A series of K-doped Mn0.5Ce0.5Oδ （K-MCO） catalysts with three-dimensionally ordered macroporous （3DOM） structure and different K loadings were successfully synthesized using simple methods. These catalysts exhibi...A series of K-doped Mn0.5Ce0.5Oδ （K-MCO） catalysts with three-dimensionally ordered macroporous （3DOM） structure and different K loadings were successfully synthesized using simple methods. These catalysts exhibited well-defined 3DOM nanostructure, which consisted of extensive interconnecting networks of spherical voids. The effects of the calcination temperature and calcination time on the morphological characteristics and crystalline forms of the catalysts were systematically studied. The catalysts showed high catalytic activity for the combustion of soot. 3DOM 20% K-MCO-4h catalyst, in particular, showed the highest catalytic activity of all of the catalysts studied （e.g., Ts0 = 331 ~C and Smco2 = 95.3%）. The occurrence of structural and synergistic effects among the K, Mn, and Ce atoms in the catalysts was favorable for enhancing their catalytic activity towards the combustion of diesel soot. Furthermore, the temperatures required for the complete combustion of the soot （〈400 ℃） were well within the exhaust temperature range （175-400 ℃）, which means that the accumulated soot can be removed under the conditions of the diesel exhaust gas. These catalysts could therefore be used in numerous practical applications because they are easy to synthesize, exhibit high catalytic activity, and can be made from low cost materials.展开更多
Three-dimensional ordered macroporous (3DOM) La1?xKxNiO3 perovskite-type catalysts were successfully prepared by a colloidal crystal template method and characterized by scanning electron microscopy, transmission elec...Three-dimensional ordered macroporous (3DOM) La1?xKxNiO3 perovskite-type catalysts were successfully prepared by a colloidal crystal template method and characterized by scanning electron microscopy, transmission electron microscopy, high-resolution transmission electron microscopy, energy-dispersive X-ray scattering elemental mapping, X-ray diffraction, Raman and X-ray photoelectron spectroscopy, and temperature-programmed reduction of H2. Further, their catalytic activity in soot combustion was determined by temperature-programmed oxidation reaction. K substitution into the LaNiO3 lattice led to remarkably improved catalytic activity of this catalyst in soot combustion. Amongst various catalysts, La0.95K0.05NiO3 exhibited the highest activity in soot combustion (with its T50 and CO2 S values being 338 °C and 98.2%, respectively), which is comparable to the catalytic activities of Pt-based catalysts under the condition of poor contact between the soot and the catalyst. K-substitution improves the valence state of Ni and increases the number of oxygen vacancies, thereby leading to increased density of surface-active oxygen species. The active oxygen species play a vital role in catalyzing the elimination of soot. The perovskite-type La1?xKxNiO3 nanocatalysts with 3DOM structure without noble metals have potential for practical applications in the catalytic combustion of diesel soot particles.展开更多
The performance of catalysts used in after-treatment systems is the key factor for the removal of diesel soot,which is an important component of atmosphericfine particle emissions.Herein,three-dimensionally ordered ma...The performance of catalysts used in after-treatment systems is the key factor for the removal of diesel soot,which is an important component of atmosphericfine particle emissions.Herein,three-dimensionally ordered macroporous–mesoporous Ti_(x)Si+(1-x)O_(2)(3DOM-m Ti_(x)Si+(1-x)O_(2))and its supported MnO_(x)catalysts doped with different alkali/alkaline-earth metals(AMnO_(x)/3 DOM-m Ti_(0.7)Si_(0.3)O_(2)(A:Li,Na,K,Ru,Cs,Mg,Ca,Sr,Ba))were prepared by mesoporous template(P123)-assisted colloidal crystal template(CCT)and incipient wetness impregnation methods,respectively.Physicochemical characterizations of the catalysts were performed using scanning electron microscopy,X-ray diffraction,N_(2)adsorption–desorption,H_(2)temperature-programmed reduction,O_(2)temperature-programmed desorption,NO temperature-programmed oxidation,and Raman spectroscopy techniques;then,we evaluated their catalytic performances for the removal of diesel soot particles.The results show that the 3DOM-m Ti_(0.7)Si_(0.3)O_(2)supports exhibited a well-defined 3DOM-m nanostructure,and AMnO_(x)nanoparticles with 10–50 nm were evenly dispersed on the inner walls of the uniform macropores.In addition,the as-prepared catalysts exhibited good catalytic performance for soot combustion.Among the prepared catalysts,CsMnO_(x)/3DOM-m Ti_(0.7)Si_(0.3)O_(2)had the highest catalytic activity for soot combustion,with T10,T50,and T90(the temperatures corresponding to soot conversion rates of 10%,50%,and 90%)values of 285,355,and 393℃,respectively.The high catalytic activity of the CsMnO_(x)/3 DOM-m Ti_(0.7)Si_(0.3)O_(2)catalysts was attributed to their excellent low-temperature reducibility and homogeneous macroporous–mesoporous structure,as well as to the synergistic effects between Cs and Mn species and between CsMnO_(x)and the Ti_(0.7)Si_(0.3)O_(2)support.展开更多
A series of three‐dimensionally ordered macroporous(3DOM)SnO2‐based catalysts modified by the cations Ce4+,Mn3+,and Cu2+have been prepared by using a colloidal crystal templating method and tested for soot combustio...A series of three‐dimensionally ordered macroporous(3DOM)SnO2‐based catalysts modified by the cations Ce4+,Mn3+,and Cu2+have been prepared by using a colloidal crystal templating method and tested for soot combustion under loose contact condition.XRD and STEM mapping results confirm that all the secondary metal cations have entered the lattice matrix of tetragonal rutile SnO2 to form non‐continuous solid solutions,thus impeding crystallization and improving the surface areas and pore volumes of the modified catalysts.In comparison with regular SnO2 nanoparticles,the 3DOM SnO2 displays evidently improved activity,testifying that the formation of the 3DOM structure can anchor the soot particulates in the macro‐pores,which ensures that the contact of the soot particles with the active sites on the 3DOM skeleton is more easily formed,thus benefiting the target reaction.With the incorporation of the secondary metal cations,the activity of the catalyst can be further improved due to the formation of more abundant mobile oxygen species.In summary,these effects are believed to be the major factors responsible for the activity of the catalyst.展开更多
