To meet the growing emission of water contaminants,the development of new materials that enhance the efficiency of the water treatment system is urgent.Ordered mesoporous materials provide opportunities in environment...To meet the growing emission of water contaminants,the development of new materials that enhance the efficiency of the water treatment system is urgent.Ordered mesoporous materials provide opportunities in environmental processing applications due to their exceptionally high surface areas,large pore sizes,and enough pore volumes.These properties might enhance the performance of materials concerning adsorption/catalysis capability,durability,and stability.In this review,we enumerate the ordered mesoporous materials as adsorbents/catalysts and their modifications in water pollution treatment from the past decade,including heavy metals(Hg^(2+),Pb^(2+),Cd^(2+),Cr^(6+),etc.),toxic anions(nitrate,phosphate,fluoride,etc.),and organic contaminants(organic dyes,antibiotics,etc.).These contributions demonstrate a deep understanding of the synergistic effect between the incorporated framework and homogeneous active centers.Besides,the challenges and perspectives of the future developments of ordered mesoporous materials in wastewater treatment are proposed.This work provides a theoretical basis and complete summary for the application of ordered mesoporous materials in the removal of contaminants from aqueous solutions.展开更多
This paper proposes a new element-based multi-material topology optimization algorithm using a single variable for minimizing compliance subject to a mass constraint.A single variable based on the normalized elemental...This paper proposes a new element-based multi-material topology optimization algorithm using a single variable for minimizing compliance subject to a mass constraint.A single variable based on the normalized elemental density is used to overcome the occurrence of meaningless design variables and save computational cost.Different from the traditional material penalization scheme,the algorithm is established on the ordered ersatz material model,which linearly interpolates Young’s modulus for relaxed design variables.To achieve a multi-material design,the multiple floating projection constraints are adopted to gradually push elemental design variables to multiple discrete values.For the convergent element-based solution,the multiple level-set functions are constructed to tentatively extract the smooth interface between two adjacent materials.Some 2D and 3D numerical examples are presented to demonstrate the effectiveness of the proposed algorithm and the possible advantage of the multi-material designs over the traditional solid-void designs.展开更多
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
Three-dimensional（3D）ordered mesoporous MnO2 was prepared using KIT-6 mesoporous molecular sieves as a hard template.The material was used for catalytic oxidation of HCHO.The material has high surface areas and the ...Three-dimensional（3D）ordered mesoporous MnO2 was prepared using KIT-6 mesoporous molecular sieves as a hard template.The material was used for catalytic oxidation of HCHO.The material has high surface areas and the mesoporous characteristics of the template,with cubic symmetry（ia3d）.It consists of a β-MnO2 crystalline phase corresponding to pyrolusite,with a rutile structure.Transmission electron microscopy and X-ray photoelectron spectroscopy showed that the 3D-MnO2 catalyst has a large number of exposed Mn4＋ ions on the（110）crystal plane surfaces,with a lattice spacing of 0.311 nm; this enhances oxidation of HCHO.Complete conversion of HCHO to CO2 and H2O was achieved at 130 °C on 3D-MnO2; the same conversions on α-MnO2 and β-MnO2 nanorods were obtained at 140 and 180 °C,respectively,under the same conditions.The specific mesoporous structure,high specific surface area,and large number of surface Mn4＋ ions are responsible for the catalytic activity of 3D-MnO2 in HCHO oxidation.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
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
