The Ni-CeO2/Al2O3 catalysts with a nickel content of 15 wt% prepared via impregnating boehmite were found to be highly active and stable for methanation of carbon dioxide with hydrogen at a H2/CO2 molar ratio of 4. Th...The Ni-CeO2/Al2O3 catalysts with a nickel content of 15 wt% prepared via impregnating boehmite were found to be highly active and stable for methanation of carbon dioxide with hydrogen at a H2/CO2 molar ratio of 4. The effects of CeO2 content and reaction temperature on the performance of the Ni-CeO2/Al2O3 catalysts were studied in detail. The results showed that the catalytic performance was strongly dependent on the CeO2 content in Ni-CeO2/Al2O3 catalysts and that the catalysts with 2 wt% CeO2 had the highest catalytic activity among the tested ones at 350 ℃. The XRD and H2-TPR characterizations revealed that the addition of CeO2 decreased the reduction temperature by altering the interaction between Ni and Al2O3, and improved the reducibility of the catalyst. Preliminary stability test of 120 h on stream over the Ni-2CeO2/Al2O3 catalyst at 350 ℃ revealed that the catalyst was much better than the unpromoted one.展开更多
The catalyst function was achieved in two regions in an oxygen permeation membrane reactor: H2 dissociated and reacted with lattice oxygen or oxygen ions to form H20 near the membrane surface. The H20 formed could re...The catalyst function was achieved in two regions in an oxygen permeation membrane reactor: H2 dissociated and reacted with lattice oxygen or oxygen ions to form H20 near the membrane surface. The H20 formed could react with the residual CH4 away from the membrane surface area.展开更多
It is shown that active-tunable terahertz absorbers can be realized in a sandwich-structured system comprising an ultrathin dielectric film(polyimide) on a temperature-sensitive substrate(InSb) with a metal film on th...It is shown that active-tunable terahertz absorbers can be realized in a sandwich-structured system comprising an ultrathin dielectric film(polyimide) on a temperature-sensitive substrate(InSb) with a metal film on the back by utilizing the intrinsic carrier density(N) variation in InSb. When increasing the temperature from 250 to 320 K, N in InSb varied from ~5.50×1015 to ~2.98×1016 cm–3. Fixing the thickness of dielectric film with the value of 1.37 μm, the absorption peak shifted from 1.41 to 3.29 THz while keeping absorption higher than 99%. This active tunability can respond to even a slight temperature perturbation, and shows polarization insensitivity as well as high tolerance of incidence-angle(absorption peak can still exceed 90% even the incidence angle reaches 60°). Besides, the refractive index of polyimide(PI) has thermal stability at the terahertz range and the merit of good workability. These characteristics guarantee the stability of activetunable performance. The peculiarities and innovations of this proposal promise a wide range of high efficiency terahertz devices, such as thermal sensors, spatial light modulators(SLMs) and so on.展开更多
Mesocrystals, the non-classical crystals with highly ordered nanoparticle superstructures, have shown great potential in many applications because of their newly collective properties. However, there is still a lack o...Mesocrystals, the non-classical crystals with highly ordered nanoparticle superstructures, have shown great potential in many applications because of their newly collective properties. However, there is still a lack of a facile and general synthesis strategy to organize and integrate distinct components into complex mesocrystals, and of reported application for them in industrial catalytic reactions. Herein we report a general bottom-up synthesis of CuO-based trimetallic oxide mesocrystals (denoted as CuO-M1Ox-M2Oy, where M1 and M2 = Zn, In, Fe, Ni, Mn, and Co) using a simple precipitation method followed by a hydrothermal treatment and a topotactic transformation via calcination. When these mesocrystals were used as the catalyst to produce trichlorosilane (TCS) via Si hydrochlorination reaction, they exhibited excellent catalytic performance with much increased Si conversion and TCS selectivity. In particular, the TCS yield was increased 19-fold than that of the catalyst-free process. The latter is the current industrial process. The efficiently catalytic property of these mesocrystals is attributed to the formation of well-defined nanoscale heterointerfaces that can effectively facilitate the charge transfer, and the generation of the compressive and tensile strain on CuO near the interfaces among different metal oxides. The synthetic approach developed here could be applicable to fabricate versatile complicated metal oxide mesocrystals as novel catalysts for various industrial chemical reactions.展开更多
In this work, we report a simple and inexpensive approach to synthesize effective multicomponent Cu-Cu2O-CuO catalysts for the Rochow process from industrial waste contact masses (WCMs). WCMs from the organosilane i...In this work, we report a simple and inexpensive approach to synthesize effective multicomponent Cu-Cu2O-CuO catalysts for the Rochow process from industrial waste contact masses (WCMs). WCMs from the organosilane industry were treated with acid followed by reduction with metallic iron powder. The obtained copper powder was then subjected to controlled oxidation in air at different temperatures, followed by ball milling. The orthogonal array approach was applied to optimize this process, and the stirring speed and pH were found to significantly affect the leaching ratio and copper yield, respectively. When used for the Rochow process, the optimized ternary Cu-Cu2O-CuO catalyst greatly enhanced the dimethyldichlorosilane selectivity and Si conversion compared with Cu-Cu2O-CuO catalysts prepared without ball milling, bare Cu catalysts, and Cu-Cu2O-CuO catalysts with different compositions. This could be attributed to their small particle size and the strong synergistic effect among the multiple components in the catalyst with the optimized composition.展开更多
基金supported by the National High Technology Research and Development Program of China(Grant No.2006AA11A189)Science and Technology Commission of Shanghai Municipality(Grant No.07DZ12036,and08DZ12064)Shanghai Pujiang Program(Grant No.08PJ1405900)
文摘The Ni-CeO2/Al2O3 catalysts with a nickel content of 15 wt% prepared via impregnating boehmite were found to be highly active and stable for methanation of carbon dioxide with hydrogen at a H2/CO2 molar ratio of 4. The effects of CeO2 content and reaction temperature on the performance of the Ni-CeO2/Al2O3 catalysts were studied in detail. The results showed that the catalytic performance was strongly dependent on the CeO2 content in Ni-CeO2/Al2O3 catalysts and that the catalysts with 2 wt% CeO2 had the highest catalytic activity among the tested ones at 350 ℃. The XRD and H2-TPR characterizations revealed that the addition of CeO2 decreased the reduction temperature by altering the interaction between Ni and Al2O3, and improved the reducibility of the catalyst. Preliminary stability test of 120 h on stream over the Ni-2CeO2/Al2O3 catalyst at 350 ℃ revealed that the catalyst was much better than the unpromoted one.