Three-dimensionally ordered（3DOM） macroporous phosphotungstic acid/SiO_2（HPW/SiO_2） materials were prepared by using colloidal crystal as templates and applied for oxidative desulfurization（ODS） of the model fue...Three-dimensionally ordered（3DOM） macroporous phosphotungstic acid/SiO_2（HPW/SiO_2） materials were prepared by using colloidal crystal as templates and applied for oxidative desulfurization（ODS） of the model fuel oil. The obtained HPW/SiO_2 materials were characterized through scanning electron microscopy, powder X-ray diffraction, N_2 sorption, and Fourier transform infrared spectroscopy. The results indicated that 3 DOM HPW/SiO_2 possessed hierarchical pore architectures which contained ordered macropores and disordered mesopores, with the Keggin type HPW embedded in the framework of pore structure. The removal rate of dibenzothiophene（DBT） could reach 100% under the optimum conditions, moreover. The performance was only slightly decreased for the regenerated catalyst after 7 cycles.展开更多
A versatile and effective method for incorporating functional groups on the pore wall of three-dimensionally ordered macroporous cross-linked polystyrene（3DOM CLPS） by hydrophilic spacer arm has been investigated.Th...A versatile and effective method for incorporating functional groups on the pore wall of three-dimensionally ordered macroporous cross-linked polystyrene（3DOM CLPS） by hydrophilic spacer arm has been investigated.The 3DOM CLPS with pore size 865 nm was prepared by sacrifice template method.The hydrophilic spacer arm（polyethylene glycol,molecular weight is 600） was grafted to the 3DOM CLPS via nucleophilic substitution reaction.The other side of active hydroxyl can be further converted into a lot of other functional groups.In this report,the chelating ligand 2-mercaptobenzothiazole（MBZ） group was introduced on the end of the PGE chain to evidence the versatile functionalization approach.The functionalized ordered macroporous materials were characterized by FT-IR,element analyzer,SEM.The results reveal that the pores were successfully bonded with 2-mercaptobenzothiazole groups via hydrophilic spacer arms and the original morphology of ordered macroporous materials were remained after functionalization.The MBZ group density is 0.052 mmol/m^2.The functionalized 3DOM CLPS are expected to application as heavy metal ions adsorbent.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
The silica opal templates were prepared from three silica colloids of different diameters of 230 nm, 500 nm and 1.5 mm by a filtration route. The large-scale stable opal template membranes after sintering the deposite...The silica opal templates were prepared from three silica colloids of different diameters of 230 nm, 500 nm and 1.5 mm by a filtration route. The large-scale stable opal template membranes after sintering the deposited SiO2 opal template can be successfully obtained by optimizing the pH value and NaCl concentration in silica colloidal solutions. The three-dimensionally ordered macroporous（3DOM） polyimide membranes without crack were fabricated by reproducing the structure of silica opal template. We prepared the pore-filling composite proton exchange membranes by filling the 3DOM structure with proton conducting organosilane sol. The result indicates that the composite membranes exhibit higher water uptake than pure filling organosilane gel. The proton conductivity increased with the increasing of pore cell in composite membranes.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
Macroporous magnetic poly(GMA-EGDMA-DVB) microspheres synthesized by suspension polymerization were used as supports for palladium catalyst.The results showed the novel magnetic catalyst can promote Heck reaction of a...Macroporous magnetic poly(GMA-EGDMA-DVB) microspheres synthesized by suspension polymerization were used as supports for palladium catalyst.The results showed the novel magnetic catalyst can promote Heck reaction of aryl halides with acrylic acid efficiently without an inert atmosphere.In addition,the novel catalyst can be conveniently recovered by applying an external magnet and reused at least five times without significant loss of its activity.展开更多
A series of macroporous CuO-ZnO-ZrO2 （CZZ） catalysts with different Zn/Zr ratios were successfully prepared by template method and characterized by X-ray diffraction （XRD）, N2 adsorption, reactive N2O adsorption, ...A series of macroporous CuO-ZnO-ZrO2 （CZZ） catalysts with different Zn/Zr ratios were successfully prepared by template method and characterized by X-ray diffraction （XRD）, N2 adsorption, reactive N2O adsorption, scanning electron microscopy （SEM）, H2 temperature-pro- grammed reduction （H2-TPR）, and transmission electron microscopy （TEM）. The activity of the catalysts was tested for methanol synthesis from CO2 hydrogenation. It is found that the increase in the Zn/Zr ratio could lead to the sintering of the catalysts, destroying the macroporous structure integrity. The macroporous CZZ catalysts own lower Zn/Zr ratio, exhibiting a better morphology and activity. For comparison, the conventional nonporous CZZ catalysts were also investigated. The results show that the CZZ catalysts with macroporous structure own smaller particles, higher CO2 conversion, and CH3OH yield. It reveals that the macroporous structure could inhibit the growth of the par- ticle size, and the special porous structure is favorable for diffusion and penetration of CO2, which could improve the catalytic activities.展开更多