The magnetic and electronic properties of the geometrically frustrated triangular antiferromagnet CuCrO2 are investigated by first principles through density functional theory calculations within the generalized gradi...The magnetic and electronic properties of the geometrically frustrated triangular antiferromagnet CuCrO2 are investigated by first principles through density functional theory calculations within the generalized gradient approxi- mations （GGA）＋U scheme. The spin exchange interactions up to the third nearest neighbours in the ab plane as well as the coupling between adjacent layers are calculated to examine the magnetism and spin frustration. It is found that CuCrO2 has a natural two-dimensional characteristic of the magnetic interaction. Using Monte Carlo simulation, we obtain the Neel temperature to be 29.9 K, which accords well with the experimental value of 24 K. Based on non- collinear magnetic structure calculations, we verify that the incommensurate spiral-spin structure with （110） spiral plane is believable for the magnetic ground state, which is consistent with the experimental observations. Due to intra-layer geometric spin frustration, parallel helical-spin chains arise along the a, b, or a＋ b directions, each with a screw-rotation angle of about I20°. Our calculations of the density of states show that the spin frustration plays an important role in the change of d-p hybridization, while the spin-orbit coupling has a very limited influence on the electronic structure.展开更多
Ordered mesoporous silica were synthesized under different conditions:hydrothermal synthesis in basic medium,room temperature synthesis in acid medium and sol gel synthesis in neutral medium,and pore structure,specif...Ordered mesoporous silica were synthesized under different conditions:hydrothermal synthesis in basic medium,room temperature synthesis in acid medium and sol gel synthesis in neutral medium,and pore structure,specific surface area and pore size distribution of samples were studied and compared in detail by means of SAXRD,HRTEM,BET,FT IR.The results show that the mesopores in the samples obtained via above three methods all possess uniform hexagonal arrays in short range.Mesoporous silica obtained in acid medium possesses narrow pore size distribution centered around 1.24nm with specific surface area of 1220 m 2·g -1 ;Mesoporous silica obtained in basic medium by hydrothermal synthesis at 160℃ possesses narrow pore size distribution centered around 1.90nm with specific surface area of 542.8 m 2·g -1 ;and mesoporous silica obtained in neutral medium by sol gel synthesis possesses broader pore size distribution centered around 4.01nm,specific surface area of 485.0 m 2·g -1 .Therefore,ordered mesoporous silicas with different pore sizes can be prepared using various synthetic methods and conditions.After heat treatment,Si O Si bending vibration strengthens and the adsorption peak of asymmetrical Si O Si stretching vibration broadens,and the crosslinking and condensation reaction of silica skeleton strengthen, meanwhile the amount of active centers of hydroxyl group on the surface of mesopores may be influenced,thus chemical assembly activity of mesopores may also be influenced.展开更多
Nb_(3)Al nanoparticles were directly synthesized by metallothermic reduction process in the molten salts with mNbCl_(5)-nAlCl_(3) powders as raw materials and sodium as reducing reagent. The effects of different feedi...Nb_(3)Al nanoparticles were directly synthesized by metallothermic reduction process in the molten salts with mNbCl_(5)-nAlCl_(3) powders as raw materials and sodium as reducing reagent. The effects of different feeding material orders, soaking time, Nb content in raw materials, and 3NbCl_(5)-AlCl_(3) content in molten salts on the obtained Nb_(3)Al powder were discussed. The as-prepared samples were characterized by X-ray diffraction(XRD), scanning electron microscopy(SEM), and transmission electron microscopy(TEM). It is found that the only phase Nb_(3)Al nanoparticles are obtained by controlling the variation of the feeding material orders, soaking time, and Nb content in raw materials. And the morphologies of as-prepared nanoparticles change owning to different 3NbCl_(5)-AlCl_(3) contents in molten salts.展开更多
In this paper,SmCo6.9 Hf0.1 as-cast alloys and ribbons with the addition of either graphite（C） or carbon nanotubes（CNTs） were prepared by arc melting and melt-spinning,respectively.The effects of adding carbon on ...In this paper,SmCo6.9 Hf0.1 as-cast alloys and ribbons with the addition of either graphite（C） or carbon nanotubes（CNTs） were prepared by arc melting and melt-spinning,respectively.The effects of adding carbon on the structure and magnetic properties SmCo6.9 Hf0.1 were investigated by means of X-ray diffraction（XRD）,scanning electron microscopy（SEM）,transmission electron microscopy（TEM）,magnetic force microscopy（MFM） and vibrating sample magnetometer（VSM）.It was found that the microstructure and magnetic structure of SmCo6.9 Hf0.1 ribbons were changed obviously due to the introduction of C or CNTs,although their crystal structure was characterized as the same Sm（Co,Hf）7 single phase,no matter carbon was added or not.As a result,the magnetic properties of carbon-contained ribbons were enhanced in a certain degree.This was considered to be related to the refined equiaxed grains,small domain size and the pinning effect of C or CNTs-rich regions.The magnetic properties of SmCo6.9 Hf0.1（CNTs）0.05 ribbons reached Hc =12.5 kOe,Mr =57.0 emu/g and Mr/M2 T =0.788.展开更多
