Ordered mesoporous Mn2O3 (meso‐Mn2O3) and meso‐Mn2O3‐supported Pd, Pt, and Pd‐Pt alloy x(PdyPt)/meso‐Mn2O3; x = (0.10?1.50) wt%; Pd/Pt molar ratio (y) = 4.9?5.1 nanocatalysts were prepared using KIT‐6‐templated...Ordered mesoporous Mn2O3 (meso‐Mn2O3) and meso‐Mn2O3‐supported Pd, Pt, and Pd‐Pt alloy x(PdyPt)/meso‐Mn2O3; x = (0.10?1.50) wt%; Pd/Pt molar ratio (y) = 4.9?5.1 nanocatalysts were prepared using KIT‐6‐templated and poly(vinyl alcohol)‐protected reduction methods, respectively.The meso‐Mn2O3 had a high surface area, i.e., 106 m2/g, and a cubic crystal structure. Noble‐metalnanoparticles (NPs) of size 2.1?2.8 nm were uniformly dispersed on the meso‐Mn2O3 surfaces. AlloyingPd with Pt enhanced the catalytic activity in methane combustion; 1.41(Pd5.1Pt)/meso‐Mn2O3gave the best performance; T10%, T50%, and T90% (the temperatures required for achieving methaneconversions of 10%, 50%, and 90%) were 265, 345, and 425 °C, respectively, at a space velocity of20000 mL/(g?h). The effects of SO2, CO2, H2O, and NO on methane combustion over1.41(Pd5.1Pt)/meso‐Mn2O3 were also examined. We conclude that the good catalytic performance of1.41(Pd5.1Pt)/meso‐Mn2O3 is associated with its high‐quality porous structure, high adsorbed oxygen species concentration, good low‐temperature reducibility, and strong interactions between Pd‐Pt alloy NPs and the meso‐Mn2O3 support.展开更多
The meso-Co3O4 and AgxAuyPd/meso-Co3O4 catalysts were prepared using the KIT-6-templating and polyvinyl alcohol-protected NaBH4 reduction methods,respectively.Various techniques were used to characterize physicochemic...The meso-Co3O4 and AgxAuyPd/meso-Co3O4 catalysts were prepared using the KIT-6-templating and polyvinyl alcohol-protected NaBH4 reduction methods,respectively.Various techniques were used to characterize physicochemical properties of these materials.Catalytic performance of the samples was evaluated for methanol combustion.The cubically crystallized Co3O4 support displayed a three-dimensionally ordered mesoporous structure.The supported noble metal nanoparticles(NPs)possessed a surface area of 115.125 m^2/g,with the noble NPs(average size=2.8.4.5 nm)being uniformly dispersed on the surface of meso-Co3O4.Among all of the samples,0.68 wt%Ag0.75Au1.14Pd/meso-Co3O4 showed the highest catalytic activity(T50%=100℃and T90%=112℃at a space velocity of 80000 mL(g^–1 h^–1).The partial deactivation of the 0.68 wt%Ag0.75Au1.14Pd/meso-Co3O4 sample due to water vapor or carbon dioxide introduction was reversible.It is concluded that the good catalytic performance of 0.68 wt%Ag0.75Au1.14Pd/meso-Co3O4 was associated with its highly dispersed Ag0.75Au1.14Pd alloy NPs,high adsorbed oxygen species concentration,good low-temperature reducibility,and strong interaction between Ag0.75Au1.14Pd alloy NPs and meso-Co3O4.展开更多
Noble metals are downsized to nano-/subnanoscale to improve their catalytic activity and atom-economy.However,the stabilities in chemical state and catalytic performance of these nanocatalysts often suffer during hars...Noble metals are downsized to nano-/subnanoscale to improve their catalytic activity and atom-economy.However,the stabilities in chemical state and catalytic performance of these nanocatalysts often suffer during harsh conditions.For Pt nanoparticles(NPs)supported on CeO2,activated oxygen diffused from the support over-stabilizes the active sites of Pt,degrading its performance at mild temperature.In this work,Pt nanocatalysts with unique structure of triple-junction are synthesized by selectively growing Pt NPs on the carbon-CeO2 interface.Impressively,the Pt NPs exhibit much enhanced catalytic stability and high activity for CO oxidation at mild temperature.The enhancement is attributed to electron donation from graphitized carbon and the confinement effect from the high-density nanopores of the CeO2 support.The triple-junction of Pt-C-CeO2,combining the merits of CeO2 for activating O2 and electron donating capability of carbon,provides new inspiration to the fabrication of high-performance nanocatalysts.展开更多
Integration of molybdenum disulfide （MoS2） onto high surface area photocathod is highly desired to minimize the overpotential for the solar-powered hydrogen evolution reaction （HER）. Semiconductor nanowires （NWs...Integration of molybdenum disulfide （MoS2） onto high surface area photocathod is highly desired to minimize the overpotential for the solar-powered hydrogen evolution reaction （HER）. Semiconductor nanowires （NWs） are beneficial use in photoelectrochemistry because of their large electrochemically availab surface area and inherent ability to decouple light absorption and the transpo of minority carriers. Here, silicon （Si） NW arrays were employed as a mod photocathode system for MoS2 wrapping, and their solar-driven HER activil was evaluated. The photocathode is made up of a well-defined MoSJTiO2/Si coaxial NW heterostructure, which yielded photocurrent density up to 15 mA/cm2 （at 0 V vs. the reversible hydrogen electrode （RHE）） with goo stability under the operating conditions employed. This work reveals the earth-abundant electrocatalysts coupled with high surface area NW electrod~ can provide performance comparable to noble metal catalysts for photocathod hydrogen evolution.展开更多