Developing the alternative supported noble metal catalysts with low cost,high catalytic efficiency,and good resistance toward carbon dioxide and water vapor is critically demanded for the oxidative removal of volatile...Developing the alternative supported noble metal catalysts with low cost,high catalytic efficiency,and good resistance toward carbon dioxide and water vapor is critically demanded for the oxidative removal of volatile organic compounds(VOCs).In this work,we prepared the mesoporous chromia-supported bimetallic Co and Ni single-atom(Co_(1)Ni_(1)/meso-Cr_(2)O_(3))and bimetallic Co and Ni nanoparticle(Co_(NP)Ni_(NP)/mesoCr_(2)O_(3))catalysts adopting the one-pot polyvinyl pyrrolidone(PVP)-and polyvinyl alcohol(PVA)-protecting approaches,respectively.The results indicate that the Co_(1)Ni_(1)/meso-Cr_(2)O_(3)catalyst exhibited the best catalytic activity for n-hexane(C_(6)H_(14))combustion(T_(50%)and T_(90%)were 239 and 263℃ at a space velocity of 40,000 mL g^(-1)h^(-1);apparent activation energy and specific reaction rate at 260℃ were 54.7 kJ mol^(-1)and 4.3×10^(-7)mol g^(-1)_(cat)s^(-1),respectively),which was associated with its higher(Cr^(5+)+Cr^(6+))amount,large n-hexane adsorption capacity,and good lattice oxygen mobility that could enhance the deep oxidation of n-hexane,in which Ni_(1) was beneficial for the enhancements in surface lattice oxygen mobility and low-temperature reducibility,while Co_(1) preferred to generate higher contents of the high-valence states of chromium and surface oxygen species as well as adsorption and activation of n-hexane.n-Hexane combustion takes place via the Mars van Krevelen(MvK)mechanism,and its reaction pathways are as follows:n-hexane→olefins or 3-hexyl hydroperoxide→3-hexanone,2-hexanone or 2,5-dimethyltetrahydrofuran→2-methyloxirane or 2-ethyl-oxetane→acrylic acid→CO_x→CO_(2)and H_(2)O.展开更多
Developing bifunctional catalysts that increase both the OER and ORR kinetics and transport reactants with high efficiency is desirable. Herein, micro–meso-macroporous FeCo-N-C-X(denoted as "MFeCo-N-C-X", X...Developing bifunctional catalysts that increase both the OER and ORR kinetics and transport reactants with high efficiency is desirable. Herein, micro–meso-macroporous FeCo-N-C-X(denoted as "MFeCo-N-C-X", X represents Fe/Co molar ratio in bimetallic zeolite imidazole frameworks FeCo-ZIFs) catalysts derived from hierarchical M-FeCo-ZIFs-X was prepared. The micropores in M-FeCo-N-C-X have strong capability in O2 capture as well as dictate the nucleation and early-stage deposition of Li2O2,the mesopores provided a channel for the electrolyte wetting, and the macroporous structure promoted more available active sites when used as cathode for Li-O2 batteries. More importantly, M-Fe CoN-C-0.2 based cathode showed a high initial capacity(18,750 mAh g-1@0.1 A g-1), good rate capability(7900 m Ah g-1@0.5 A g-1), and cycle stability up to 192 cycles. Interestingly, the FeCo-N-C-0.2 without macropores suffered relatively poorer stability with only 75 cycles, although its discharge capacity was still as high as 17,200 mA h g-1(@0.1 A g-1). The excellent performance attributed to the synergistic contribution of homogeneous Fe, Co nanoparticles and N co-doping carbon frameworks with special micro–meso-macroporous structure. The results showed that hierarchical FeCo-N-C architectures are promising cathode catalysts for Li-O2 batteries.展开更多
Three-dimensional ordered macro/mesoporous carbon(3DOM/m-C)with high specific surface area was synthesized by colloid crystal template method with chemical activation by KOH and used as the adsorbent for removing mala...Three-dimensional ordered macro/mesoporous carbon(3DOM/m-C)with high specific surface area was synthesized by colloid crystal template method with chemical activation by KOH and used as the adsorbent for removing malachite green(MG)in aqueous solution.The microstructures of the adsorbents were characterized by FESEM,TEM and BET,and the effects of initial dye concentration,contact time,solution pH,and temperature on adsorption performance were investigated.The results show that the 3DOM/m-C exhibits extremely high adsorption capacity of 3541.1 mg/g within 2 h,which could be attributed to the novel ordered hierarchical structure with mesopores on three-dimensional ordered macroporous carbon walls.And the adsorption behavior conforms to the pseudo-second-order kinetic and Langmuir adsorption isotherm.3DOM/m-C can be recycled after being desorbed by absolute ethanol,and still maintains a high capacity of 2762.06 mg/g after 5 cycles.展开更多
Sodium-ion hybrid capacitor(SIHC)is one of the most promising alternatives for large-scale energy storage due to its high energy and power densities,natural abundance,and low cost.However,overcoming the imbalance betw...Sodium-ion hybrid capacitor(SIHC)is one of the most promising alternatives for large-scale energy storage due to its high energy and power densities,natural abundance,and low cost.However,overcoming the imbalance between slow Na^(+)reaction kinetics of battery-type anodes and rapid ion adsorption/desorption of capacitive cathodes is a significant challenge.Here,we propose the high-rate-performance NiS_(2)@OMGC anode material composed of monodispersed NiS_(2) nanocrystals(8.8±1.7 nm in size)and N,S-co-doped graphenic carbon(GC).The NiS_(2)@OMGC material has a three-dimensionally ordered macroporous(3DOM)morphology,and numerous NiS_(2) nanocrystals are uniformly embedded in GC,forming a core-shell structure in the local area.Ultrafine NiS_(2) nanocrystals and their nano-microstructure demonstrate high pseudocapacitive Na-storage capability and thus excellent rate performance(355.7 mAh/g at 20.0 A/g).A SIHC device fabricated using NiS_(2)@OMGC and commercial activated carbon(AC)cathode exhibits ultrahigh energy densities(197.4 Wh/kg at 398.8 W/kg)and power densities(43.9 kW/kg at 41.3 Wh/kg),together with a long life span.This outcome exemplifies the rational architecture and composition design of this type of anode material.This strategy can be extended to the design and synthesis of a wide range of high-performance electrode materials for energy storage applications.展开更多