A β-zeolite/polystyrene composite material was synthesized by co-deposition of mono-disperse polystyrene spheres and nano β-zeolite particles in aqueous suspension on a vertical substrate. Macro-porous β-zeolite wa...A β-zeolite/polystyrene composite material was synthesized by co-deposition of mono-disperse polystyrene spheres and nano β-zeolite particles in aqueous suspension on a vertical substrate. Macro-porous β-zeolite was obtained after the polystyrene template was removed by calcination. The micro/macro-pore structure of the prepared β-zeolite was highly ordered. In comparison with other assembly methods, the co-deposition method could obtain a highly ordered macro-porous material with relatively large zeolite filling particles, and therefore the co-deposition of particles with different size is a promising method for the fabrication of macro-porous materials.展开更多
The characteristics of the strains induced by transformation and magnetic field in ascast Ni-Mn-Ga alloy were systematically investigated.It is found that internal stress and texture introduced during casting bring th...The characteristics of the strains induced by transformation and magnetic field in ascast Ni-Mn-Ga alloy were systematically investigated.It is found that internal stress and texture introduced during casting bring the anisotropy of temperature-induced strains.However,no anisotropy of field-induced strains is induced,and the internal stress and the texture modulate only the temperature dependence of field-induced strains.Large retardance of field-induced strains was observed,which indicates the rearrangement of martensitic variants as a competition process between the stress energy and Zeeman energy.The non-continuous field dependence of strain indicates the unstable microstructure during martensitic transformation.展开更多
Polycrystalline samples of pseudo-ternary intermetallic Nd3–xGdxCo11B4 （x=0,1,2,3） borides prepared by standard arc-melting were characterized by X-ray powder diffraction （XRPD）,magnetization and differential sca...Polycrystalline samples of pseudo-ternary intermetallic Nd3–xGdxCo11B4 （x=0,1,2,3） borides prepared by standard arc-melting were characterized by X-ray powder diffraction （XRPD）,magnetization and differential scanning calorimetry （DSC） measurements. The X-ray diffraction patterns indicated the hexagonal Ce3Co11B4-type structure with P6/mmm space group for each composition. The substitution of Gd for Nd led to a decrease of the unit-cell parameters a and the unit-cell volume V,while the unit-cell parameter c increased linearly. Magnetic measurements indicated that all samples were ordered magnetically below the Curie temperature. The Curie temperatures increased as Nd was substituted by Gd. The saturation magnetization at 4 K decreased upon the Gd substitution up to x=1,and then increased.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
This paper studies the normal state properties of itinerant electrons in a toy model, which is constructed according to the model for coexisting ferromagnetism and superconductivity proposed by Suhl [Suhl H 2001 Phys....This paper studies the normal state properties of itinerant electrons in a toy model, which is constructed according to the model for coexisting ferromagnetism and superconductivity proposed by Suhl [Suhl H 2001 Phys. Rev. Lett. 87 167007]. In this theory with ferromagnetic ordering based on localized spins, the exchange interaction J between conduction electrons and localized spin is taken as the pairing glue for s-wave superconductivity. It shows that this J term will first renormalize the normal state single conduction electron structures substantially. It finds dramatically enhanced or suppressed magnetization of itinerant electrons for positive or negative J. Singlet Cooper pairing can be ruled out due to strong spin polarisation in the J 〉 0 case while a narrow window for s-wave superconductivity is opened around some ferromagnetic J.展开更多
