materials were prepared, and the influence of doping concentra- tion of Yb3+ or Er3+ ions on upconversion property was investigated. Green and red upconversion e...The three-dimensional ordered macroporous CeO2:Yb,Er materials were prepared, and the influence of doping concentra- tion of Yb3+ or Er3+ ions on upconversion property was investigated. Green and red upconversion emissions were observed under the excitation of 980 nm at room temperature. It was found that the ratio of red to green upconversion emission intensity increased with increasing of concentration of the Yb3+ or Er3+ ions in the three-dimensional ordered macroporous CeO2:Yb,Er materials. When the concentration of Yb3+ was 10 mol%, pure red upconversion emission was obtained. The varied mechanism of ratio of red to green upconversion emission intensity was discussed with the concentration of Yb3+ or Er3+ ions.展开更多
Ordered macroporous materials with rapid mass transport and enhanced active site accessibility are essential for achieving improved catalytic activity.In this study,boron phosphate crystals with a three-dimensionally ...Ordered macroporous materials with rapid mass transport and enhanced active site accessibility are essential for achieving improved catalytic activity.In this study,boron phosphate crystals with a three-dimensionally interconnected ordered macroporous structure and a robust framework were fabricated and used as stable and selective catalysts in the oxidative dehydrogenation(ODH)of propane.Due to the improved mass diffusion and higher number of exposed active sites in the ordered macroporous structure,the catalyst exhibited a remarkable olefin productivity of^16 golefin gcat^-1 h^-1,which is up to 2–100 times higher than that of ODH catalysts reported to date.The selectivity for olefins was 91.5%(propene:82.5%,ethene:9.0%)at 515℃,with a propane conversion of 14.3%.At the same time,the selectivity for the unwanted deep-oxidized CO2 product remained less than 1.0%.The tri-coordinated surface boron species were identified as the active catalytic sites for the ODH of propane.This study provides a route for preparing a new type of metal-free catalyst with stable structure against oxidation and remarkable catalytic activity,which may represent a potential candidate to promote the industrialization of the ODH process.展开更多
Nanocatalysts consisting of three‐dimensionally ordered macroporous(3DOM)TiO2‐supported ultrafine Pd nanoparticles(Pd/3DOM‐TiO2‐GBMR)were readily fabricated by gas bubbling‐assisted membrane reduction(GBMR)method...Nanocatalysts consisting of three‐dimensionally ordered macroporous(3DOM)TiO2‐supported ultrafine Pd nanoparticles(Pd/3DOM‐TiO2‐GBMR)were readily fabricated by gas bubbling‐assisted membrane reduction(GBMR)method.These catalysts had a well‐defined and highly ordered macroporous nanostructure with an average pore size of 280 nm.In addition,ultrafine hemispherical Pd nanoparticles(NPs)with a mean particle size of 1.1 nm were found to be well dispersed over the surface of the 3DOM‐TiO2 support and deposited on the inner walls of the material.The nanostructure of the 3DOM‐TiO2 support ensured efficient contact between soot particles and the catalyst.The large interface area between the ultrafine Pd NPs and the TiO2 also increased the density of sites for O2 activation as a result of the strong metal(Pd)‐support(TiO2)interaction(SMSI).A Pd/3DOM‐TiO2‐GBMR catalyst with ultrafine Pd NPs(1.1 nm)exhibited higher catalytic activity during diesel soot combustion compared with that obtained from a specimen having relatively large Pd NPs(5.0 nm).The T10,T50 and T90 values obtained from the former were 295,370 and 415°C.Both the activity and nanostructure of the Pd/3DOM‐TiO2‐GBMR catalyst were stable over five replicate soot oxidation trials.These results suggest that nanocatalysts having a 3DOM structure together with ultrafine Pd NPs can decrease the amount of Pd required,and that this approach has potential practical applications in the catalytic combustion of diesel soot particles.展开更多