Three-dimensionally ordered macro-/mesoporous alumina（3DOM Al2O3）-supported cobalt oxide and platinum nanocatalysts（xPt/yCo3O4/3DOM Al2O3,Pt mass fraction（x%）= 0-1.4%,Co3O4 mass fraction（y%） = 0-9.2%） were pre...Three-dimensionally ordered macro-/mesoporous alumina（3DOM Al2O3）-supported cobalt oxide and platinum nanocatalysts（xPt/yCo3O4/3DOM Al2O3,Pt mass fraction（x%）= 0-1.4%,Co3O4 mass fraction（y%） = 0-9.2%） were prepared using poly（methyl methacrylate） templating,incipient wetness impregnation and polyvinyl alcohol-protected reduction.The resulting xPt/yCo3O4/3DOM Al2O3 samples displayed a high-quality 3DOM architecture with macropores（180-200 nm in diameter） and mesopores（4-6 nm in diameter） together with surface areas in the range of 94 to 102m^2/g.Using these techniques,Co3O4 nanoparticles（NPs,18.3 nm） were loaded on the 3DOM Al2O3 surface,after which Pt NPs（2.3-2.5 nm） were uniformly dispersed on theyCo3O4/3DOM Al2O3.The1.3Pt/8.9Co3O4/3DOM Al2O3 exhibited the best performance for toluene oxidation,with a T（90%） value（the temperature required to achieve 90%toluene conversion） of 160 ℃ at a space velocity of20000 mL g^（-1） h^（-1）.It is concluded that the excellent catalytic performance of the 1.3Pt/8.9Co3O4/3DOM Al2O3 is owing to well-dispersed Pt NPs,the high concentration of adsorbed oxygen species,good low-temperature reducibility,and strong interaction between the Pt and Co3O4 NPs,as well as the unique bimodal porous structure of the support.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
Heterogeneous catalytic combustion provides a feasible technique for high efficient methane utilization.Perovskites ABO_3-type materials have received renewed attention as a potential alternative for noble metals supp...Heterogeneous catalytic combustion provides a feasible technique for high efficient methane utilization.Perovskites ABO_3-type materials have received renewed attention as a potential alternative for noble metals supported catalysts in catalytic methane combustion due to excellent hydrothermal stability and sulfur resistance. Recently, the emergence of nanostructured perovskite oxides（such as threedimensional ordered nanostructure, nano-array structure） with outstanding catalytic activity has further driven methane catalytic combustion research into spotlight. In this review, we summarize the recent development of nanostructured perovskite oxide catalysts for methane combustion, and shed some light on the rational design of high efficient nanostructured perovskite catalysts via lattice oxygen activation,lattice oxygen mobility and materials morphology engineering. The emergent issues needed to be addressed on perovskite catalysts were also proposed.展开更多
A series of 3DOM CeMnO3 perovskite catalysts were prepared by poly(methyl methacrylate)hardtemplating-excessive impregnation method at calcination temperature of x℃(x=600,700,800)and the heating rate of y℃/min(y=1,2...A series of 3DOM CeMnO3 perovskite catalysts were prepared by poly(methyl methacrylate)hardtemplating-excessive impregnation method at calcination temperature of x℃(x=600,700,800)and the heating rate of y℃/min(y=1,2,5,10).The samples were characterized by Brunauer-Emmett-Teller method,scanning electron microscopy,transmission electron microscopy,H2-temperature programmed reduction,X-ray photoelectron spectroscopy,X-ray diffraction,moreover,the effect of the calcination process on the catalytic activity of the samples were discussed by the catalytic combustion of toluene.The results show that the 3DOM CeMnO3 catalysts calcined at 600℃promote the formation of a perovskite structure,inhibit the reduction of the Mn4+species in the catalyst with high temperature.The catalyst expresses the complete macroporous structure,large specific surface area(38.8 m^(2)/g),higher adsorption oxygen concentration and Mn4+substance concentration,with a low T90%=172℃.By preparing the catalysts at different calcination heating rates,it can be concluded that the catalyst possesses a high concentration of adsorbed oxygen and a low reduction temperature and a large specific surface area(40.42 m^(2)/g)greatly promotes adsorption stage catalytic oxidation reaction and catalytic combustion of toluene at low temperature under the heating rate of 5℃/min.When the heating rate is 1℃/min,the catalyst has a complete macroporous structure(>250 nm),which is beneficial to the exchange of macromolecular substances during the catalytic reaction and the catalyst has a high concentration of lattice oxygen suitable for the catalysis of toluene in high temperature flue gas combustion.展开更多
A novel type of glucose sensor was fabricated based on a glucose oxidase(GOD)-N,N-dimethtylformamide(DMF)-[BMIm][BF4] composites modified three-dimensional ordered macroporous(3DOM) gold film electrode.The immobilized...A novel type of glucose sensor was fabricated based on a glucose oxidase(GOD)-N,N-dimethtylformamide(DMF)-[BMIm][BF4] composites modified three-dimensional ordered macroporous(3DOM) gold film electrode.The immobilized GOD exhibits a pair of well-defined reversible peaks in 50 mM pH 7.0 phosphate buffer solutions(PBS),which could be attributed to the redox of flavin adenine dinucleotide(FAD) in GOD.The research results show that ionic liquid([BMIm][BF4]),DMF and 3DOM gold film are crucial for GOD to exhibit a pair of stable and reversible peaks.It is believed that the large active area of 3DOM gold film can increase the amount of immobilized GOD.Simultaneously,the application of IL enhances the stability of GOD and facilitates the electron transfer between GOD and the electrode.The synergetic effect of DMF can help the GOD to maintain its bioactivity better.GOD immobilized on the electrode exhibits the favorable electrocatalytic property to glucose,and the prepared sensor has a linear range from 10 to 125 nM with a detection limit of 3.3 nM at a signal-to-noise ratio of 3σ.The apparent Km(Michaelis-Menten constant) for the enzymatic reaction is 0.018 mM.展开更多