In this paper, the magnetic and transport properties in ABO3-type perovskite-like manganites as functions of the structure have been discussed from the viewpoints of A- and B-site doping, respectively. For the A-site ...In this paper, the magnetic and transport properties in ABO3-type perovskite-like manganites as functions of the structure have been discussed from the viewpoints of A- and B-site doping, respectively. For the A-site doping, two simple parameters, tolerance factor t and variance of the A-cation radius distribution s, can be used to characterize the magnetic/resistive phase diagram. For the B-site doping, the case is complicated due to the direct action to the center of double exchange. However, the dopant-size-induced local strain effect plays an important role in the physical properties besides the size mismatch between A- and B-site ions.展开更多
The effects of plastic deformation on the magnetic properties of austenite structure in an Fe-40% Ni-2 % Mn alloy is investigated by using Mossbauer spectroscopy and Differential Scanning Calorimetry （DSC） technique...The effects of plastic deformation on the magnetic properties of austenite structure in an Fe-40% Ni-2 % Mn alloy is investigated by using Mossbauer spectroscopy and Differential Scanning Calorimetry （DSC） techniques The morphology of the alloy has been obtained by using Scanning Electron Microscopy （SEM）. The magnetic behaviour of austenite state is ferromagnetic. After plastic deformation, a mixed magnetic structure including both paramagnet- ic and ferromagnetic states has been obtained at the room temperature. The volume fraction changes, the effective hyperfine fields of the ferromagnetic austenite phase and isomery shift values have also been determined by Mossbauer spectroscopy. The Curie point （Tc） and the Neel temperature （TN） have been investigated by means of DSC system for non-deformed and deformed Fe-Ni-Mn alloy. The plastic deformation of the alloy reduces the TN and enhances the paramagnetic character of austenitic Fe-Ni-Mn alloy.展开更多
Magnetic Mn1-xCuxFe2O4（x=0.2,0.5,0.8 and 1.0） nanoparticles were synthesized by single citrate precursor method.The samples were characterized by powder X-ray diffraction,vibrating sample magnetometry and electron p...Magnetic Mn1-xCuxFe2O4（x=0.2,0.5,0.8 and 1.0） nanoparticles were synthesized by single citrate precursor method.The samples were characterized by powder X-ray diffraction,vibrating sample magnetometry and electron paramagnetic resonance（EPR）.For samples with a low copper content（x0.5）,the copper ions have a tendency to occupy and substitute the Fe^3＋ at the tetrahedral（A） sites.For samples with a high copper content（x0.5）,most Cu^2＋ enter into the octahedral（B） sites.Transfer of Fe^3＋ from octahedral sites to tetrahedral sites leads to the decrease of the saturation magnetization.Maximum coercivity is observed for CuFe2O4 nanoparticles due to the strengthened magnetic anisotropy arisen from the Jahn-Teller effect of the octahedral copper ions.The dependence of magnetic properties of Mn0.8Cu0.2Fe2O4 nanoparticles on calcination temperature was investigated.The cation distribution in Mn0.8Cu0.2Fe2O4 is sensitive to the calcination temperature.展开更多
Single-atom catalysts(SACs)are attracting extensive attention due to their incredibly catalytic activity and selectivity,high utilization of metal atoms,and obvious cost reduction.The unique ordered porous materials(O...Single-atom catalysts(SACs)are attracting extensive attention due to their incredibly catalytic activity and selectivity,high utilization of metal atoms,and obvious cost reduction.The unique ordered porous materials(OPMs)are promising carriers for stabilizing single atoms due to their large surface areas and uniformly tunable pore sizes.Meantime,the geometric and electronic structures of single-atom metals can be tuned by the interaction between the single-atoms(SAs)and OPMs to enhance the catalytic activity of SACs.The SACs based on OPMs,such as zeolites,metal-organic frameworks,and ordered mesoporous materials,have been developing fast recently.Herein,we review recent advancements on structural feature,synthetic strategy,characterization technique,and catalytic applications of OPMs-based SACs.The opportunities and challenges about SAs/OPMs are also provided to develop the novel catalysts with superior catalytic performances in the future.展开更多
基金supported by the National Natural Science Foundation of China(52370041)National Natural Science Foundation of China(21976134 and 21707104)State Key Laboratory of Pollution treatment and Resource Reuse Foundation(NO.PCRRK21001).