基金supported by the Ph.D.Program Foundation of Ministry of Education of China(20131103110002)the NNSF of China(21377008)+2 种基金National High Technology Research and Development Program(863 Program,2015AA034603)Foundation on the Creative Research Team Con-struction Promotion Project of Beijing Municipal InstitutionsScientific Research Base Construction-Science and Technology Creation Plat-form-National Materials Research Base Construction~~
文摘Ordered mesoporous Mn2O3 (meso‐Mn2O3) and meso‐Mn2O3‐supported Pd, Pt, and Pd‐Pt alloy x(PdyPt)/meso‐Mn2O3; x = (0.10?1.50) wt%; Pd/Pt molar ratio (y) = 4.9?5.1 nanocatalysts were prepared using KIT‐6‐templated and poly(vinyl alcohol)‐protected reduction methods, respectively.The meso‐Mn2O3 had a high surface area, i.e., 106 m2/g, and a cubic crystal structure. Noble‐metalnanoparticles (NPs) of size 2.1?2.8 nm were uniformly dispersed on the meso‐Mn2O3 surfaces. AlloyingPd with Pt enhanced the catalytic activity in methane combustion; 1.41(Pd5.1Pt)/meso‐Mn2O3gave the best performance; T10%, T50%, and T90% (the temperatures required for achieving methaneconversions of 10%, 50%, and 90%) were 265, 345, and 425 °C, respectively, at a space velocity of20000 mL/(g?h). The effects of SO2, CO2, H2O, and NO on methane combustion over1.41(Pd5.1Pt)/meso‐Mn2O3 were also examined. We conclude that the good catalytic performance of1.41(Pd5.1Pt)/meso‐Mn2O3 is associated with its high‐quality porous structure, high adsorbed oxygen species concentration, good low‐temperature reducibility, and strong interactions between Pd‐Pt alloy NPs and the meso‐Mn2O3 support.
基金supported by the National Natural Science Foundation of China(21677004,21876006,and 21622701)the National High Technology Research and Development Program of China(863 Program,2015AA034603)~~
文摘The meso-Co3O4 and AgxAuyPd/meso-Co3O4 catalysts were prepared using the KIT-6-templating and polyvinyl alcohol-protected NaBH4 reduction methods,respectively.Various techniques were used to characterize physicochemical properties of these materials.Catalytic performance of the samples was evaluated for methanol combustion.The cubically crystallized Co3O4 support displayed a three-dimensionally ordered mesoporous structure.The supported noble metal nanoparticles(NPs)possessed a surface area of 115.125 m^2/g,with the noble NPs(average size=2.8.4.5 nm)being uniformly dispersed on the surface of meso-Co3O4.Among all of the samples,0.68 wt%Ag0.75Au1.14Pd/meso-Co3O4 showed the highest catalytic activity(T50%=100℃and T90%=112℃at a space velocity of 80000 mL(g^–1 h^–1).The partial deactivation of the 0.68 wt%Ag0.75Au1.14Pd/meso-Co3O4 sample due to water vapor or carbon dioxide introduction was reversible.It is concluded that the good catalytic performance of 0.68 wt%Ag0.75Au1.14Pd/meso-Co3O4 was associated with its highly dispersed Ag0.75Au1.14Pd alloy NPs,high adsorbed oxygen species concentration,good low-temperature reducibility,and strong interaction between Ag0.75Au1.14Pd alloy NPs and meso-Co3O4.
基金supported by the National Key Research and Development Program of China(2016YFB0701100)the National Natural Science Foundation of China(51771047,51525101 and 51971059)the Fundamental Research Funds for the Central Universities(N180204014)。
文摘Noble metals are downsized to nano-/subnanoscale to improve their catalytic activity and atom-economy.However,the stabilities in chemical state and catalytic performance of these nanocatalysts often suffer during harsh conditions.For Pt nanoparticles(NPs)supported on CeO2,activated oxygen diffused from the support over-stabilizes the active sites of Pt,degrading its performance at mild temperature.In this work,Pt nanocatalysts with unique structure of triple-junction are synthesized by selectively growing Pt NPs on the carbon-CeO2 interface.Impressively,the Pt NPs exhibit much enhanced catalytic stability and high activity for CO oxidation at mild temperature.The enhancement is attributed to electron donation from graphitized carbon and the confinement effect from the high-density nanopores of the CeO2 support.The triple-junction of Pt-C-CeO2,combining the merits of CeO2 for activating O2 and electron donating capability of carbon,provides new inspiration to the fabrication of high-performance nanocatalysts.
文摘Integration of molybdenum disulfide （MoS2） onto high surface area photocathod is highly desired to minimize the overpotential for the solar-powered hydrogen evolution reaction （HER）. Semiconductor nanowires （NWs） are beneficial use in photoelectrochemistry because of their large electrochemically availab surface area and inherent ability to decouple light absorption and the transpo of minority carriers. Here, silicon （Si） NW arrays were employed as a mod photocathode system for MoS2 wrapping, and their solar-driven HER activil was evaluated. The photocathode is made up of a well-defined MoSJTiO2/Si coaxial NW heterostructure, which yielded photocurrent density up to 15 mA/cm2 （at 0 V vs. the reversible hydrogen electrode （RHE）） with goo stability under the operating conditions employed. This work reveals the earth-abundant electrocatalysts coupled with high surface area NW electrod~ can provide performance comparable to noble metal catalysts for photocathod hydrogen evolution.