基金supported by the National Natural Science Foundation of China(21177160,21303263,21477164)Beijing Nova Program(Z141109001814072)+1 种基金Specialized Research Fund for the Doctoral Program of High Education of China(20130007120011)the Science Foundation of China University of Petroleum-Beijing(2462013YJRC13,2462013BJRC003)~~
文摘A series of K-doped Mn0.5Ce0.5Oδ （K-MCO） catalysts with three-dimensionally ordered macroporous （3DOM） structure and different K loadings were successfully synthesized using simple methods. These catalysts exhibited well-defined 3DOM nanostructure, which consisted of extensive interconnecting networks of spherical voids. The effects of the calcination temperature and calcination time on the morphological characteristics and crystalline forms of the catalysts were systematically studied. The catalysts showed high catalytic activity for the combustion of soot. 3DOM 20% K-MCO-4h catalyst, in particular, showed the highest catalytic activity of all of the catalysts studied （e.g., Ts0 = 331 ~C and Smco2 = 95.3%）. The occurrence of structural and synergistic effects among the K, Mn, and Ce atoms in the catalysts was favorable for enhancing their catalytic activity towards the combustion of diesel soot. Furthermore, the temperatures required for the complete combustion of the soot （〈400 ℃） were well within the exhaust temperature range （175-400 ℃）, which means that the accumulated soot can be removed under the conditions of the diesel exhaust gas. These catalysts could therefore be used in numerous practical applications because they are easy to synthesize, exhibit high catalytic activity, and can be made from low cost materials.
基金supported by the National Natural Science Foundation of China(21673142)National Engineering Laboratory for Mobile Source Emission Control Technology(NELMS2017A05)+1 种基金PetroChina Innovation Foundation(2018D-5007-0505)Science Foundation of China University of Petroleum,Beijing(242017QNXZ02,2462018BJC005)~~
文摘Three-dimensional ordered macroporous (3DOM) La1?xKxNiO3 perovskite-type catalysts were successfully prepared by a colloidal crystal template method and characterized by scanning electron microscopy, transmission electron microscopy, high-resolution transmission electron microscopy, energy-dispersive X-ray scattering elemental mapping, X-ray diffraction, Raman and X-ray photoelectron spectroscopy, and temperature-programmed reduction of H2. Further, their catalytic activity in soot combustion was determined by temperature-programmed oxidation reaction. K substitution into the LaNiO3 lattice led to remarkably improved catalytic activity of this catalyst in soot combustion. Amongst various catalysts, La0.95K0.05NiO3 exhibited the highest activity in soot combustion (with its T50 and CO2 S values being 338 °C and 98.2%, respectively), which is comparable to the catalytic activities of Pt-based catalysts under the condition of poor contact between the soot and the catalyst. K-substitution improves the valence state of Ni and increases the number of oxygen vacancies, thereby leading to increased density of surface-active oxygen species. The active oxygen species play a vital role in catalyzing the elimination of soot. The perovskite-type La1?xKxNiO3 nanocatalysts with 3DOM structure without noble metals have potential for practical applications in the catalytic combustion of diesel soot particles.
基金supported by Key Research and Development Program of Ministry of Science and Technology of the People’s Republic of China(MOST)(No.2017YFE0131200)for collaboration between China and PolandNational Nature Science Foundation of China(NSFC)(Nos.22072095,U1908204,21761162016)+3 种基金General Projects of Liaoning Province Natural Fund(No.2019-MS-284)National Engineering Laboratory for Mobile Source Emission Control Technology(No.NELMS2018A04)University level innovation team of Shenyang Normal University,Major Incubation Program of Shenyang Normal University(No.ZD201901)supported by the Research Grants Council(RGC)of Hong Kong through NSFC/RGC Joint Research Scheme(No.N_CUHK451/17)。
文摘The performance of catalysts used in after-treatment systems is the key factor for the removal of diesel soot,which is an important component of atmosphericfine particle emissions.Herein,three-dimensionally ordered macroporous–mesoporous Ti_(x)Si+(1-x)O_(2)(3DOM-m Ti_(x)Si+(1-x)O_(2))and its supported MnO_(x)catalysts doped with different alkali/alkaline-earth metals(AMnO_(x)/3 DOM-m Ti_(0.7)Si_(0.3)O_(2)(A:Li,Na,K,Ru,Cs,Mg,Ca,Sr,Ba))were prepared by mesoporous template(P123)-assisted colloidal crystal template(CCT)and incipient wetness impregnation methods,respectively.Physicochemical characterizations of the catalysts were performed using scanning electron microscopy,X-ray diffraction,N_(2)adsorption–desorption,H_(2)temperature-programmed reduction,O_(2)temperature-programmed desorption,NO temperature-programmed oxidation,and Raman spectroscopy techniques;then,we evaluated their catalytic performances for the removal of diesel soot particles.The results show that the 3DOM-m Ti_(0.7)Si_(0.3)O_(2)supports exhibited a well-defined 3DOM-m nanostructure,and AMnO_(x)nanoparticles with 10–50 nm were evenly dispersed on the inner walls of the uniform macropores.In addition,the as-prepared catalysts exhibited good catalytic performance for soot combustion.Among the prepared catalysts,CsMnO_(x)/3DOM-m Ti_(0.7)Si_(0.3)O_(2)had the highest catalytic activity for soot combustion,with T10,T50,and T90(the temperatures corresponding to soot conversion rates of 10%,50%,and 90%)values of 285,355,and 393℃,respectively.The high catalytic activity of the CsMnO_(x)/3 DOM-m Ti_(0.7)Si_(0.3)O_(2)catalysts was attributed to their excellent low-temperature reducibility and homogeneous macroporous–mesoporous structure,as well as to the synergistic effects between Cs and Mn species and between CsMnO_(x)and the Ti_(0.7)Si_(0.3)O_(2)support.