文摘To meet the growing emission of water contaminants,the development of new materials that enhance the efficiency of the water treatment system is urgent.Ordered mesoporous materials provide opportunities in environmental processing applications due to their exceptionally high surface areas,large pore sizes,and enough pore volumes.These properties might enhance the performance of materials concerning adsorption/catalysis capability,durability,and stability.In this review,we enumerate the ordered mesoporous materials as adsorbents/catalysts and their modifications in water pollution treatment from the past decade,including heavy metals(Hg^(2+),Pb^(2+),Cd^(2+),Cr^(6+),etc.),toxic anions(nitrate,phosphate,fluoride,etc.),and organic contaminants(organic dyes,antibiotics,etc.).These contributions demonstrate a deep understanding of the synergistic effect between the incorporated framework and homogeneous active centers.Besides,the challenges and perspectives of the future developments of ordered mesoporous materials in wastewater treatment are proposed.This work provides a theoretical basis and complete summary for the application of ordered mesoporous materials in the removal of contaminants from aqueous solutions.
基金This work was supported by Hunan Provincial Innovation Foundation for Postgraduate(CX20190278)FJUT Scientific Research Foundation(GY-Z17015)Open Fund of Fujian Key Laboratory of Automotive Electronics and Electric Drive(KF-X19001).
文摘This paper proposes a new element-based multi-material topology optimization algorithm using a single variable for minimizing compliance subject to a mass constraint.A single variable based on the normalized elemental density is used to overcome the occurrence of meaningless design variables and save computational cost.Different from the traditional material penalization scheme,the algorithm is established on the ordered ersatz material model,which linearly interpolates Young’s modulus for relaxed design variables.To achieve a multi-material design,the multiple floating projection constraints are adopted to gradually push elemental design variables to multiple discrete values.For the convergent element-based solution,the multiple level-set functions are constructed to tentatively extract the smooth interface between two adjacent materials.Some 2D and 3D numerical examples are presented to demonstrate the effectiveness of the proposed algorithm and the possible advantage of the multi-material designs over the traditional solid-void designs.
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.
基金supported by the National Natural Science Foundation of China(21325731,21221004 and 51478241)~~
文摘Three-dimensional（3D）ordered mesoporous MnO2 was prepared using KIT-6 mesoporous molecular sieves as a hard template.The material was used for catalytic oxidation of HCHO.The material has high surface areas and the mesoporous characteristics of the template,with cubic symmetry（ia3d）.It consists of a β-MnO2 crystalline phase corresponding to pyrolusite,with a rutile structure.Transmission electron microscopy and X-ray photoelectron spectroscopy showed that the 3D-MnO2 catalyst has a large number of exposed Mn4＋ ions on the（110）crystal plane surfaces,with a lattice spacing of 0.311 nm; this enhances oxidation of HCHO.Complete conversion of HCHO to CO2 and H2O was achieved at 130 °C on 3D-MnO2; the same conversions on α-MnO2 and β-MnO2 nanorods were obtained at 140 and 180 °C,respectively,under the same conditions.The specific mesoporous structure,high specific surface area,and large number of surface Mn4＋ ions are responsible for the catalytic activity of 3D-MnO2 in HCHO oxidation.
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.