Meso-structured (opal and inverse opal) polymeric hydrogels of varied morphology and composition wereprepared by using two methods: post-modification of the template-synthesized structured polymers and template-polyme...Meso-structured (opal and inverse opal) polymeric hydrogels of varied morphology and composition wereprepared by using two methods: post-modification of the template-synthesized structured polymers and template-polymerization of functional monomers. A polyacrylic acid based inverse opal hydrogel was chosen to demonstrate its fastpH response by changing color, which is important in designing tunable photonic crystals. Template effects of the hydrogelson controlling structure of the template-synthesized inorganic materials were discussed. The catalytic effect of acid groups inthe templates was emphasized for a preferential formation of TiO_2 in the region containing acid groups, which allowedduplicating inorganic colloidal crytals from colloidal crystal hydrogels (or macroporous products from macroporoushydrogels) via one step duplication.展开更多
Au/3DOM(three-dimensionally ordered macroporous) Al2O3 and Au/CeO2/3DOM Al2O3 were prepared using a reduction-deposition method and characterized using scanning electron microscopy,N2 adsorption-desorption,X-ray dif...Au/3DOM(three-dimensionally ordered macroporous) Al2O3 and Au/CeO2/3DOM Al2O3 were prepared using a reduction-deposition method and characterized using scanning electron microscopy,N2 adsorption-desorption,X-ray diffraction,transmission electron microscopy,ultraviolet-visible spectroscopy,temperature-programmed hydrogen reduction,and X-ray photoelectron spectroscopy.Au nanoparticles of similar sizes were well dispersed and supported on the inner walls of uniform macropores.The norminal Au loading is 2%.Al-Ce-O solid solution in CeO2/3DOM Al2O3 catalysts can be formed due to the incorporation of Al^3+ ions into the ceria lattice,which causes the creation of extrinsic oxygen vacancies.The extrinsic oxygen vacancies improved the oxygen-transport properties.The strong metal-support interactions between Au and CeO2 increased the amount of active oxygen on the Au nanoparticle surfaces,and this promoted soot oxidation.The activities of the Au-based catalysts were higher than those of the supports(Al2O3 or CeO2/3DOM Al2O3) at low temperature.Au/CeO2/3DOM Al2O3 had the highest catalytic activity for soot combustion,with T(10),T(50),and T(90) values of 273,364,and 412℃,respectively.展开更多
基金supported by the Reserve Talents Project of Yunnan Province(2013HB068)Applied Basic Research Program of Yunnan Province(2014FB127)
文摘The three-dimensional ordered macroporous CeO2:Yb,Er materials were prepared, and the influence of doping concentra- tion of Yb3+ or Er3+ ions on upconversion property was investigated. Green and red upconversion emissions were observed under the excitation of 980 nm at room temperature. It was found that the ratio of red to green upconversion emission intensity increased with increasing of concentration of the Yb3+ or Er3+ ions in the three-dimensional ordered macroporous CeO2:Yb,Er materials. When the concentration of Yb3+ was 10 mol%, pure red upconversion emission was obtained. The varied mechanism of ratio of red to green upconversion emission intensity was discussed with the concentration of Yb3+ or Er3+ ions.
文摘Ordered macroporous materials with rapid mass transport and enhanced active site accessibility are essential for achieving improved catalytic activity.In this study,boron phosphate crystals with a three-dimensionally interconnected ordered macroporous structure and a robust framework were fabricated and used as stable and selective catalysts in the oxidative dehydrogenation(ODH)of propane.Due to the improved mass diffusion and higher number of exposed active sites in the ordered macroporous structure,the catalyst exhibited a remarkable olefin productivity of^16 golefin gcat^-1 h^-1,which is up to 2–100 times higher than that of ODH catalysts reported to date.The selectivity for olefins was 91.5%(propene:82.5%,ethene:9.0%)at 515℃,with a propane conversion of 14.3%.At the same time,the selectivity for the unwanted deep-oxidized CO2 product remained less than 1.0%.The tri-coordinated surface boron species were identified as the active catalytic sites for the ODH of propane.This study provides a route for preparing a new type of metal-free catalyst with stable structure against oxidation and remarkable catalytic activity,which may represent a potential candidate to promote the industrialization of the ODH process.