基金the Natural Science Foundation of China(21567016,21503106)the Natural Science Foundation of Jiangxi Province(20171BAB213013)+3 种基金the Education Department Foundation of Jiangxi Province(KJLD14005)National Key Research and Development Program of China(2016YFC0209302)the Innovation Fund Designated for Graduate Students of Jiangxi Province(YC2015-B017)the Innovation Fund Designated for Undergraduate Students of China(201701035)~~
文摘A series of three‐dimensionally ordered macroporous(3DOM)SnO2‐based catalysts modified by the cations Ce4+,Mn3+,and Cu2+have been prepared by using a colloidal crystal templating method and tested for soot combustion under loose contact condition.XRD and STEM mapping results confirm that all the secondary metal cations have entered the lattice matrix of tetragonal rutile SnO2 to form non‐continuous solid solutions,thus impeding crystallization and improving the surface areas and pore volumes of the modified catalysts.In comparison with regular SnO2 nanoparticles,the 3DOM SnO2 displays evidently improved activity,testifying that the formation of the 3DOM structure can anchor the soot particulates in the macro‐pores,which ensures that the contact of the soot particles with the active sites on the 3DOM skeleton is more easily formed,thus benefiting the target reaction.With the incorporation of the secondary metal cations,the activity of the catalyst can be further improved due to the formation of more abundant mobile oxygen species.In summary,these effects are believed to be the major factors responsible for the activity of the catalyst.
基金the National Nature Science Foundation of China(No.21476177)
文摘Three-dimensionally ordered（3DOM） macroporous phosphotungstic acid/SiO_2（HPW/SiO_2） materials were prepared by using colloidal crystal as templates and applied for oxidative desulfurization（ODS） of the model fuel oil. The obtained HPW/SiO_2 materials were characterized through scanning electron microscopy, powder X-ray diffraction, N_2 sorption, and Fourier transform infrared spectroscopy. The results indicated that 3 DOM HPW/SiO_2 possessed hierarchical pore architectures which contained ordered macropores and disordered mesopores, with the Keggin type HPW embedded in the framework of pore structure. The removal rate of dibenzothiophene（DBT） could reach 100% under the optimum conditions, moreover. The performance was only slightly decreased for the regenerated catalyst after 7 cycles.
基金supported by National Natural Science Funds for Young Scholar(No.50903027)the Natural Science Foundation of Hebei Province(No.E2010000058)Education Department Science Research Plan of Hebei Province(No.2007307).
文摘A versatile and effective method for incorporating functional groups on the pore wall of three-dimensionally ordered macroporous cross-linked polystyrene（3DOM CLPS） by hydrophilic spacer arm has been investigated.The 3DOM CLPS with pore size 865 nm was prepared by sacrifice template method.The hydrophilic spacer arm（polyethylene glycol,molecular weight is 600） was grafted to the 3DOM CLPS via nucleophilic substitution reaction.The other side of active hydroxyl can be further converted into a lot of other functional groups.In this report,the chelating ligand 2-mercaptobenzothiazole（MBZ） group was introduced on the end of the PGE chain to evidence the versatile functionalization approach.The functionalized ordered macroporous materials were characterized by FT-IR,element analyzer,SEM.The results reveal that the pores were successfully bonded with 2-mercaptobenzothiazole groups via hydrophilic spacer arms and the original morphology of ordered macroporous materials were remained after functionalization.The MBZ group density is 0.052 mmol/m^2.The functionalized 3DOM CLPS are expected to application as heavy metal ions adsorbent.
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(Nos.20704004, 21074019)the Natural Science Foundation of Jilin Province, China(No.20101539)
文摘The silica opal templates were prepared from three silica colloids of different diameters of 230 nm, 500 nm and 1.5 mm by a filtration route. The large-scale stable opal template membranes after sintering the deposited SiO2 opal template can be successfully obtained by optimizing the pH value and NaCl concentration in silica colloidal solutions. The three-dimensionally ordered macroporous（3DOM） polyimide membranes without crack were fabricated by reproducing the structure of silica opal template. We prepared the pore-filling composite proton exchange membranes by filling the 3DOM structure with proton conducting organosilane sol. The result indicates that the composite membranes exhibit higher water uptake than pure filling organosilane gel. The proton conductivity increased with the increasing of pore cell in composite membranes.
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.
文摘Macroporous magnetic poly(GMA-EGDMA-DVB) microspheres synthesized by suspension polymerization were used as supports for palladium catalyst.The results showed the novel magnetic catalyst can promote Heck reaction of aryl halides with acrylic acid efficiently without an inert atmosphere.In addition,the novel catalyst can be conveniently recovered by applying an external magnet and reused at least five times without significant loss of its activity.