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Project supported by the National Natural Science Foundation of China (Grant No. 10874021)
文摘The magnetic and electronic properties of the geometrically frustrated triangular antiferromagnet CuCrO2 are investigated by first principles through density functional theory calculations within the generalized gradient approxi- mations （GGA）＋U scheme. The spin exchange interactions up to the third nearest neighbours in the ab plane as well as the coupling between adjacent layers are calculated to examine the magnetism and spin frustration. It is found that CuCrO2 has a natural two-dimensional characteristic of the magnetic interaction. Using Monte Carlo simulation, we obtain the Neel temperature to be 29.9 K, which accords well with the experimental value of 24 K. Based on non- collinear magnetic structure calculations, we verify that the incommensurate spiral-spin structure with （110） spiral plane is believable for the magnetic ground state, which is consistent with the experimental observations. Due to intra-layer geometric spin frustration, parallel helical-spin chains arise along the a, b, or a＋ b directions, each with a screw-rotation angle of about I20°. Our calculations of the density of states show that the spin frustration plays an important role in the change of d-p hybridization, while the spin-orbit coupling has a very limited influence on the electronic structure.
基金theNationalNaturalScienceFoundationofChina (No .50 2 72048)andtheNaturalScienceFoundationofHubeiProvince (No .2 0 0 1ABB0 76)
文摘Ordered mesoporous silica were synthesized under different conditions:hydrothermal synthesis in basic medium,room temperature synthesis in acid medium and sol gel synthesis in neutral medium,and pore structure,specific surface area and pore size distribution of samples were studied and compared in detail by means of SAXRD,HRTEM,BET,FT IR.The results show that the mesopores in the samples obtained via above three methods all possess uniform hexagonal arrays in short range.Mesoporous silica obtained in acid medium possesses narrow pore size distribution centered around 1.24nm with specific surface area of 1220 m 2·g -1 ;Mesoporous silica obtained in basic medium by hydrothermal synthesis at 160℃ possesses narrow pore size distribution centered around 1.90nm with specific surface area of 542.8 m 2·g -1 ;and mesoporous silica obtained in neutral medium by sol gel synthesis possesses broader pore size distribution centered around 4.01nm,specific surface area of 485.0 m 2·g -1 .Therefore,ordered mesoporous silicas with different pore sizes can be prepared using various synthetic methods and conditions.After heat treatment,Si O Si bending vibration strengthens and the adsorption peak of asymmetrical Si O Si stretching vibration broadens,and the crosslinking and condensation reaction of silica skeleton strengthen, meanwhile the amount of active centers of hydroxyl group on the surface of mesopores may be influenced,thus chemical assembly activity of mesopores may also be influenced.
基金the National Natural Science Foundation of China(Nos.50934001,21071014,51102015,and 51401004)the Fundamental Research Funds for the Central Universities(Nos.FRF-AS-11-002A,FRF-TP12-023A,and FRF-MP-09-006B)+2 种基金the National High Technology Research and Development Program of China(No.2012AA062302)the Program of the Co-Construction with Beijing Municipal Commission of Education of China(Nos.00012047 and 00012085)the Program for New Century Excellent Talents in University(No.NCET-11-0577)。
文摘Nb_(3)Al nanoparticles were directly synthesized by metallothermic reduction process in the molten salts with mNbCl_(5)-nAlCl_(3) powders as raw materials and sodium as reducing reagent. The effects of different feeding material orders, soaking time, Nb content in raw materials, and 3NbCl_(5)-AlCl_(3) content in molten salts on the obtained Nb_(3)Al powder were discussed. The as-prepared samples were characterized by X-ray diffraction(XRD), scanning electron microscopy(SEM), and transmission electron microscopy(TEM). It is found that the only phase Nb_(3)Al nanoparticles are obtained by controlling the variation of the feeding material orders, soaking time, and Nb content in raw materials. And the morphologies of as-prepared nanoparticles change owning to different 3NbCl_(5)-AlCl_(3) contents in molten salts.