基金supported by the Natural Science Foundation of China(Grant No.51304082 and 51174133)the Natural Science Foundation of Jiangsu Province,China(Grant No.BK20130462)+1 种基金the Natural Science Foundation of the Jiangsu Higher Education Institutions of China(Grant No.12KJB450001)the Science and Technology Commission of Shanghai Municipality(Grant No.11ZR1412900)
文摘The catalyst function was achieved in two regions in an oxygen permeation membrane reactor: H2 dissociated and reacted with lattice oxygen or oxygen ions to form H20 near the membrane surface. The H20 formed could react with the residual CH4 away from the membrane surface area.
基金supported by Innovation Program of Shanghai Municipal Education Commission,the Major State Basic Research Development Program of China(No.2014CB643403)the National Science Fund for Distinguished Young Scholars(No.51225401,51574164)the Basic Major Research Program of Science and Technology Commission Foundation of Shanghai(No.14JC1491400)
基金National Key Basic Research Program of China(Grant No.2014CB339800)National Science Foundation of China(Grant No.61675145,61722509,61422509,61605143,61420106006,61735012,51677145)+1 种基金Program for Changjiang Scholars and Innovative Research Team in University(IRT)(Grant No.13033)Hebei Province Science Foundation(Grant No.F2015402156 and F2014402094)
文摘It is shown that active-tunable terahertz absorbers can be realized in a sandwich-structured system comprising an ultrathin dielectric film(polyimide) on a temperature-sensitive substrate(InSb) with a metal film on the back by utilizing the intrinsic carrier density(N) variation in InSb. When increasing the temperature from 250 to 320 K, N in InSb varied from ~5.50×1015 to ~2.98×1016 cm–3. Fixing the thickness of dielectric film with the value of 1.37 μm, the absorption peak shifted from 1.41 to 3.29 THz while keeping absorption higher than 99%. This active tunability can respond to even a slight temperature perturbation, and shows polarization insensitivity as well as high tolerance of incidence-angle(absorption peak can still exceed 90% even the incidence angle reaches 60°). Besides, the refractive index of polyimide(PI) has thermal stability at the terahertz range and the merit of good workability. These characteristics guarantee the stability of activetunable performance. The peculiarities and innovations of this proposal promise a wide range of high efficiency terahertz devices, such as thermal sensors, spatial light modulators(SLMs) and so on.
基金the National Natural Science Foundation of China(Nos.21878301,21978299,and 21908224)Z.Z.thanks the kind support of Guangdong Technion Israel Institute of Technology(GTTIT)for the collaboration.
文摘Mesocrystals, the non-classical crystals with highly ordered nanoparticle superstructures, have shown great potential in many applications because of their newly collective properties. However, there is still a lack of a facile and general synthesis strategy to organize and integrate distinct components into complex mesocrystals, and of reported application for them in industrial catalytic reactions. Herein we report a general bottom-up synthesis of CuO-based trimetallic oxide mesocrystals (denoted as CuO-M1Ox-M2Oy, where M1 and M2 = Zn, In, Fe, Ni, Mn, and Co) using a simple precipitation method followed by a hydrothermal treatment and a topotactic transformation via calcination. When these mesocrystals were used as the catalyst to produce trichlorosilane (TCS) via Si hydrochlorination reaction, they exhibited excellent catalytic performance with much increased Si conversion and TCS selectivity. In particular, the TCS yield was increased 19-fold than that of the catalyst-free process. The latter is the current industrial process. The efficiently catalytic property of these mesocrystals is attributed to the formation of well-defined nanoscale heterointerfaces that can effectively facilitate the charge transfer, and the generation of the compressive and tensile strain on CuO near the interfaces among different metal oxides. The synthetic approach developed here could be applicable to fabricate versatile complicated metal oxide mesocrystals as novel catalysts for various industrial chemical reactions.
基金The work was supported by the National Natural Science Foundation of China (grant number 21506224). Z.Z. is grateful for support from the Institute of Chemical and Engineering Sciences.
文摘In this work, we report a simple and inexpensive approach to synthesize effective multicomponent Cu-Cu2O-CuO catalysts for the Rochow process from industrial waste contact masses (WCMs). WCMs from the organosilane industry were treated with acid followed by reduction with metallic iron powder. The obtained copper powder was then subjected to controlled oxidation in air at different temperatures, followed by ball milling. The orthogonal array approach was applied to optimize this process, and the stirring speed and pH were found to significantly affect the leaching ratio and copper yield, respectively. When used for the Rochow process, the optimized ternary Cu-Cu2O-CuO catalyst greatly enhanced the dimethyldichlorosilane selectivity and Si conversion compared with Cu-Cu2O-CuO catalysts prepared without ball milling, bare Cu catalysts, and Cu-Cu2O-CuO catalysts with different compositions. This could be attributed to their small particle size and the strong synergistic effect among the multiple components in the catalyst with the optimized composition.