基金financially supported by the National Key Technologies Research & Development Program of China(No.2011BAC01B03)the National Natural Science Foundation of China(No.51304099)+1 种基金the Applied Basic Research Program of Yunnan Province(No.2013FZ035)the Testing and Analyzing Foundation of Kunming University of Science and Technology(No. 2010213)
文摘A series of macroporous CuO-ZnO-ZrO2 （CZZ） catalysts with different Zn/Zr ratios were successfully prepared by template method and characterized by X-ray diffraction （XRD）, N2 adsorption, reactive N2O adsorption, scanning electron microscopy （SEM）, H2 temperature-pro- grammed reduction （H2-TPR）, and transmission electron microscopy （TEM）. The activity of the catalysts was tested for methanol synthesis from CO2 hydrogenation. It is found that the increase in the Zn/Zr ratio could lead to the sintering of the catalysts, destroying the macroporous structure integrity. The macroporous CZZ catalysts own lower Zn/Zr ratio, exhibiting a better morphology and activity. For comparison, the conventional nonporous CZZ catalysts were also investigated. The results show that the CZZ catalysts with macroporous structure own smaller particles, higher CO2 conversion, and CH3OH yield. It reveals that the macroporous structure could inhibit the growth of the par- ticle size, and the special porous structure is favorable for diffusion and penetration of CO2, which could improve the catalytic activities.
基金supported by the National Natural Science Committee of China-Liaoning Provincial People's Government Joint Fund(U1908204)National Natural Science Foundation of China(21876006,21976009,and 21961160743)+2 种基金Foundation on the Creative Research Team Construction Promotion Project of Beijing Municipal Institutions(IDHT20190503)Natural Science Foundation of Beijing Municipal Commission of Education(KM201710005004)Development Program for the Youth Outstanding-Notch Talent of Beijing Municipal Commission of Education(CIT&TCD201904019)。
文摘Developing the alternative supported noble metal catalysts with low cost,high catalytic efficiency,and good resistance toward carbon dioxide and water vapor is critically demanded for the oxidative removal of volatile organic compounds(VOCs).In this work,we prepared the mesoporous chromia-supported bimetallic Co and Ni single-atom(Co_(1)Ni_(1)/meso-Cr_(2)O_(3))and bimetallic Co and Ni nanoparticle(Co_(NP)Ni_(NP)/mesoCr_(2)O_(3))catalysts adopting the one-pot polyvinyl pyrrolidone(PVP)-and polyvinyl alcohol(PVA)-protecting approaches,respectively.The results indicate that the Co_(1)Ni_(1)/meso-Cr_(2)O_(3)catalyst exhibited the best catalytic activity for n-hexane(C_(6)H_(14))combustion(T_(50%)and T_(90%)were 239 and 263℃ at a space velocity of 40,000 mL g^(-1)h^(-1);apparent activation energy and specific reaction rate at 260℃ were 54.7 kJ mol^(-1)and 4.3×10^(-7)mol g^(-1)_(cat)s^(-1),respectively),which was associated with its higher(Cr^(5+)+Cr^(6+))amount,large n-hexane adsorption capacity,and good lattice oxygen mobility that could enhance the deep oxidation of n-hexane,in which Ni_(1) was beneficial for the enhancements in surface lattice oxygen mobility and low-temperature reducibility,while Co_(1) preferred to generate higher contents of the high-valence states of chromium and surface oxygen species as well as adsorption and activation of n-hexane.n-Hexane combustion takes place via the Mars van Krevelen(MvK)mechanism,and its reaction pathways are as follows:n-hexane→olefins or 3-hexyl hydroperoxide→3-hexanone,2-hexanone or 2,5-dimethyltetrahydrofuran→2-methyloxirane or 2-ethyl-oxetane→acrylic acid→CO_x→CO_(2)and H_(2)O.
基金sponsored by the National Natural Science Foundation of China(21475021 and 21427807)the Fundamental Research Funds for the Central Universities(2242017 K41023)
文摘Developing bifunctional catalysts that increase both the OER and ORR kinetics and transport reactants with high efficiency is desirable. Herein, micro–meso-macroporous FeCo-N-C-X(denoted as "MFeCo-N-C-X", X represents Fe/Co molar ratio in bimetallic zeolite imidazole frameworks FeCo-ZIFs) catalysts derived from hierarchical M-FeCo-ZIFs-X was prepared. The micropores in M-FeCo-N-C-X have strong capability in O2 capture as well as dictate the nucleation and early-stage deposition of Li2O2,the mesopores provided a channel for the electrolyte wetting, and the macroporous structure promoted more available active sites when used as cathode for Li-O2 batteries. More importantly, M-Fe CoN-C-0.2 based cathode showed a high initial capacity(18,750 mAh g-1@0.1 A g-1), good rate capability(7900 m Ah g-1@0.5 A g-1), and cycle stability up to 192 cycles. Interestingly, the FeCo-N-C-0.2 without macropores suffered relatively poorer stability with only 75 cycles, although its discharge capacity was still as high as 17,200 mA h g-1(@0.1 A g-1). The excellent performance attributed to the synergistic contribution of homogeneous Fe, Co nanoparticles and N co-doping carbon frameworks with special micro–meso-macroporous structure. The results showed that hierarchical FeCo-N-C architectures are promising cathode catalysts for Li-O2 batteries.
基金Projects(U1802254,51871201)supported by the National Natural Science Foundation of ChinaProject(LY18E040003)supported by the Zhejiang Provincial Natural Science Foundation,China
文摘Three-dimensional ordered macro/mesoporous carbon(3DOM/m-C)with high specific surface area was synthesized by colloid crystal template method with chemical activation by KOH and used as the adsorbent for removing malachite green(MG)in aqueous solution.The microstructures of the adsorbents were characterized by FESEM,TEM and BET,and the effects of initial dye concentration,contact time,solution pH,and temperature on adsorption performance were investigated.The results show that the 3DOM/m-C exhibits extremely high adsorption capacity of 3541.1 mg/g within 2 h,which could be attributed to the novel ordered hierarchical structure with mesopores on three-dimensional ordered macroporous carbon walls.And the adsorption behavior conforms to the pseudo-second-order kinetic and Langmuir adsorption isotherm.3DOM/m-C can be recycled after being desorbed by absolute ethanol,and still maintains a high capacity of 2762.06 mg/g after 5 cycles.