基金supported by General Program from the National Natural Science Foundation of China(51271072)National Science Fund for Young(51301056)+1 种基金Key Program from the Science and Technology Research for Colleges and Universities in Hebei Province(ZH2011202)Hebei Natural Science Foundation of China(E2013202030)
文摘In this paper,SmCo6.9 Hf0.1 as-cast alloys and ribbons with the addition of either graphite（C） or carbon nanotubes（CNTs） were prepared by arc melting and melt-spinning,respectively.The effects of adding carbon on the structure and magnetic properties SmCo6.9 Hf0.1 were investigated by means of X-ray diffraction（XRD）,scanning electron microscopy（SEM）,transmission electron microscopy（TEM）,magnetic force microscopy（MFM） and vibrating sample magnetometer（VSM）.It was found that the microstructure and magnetic structure of SmCo6.9 Hf0.1 ribbons were changed obviously due to the introduction of C or CNTs,although their crystal structure was characterized as the same Sm（Co,Hf）7 single phase,no matter carbon was added or not.As a result,the magnetic properties of carbon-contained ribbons were enhanced in a certain degree.This was considered to be related to the refined equiaxed grains,small domain size and the pinning effect of C or CNTs-rich regions.The magnetic properties of SmCo6.9 Hf0.1（CNTs）0.05 ribbons reached Hc =12.5 kOe,Mr =57.0 emu/g and Mr/M2 T =0.788.
基金the National Basic Research Program of China （No. 2004CB217808） the National Natural Science Foundation of China （No. 20376046）.
文摘A β-zeolite/polystyrene composite material was synthesized by co-deposition of mono-disperse polystyrene spheres and nano β-zeolite particles in aqueous suspension on a vertical substrate. Macro-porous β-zeolite was obtained after the polystyrene template was removed by calcination. The micro/macro-pore structure of the prepared β-zeolite was highly ordered. In comparison with other assembly methods, the co-deposition method could obtain a highly ordered macro-porous material with relatively large zeolite filling particles, and therefore the co-deposition of particles with different size is a promising method for the fabrication of macro-porous materials.
基金Sponsored by National Natural Science Foundation of China(50001010)National High Technology Research Plan of China(AA200132722)
文摘The characteristics of the strains induced by transformation and magnetic field in ascast Ni-Mn-Ga alloy were systematically investigated.It is found that internal stress and texture introduced during casting bring the anisotropy of temperature-induced strains.However,no anisotropy of field-induced strains is induced,and the internal stress and the texture modulate only the temperature dependence of field-induced strains.Large retardance of field-induced strains was observed,which indicates the rearrangement of martensitic variants as a competition process between the stress energy and Zeeman energy.The non-continuous field dependence of strain indicates the unstable microstructure during martensitic transformation.
文摘Polycrystalline samples of pseudo-ternary intermetallic Nd3–xGdxCo11B4 （x=0,1,2,3） borides prepared by standard arc-melting were characterized by X-ray powder diffraction （XRPD）,magnetization and differential scanning calorimetry （DSC） measurements. The X-ray diffraction patterns indicated the hexagonal Ce3Co11B4-type structure with P6/mmm space group for each composition. The substitution of Gd for Nd led to a decrease of the unit-cell parameters a and the unit-cell volume V,while the unit-cell parameter c increased linearly. Magnetic measurements indicated that all samples were ordered magnetically below the Curie temperature. The Curie temperatures increased as Nd was substituted by Gd. The saturation magnetization at 4 K decreased upon the Gd substitution up to x=1,and then increased.
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 (Grant No. 10574063)
文摘This paper studies the normal state properties of itinerant electrons in a toy model, which is constructed according to the model for coexisting ferromagnetism and superconductivity proposed by Suhl [Suhl H 2001 Phys. Rev. Lett. 87 167007]. In this theory with ferromagnetic ordering based on localized spins, the exchange interaction J between conduction electrons and localized spin is taken as the pairing glue for s-wave superconductivity. It shows that this J term will first renormalize the normal state single conduction electron structures substantially. It finds dramatically enhanced or suppressed magnetization of itinerant electrons for positive or negative J. Singlet Cooper pairing can be ruled out due to strong spin polarisation in the J 〉 0 case while a narrow window for s-wave superconductivity is opened around some ferromagnetic J.
基金This work was supported by MOST of China (G19980613) NSFC (Nos. 29831010 & 20023005)+1 种基金 the Post-Doctoral Foundation of Chinathe Founder Foundation of PKU Corresponding author.