基金supported by the National Natural Science Foundation of China(21673142,21477164)the National High Technology Research and Development Program of China(863 Program,2015AA030903)~~
文摘Nanocatalysts consisting of three‐dimensionally ordered macroporous(3DOM)TiO2‐supported ultrafine Pd nanoparticles(Pd/3DOM‐TiO2‐GBMR)were readily fabricated by gas bubbling‐assisted membrane reduction(GBMR)method.These catalysts had a well‐defined and highly ordered macroporous nanostructure with an average pore size of 280 nm.In addition,ultrafine hemispherical Pd nanoparticles(NPs)with a mean particle size of 1.1 nm were found to be well dispersed over the surface of the 3DOM‐TiO2 support and deposited on the inner walls of the material.The nanostructure of the 3DOM‐TiO2 support ensured efficient contact between soot particles and the catalyst.The large interface area between the ultrafine Pd NPs and the TiO2 also increased the density of sites for O2 activation as a result of the strong metal(Pd)‐support(TiO2)interaction(SMSI).A Pd/3DOM‐TiO2‐GBMR catalyst with ultrafine Pd NPs(1.1 nm)exhibited higher catalytic activity during diesel soot combustion compared with that obtained from a specimen having relatively large Pd NPs(5.0 nm).The T10,T50 and T90 values obtained from the former were 295,370 and 415°C.Both the activity and nanostructure of the Pd/3DOM‐TiO2‐GBMR catalyst were stable over five replicate soot oxidation trials.These results suggest that nanocatalysts having a 3DOM structure together with ultrafine Pd NPs can decrease the amount of Pd required,and that this approach has potential practical applications in the catalytic combustion of diesel soot particles.
基金This work is supported by the National Natural Science Foundation of China (Grant No. 20023003 & 20128004), and Creative Funding sponsored by Center for Molecular Science, Institute of Chemistry, Chinese Academy of Sciences.
文摘Meso-structured (opal and inverse opal) polymeric hydrogels of varied morphology and composition wereprepared by using two methods: post-modification of the template-synthesized structured polymers and template-polymerization of functional monomers. A polyacrylic acid based inverse opal hydrogel was chosen to demonstrate its fastpH response by changing color, which is important in designing tunable photonic crystals. Template effects of the hydrogelson controlling structure of the template-synthesized inorganic materials were discussed. The catalytic effect of acid groups inthe templates was emphasized for a preferential formation of TiO_2 in the region containing acid groups, which allowedduplicating inorganic colloidal crytals from colloidal crystal hydrogels (or macroporous products from macroporoushydrogels) via one step duplication.
基金supported by the National Natural Science Foundation of China (21477146,21303263)the National High Technology Research and Development Program of China (863 Program,2015AA034603)+2 种基金Beijing Nova Program (Z141109001814072)the Specialized Research Fund for the Doctoral Program of Higher Education of China (20130007120011)the Science Foundation of China University of Petroleum-Beijing (YJRC-2013-13,2462013BJRC003)~~
文摘Au/3DOM(three-dimensionally ordered macroporous) Al2O3 and Au/CeO2/3DOM Al2O3 were prepared using a reduction-deposition method and characterized using scanning electron microscopy,N2 adsorption-desorption,X-ray diffraction,transmission electron microscopy,ultraviolet-visible spectroscopy,temperature-programmed hydrogen reduction,and X-ray photoelectron spectroscopy.Au nanoparticles of similar sizes were well dispersed and supported on the inner walls of uniform macropores.The norminal Au loading is 2%.Al-Ce-O solid solution in CeO2/3DOM Al2O3 catalysts can be formed due to the incorporation of Al^3+ ions into the ceria lattice,which causes the creation of extrinsic oxygen vacancies.The extrinsic oxygen vacancies improved the oxygen-transport properties.The strong metal-support interactions between Au and CeO2 increased the amount of active oxygen on the Au nanoparticle surfaces,and this promoted soot oxidation.The activities of the Au-based catalysts were higher than those of the supports(Al2O3 or CeO2/3DOM Al2O3) at low temperature.Au/CeO2/3DOM Al2O3 had the highest catalytic activity for soot combustion,with T(10),T(50),and T(90) values of 273,364,and 412℃,respectively.