文摘In this paper, the magnetic and transport properties in ABO3-type perovskite-like manganites as functions of the structure have been discussed from the viewpoints of A- and B-site doping, respectively. For the A-site doping, two simple parameters, tolerance factor t and variance of the A-cation radius distribution s, can be used to characterize the magnetic/resistive phase diagram. For the B-site doping, the case is complicated due to the direct action to the center of double exchange. However, the dopant-size-induced local strain effect plays an important role in the physical properties besides the size mismatch between A- and B-site ions.
文摘The effects of plastic deformation on the magnetic properties of austenite structure in an Fe-40% Ni-2 % Mn alloy is investigated by using Mossbauer spectroscopy and Differential Scanning Calorimetry （DSC） techniques The morphology of the alloy has been obtained by using Scanning Electron Microscopy （SEM）. The magnetic behaviour of austenite state is ferromagnetic. After plastic deformation, a mixed magnetic structure including both paramagnet- ic and ferromagnetic states has been obtained at the room temperature. The volume fraction changes, the effective hyperfine fields of the ferromagnetic austenite phase and isomery shift values have also been determined by Mossbauer spectroscopy. The Curie point （Tc） and the Neel temperature （TN） have been investigated by means of DSC system for non-deformed and deformed Fe-Ni-Mn alloy. The plastic deformation of the alloy reduces the TN and enhances the paramagnetic character of austenitic Fe-Ni-Mn alloy.
基金Supported by the Development Program for Outstanding Young Teachers of Harbin Institute of Technology,China(No.HITQNJS2009004)the Opening Funding of the National Key Laboratory of Science and Technology on Advanced Composites in Special Environments,China(No. HIT.KLOF.2009029)
文摘Magnetic Mn1-xCuxFe2O4（x=0.2,0.5,0.8 and 1.0） nanoparticles were synthesized by single citrate precursor method.The samples were characterized by powder X-ray diffraction,vibrating sample magnetometry and electron paramagnetic resonance（EPR）.For samples with a low copper content（x0.5）,the copper ions have a tendency to occupy and substitute the Fe^3＋ at the tetrahedral（A） sites.For samples with a high copper content（x0.5）,most Cu^2＋ enter into the octahedral（B） sites.Transfer of Fe^3＋ from octahedral sites to tetrahedral sites leads to the decrease of the saturation magnetization.Maximum coercivity is observed for CuFe2O4 nanoparticles due to the strengthened magnetic anisotropy arisen from the Jahn-Teller effect of the octahedral copper ions.The dependence of magnetic properties of Mn0.8Cu0.2Fe2O4 nanoparticles on calcination temperature was investigated.The cation distribution in Mn0.8Cu0.2Fe2O4 is sensitive to the calcination temperature.
基金“Chu-Tian Scholar”Program of Hubei ProvinceNational Natural Science Foundation of China,Grant/Award Number:21874031+3 种基金Tencent Foundation through the XPLORER PRIZEthe Beijing Natural Science Foundation,Grant/Award Number:JQ18005the Fund of the State Key Laboratory of Solidification Processing in NWPU,Grant/Award Number:SKLSP202004the National Science Fund for Distinguished Young Scholars,Grant/Award Number:52025133。
文摘Single-atom catalysts(SACs)are attracting extensive attention due to their incredibly catalytic activity and selectivity,high utilization of metal atoms,and obvious cost reduction.The unique ordered porous materials(OPMs)are promising carriers for stabilizing single atoms due to their large surface areas and uniformly tunable pore sizes.Meantime,the geometric and electronic structures of single-atom metals can be tuned by the interaction between the single-atoms(SAs)and OPMs to enhance the catalytic activity of SACs.The SACs based on OPMs,such as zeolites,metal-organic frameworks,and ordered mesoporous materials,have been developing fast recently.Herein,we review recent advancements on structural feature,synthetic strategy,characterization technique,and catalytic applications of OPMs-based SACs.The opportunities and challenges about SAs/OPMs are also provided to develop the novel catalysts with superior catalytic performances in the future.