基金supported by the National Natural Science Foundation of Tianjin(No.20JCQNJC01280)the National Natural Science Foundation of China(No.21905201)+1 种基金the support of the scientifi c research project from China Three Gorges Corporation(No.202103406)supported by Tohoku University and JSPS KAKENHI(No.JP16J06828).
文摘Sodium-ion hybrid capacitor(SIHC)is one of the most promising alternatives for large-scale energy storage due to its high energy and power densities,natural abundance,and low cost.However,overcoming the imbalance between slow Na^(+)reaction kinetics of battery-type anodes and rapid ion adsorption/desorption of capacitive cathodes is a significant challenge.Here,we propose the high-rate-performance NiS_(2)@OMGC anode material composed of monodispersed NiS_(2) nanocrystals(8.8±1.7 nm in size)and N,S-co-doped graphenic carbon(GC).The NiS_(2)@OMGC material has a three-dimensionally ordered macroporous(3DOM)morphology,and numerous NiS_(2) nanocrystals are uniformly embedded in GC,forming a core-shell structure in the local area.Ultrafine NiS_(2) nanocrystals and their nano-microstructure demonstrate high pseudocapacitive Na-storage capability and thus excellent rate performance(355.7 mAh/g at 20.0 A/g).A SIHC device fabricated using NiS_(2)@OMGC and commercial activated carbon(AC)cathode exhibits ultrahigh energy densities(197.4 Wh/kg at 398.8 W/kg)and power densities(43.9 kW/kg at 41.3 Wh/kg),together with a long life span.This outcome exemplifies the rational architecture and composition design of this type of anode material.This strategy can be extended to the design and synthesis of a wide range of high-performance electrode materials for energy storage applications.
基金supported by the National High Technology Research and Development Program of China(863 Program,2015AA034603)the National Natural Science Foundation of China(21377008)Foundation on the Creative Research Team Construction Promotion Project of Beijing Municipal Institutions
文摘Three-dimensionally ordered macro-/mesoporous alumina（3DOM Al2O3）-supported cobalt oxide and platinum nanocatalysts（xPt/yCo3O4/3DOM Al2O3,Pt mass fraction（x%）= 0-1.4%,Co3O4 mass fraction（y%） = 0-9.2%） were prepared using poly（methyl methacrylate） templating,incipient wetness impregnation and polyvinyl alcohol-protected reduction.The resulting xPt/yCo3O4/3DOM Al2O3 samples displayed a high-quality 3DOM architecture with macropores（180-200 nm in diameter） and mesopores（4-6 nm in diameter） together with surface areas in the range of 94 to 102m^2/g.Using these techniques,Co3O4 nanoparticles（NPs,18.3 nm） were loaded on the 3DOM Al2O3 surface,after which Pt NPs（2.3-2.5 nm） were uniformly dispersed on theyCo3O4/3DOM Al2O3.The1.3Pt/8.9Co3O4/3DOM Al2O3 exhibited the best performance for toluene oxidation,with a T（90%） value（the temperature required to achieve 90%toluene conversion） of 160 ℃ at a space velocity of20000 mL g^（-1） h^（-1）.It is concluded that the excellent catalytic performance of the 1.3Pt/8.9Co3O4/3DOM Al2O3 is owing to well-dispersed Pt NPs,the high concentration of adsorbed oxygen species,good low-temperature reducibility,and strong interaction between the Pt and Co3O4 NPs,as well as the unique bimodal porous structure of the support.
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.
基金the financial support from the Recruitment Program of Global Young Experts Start-up Fundthe Program of Introducing Talents of Discipline to Universities of China(111 Program, No. B17019)
文摘Heterogeneous catalytic combustion provides a feasible technique for high efficient methane utilization.Perovskites ABO_3-type materials have received renewed attention as a potential alternative for noble metals supported catalysts in catalytic methane combustion due to excellent hydrothermal stability and sulfur resistance. Recently, the emergence of nanostructured perovskite oxides（such as threedimensional ordered nanostructure, nano-array structure） with outstanding catalytic activity has further driven methane catalytic combustion research into spotlight. In this review, we summarize the recent development of nanostructured perovskite oxide catalysts for methane combustion, and shed some light on the rational design of high efficient nanostructured perovskite catalysts via lattice oxygen activation,lattice oxygen mobility and materials morphology engineering. The emergent issues needed to be addressed on perovskite catalysts were also proposed.
基金Project supported by Natural Science Foundation of Shandong Province(ZR2019MEE112)。
文摘A series of 3DOM CeMnO3 perovskite catalysts were prepared by poly(methyl methacrylate)hardtemplating-excessive impregnation method at calcination temperature of x℃(x=600,700,800)and the heating rate of y℃/min(y=1,2,5,10).The samples were characterized by Brunauer-Emmett-Teller method,scanning electron microscopy,transmission electron microscopy,H2-temperature programmed reduction,X-ray photoelectron spectroscopy,X-ray diffraction,moreover,the effect of the calcination process on the catalytic activity of the samples were discussed by the catalytic combustion of toluene.The results show that the 3DOM CeMnO3 catalysts calcined at 600℃promote the formation of a perovskite structure,inhibit the reduction of the Mn4+species in the catalyst with high temperature.The catalyst expresses the complete macroporous structure,large specific surface area(38.8 m^(2)/g),higher adsorption oxygen concentration and Mn4+substance concentration,with a low T90%=172℃.By preparing the catalysts at different calcination heating rates,it can be concluded that the catalyst possesses a high concentration of adsorbed oxygen and a low reduction temperature and a large specific surface area(40.42 m^(2)/g)greatly promotes adsorption stage catalytic oxidation reaction and catalytic combustion of toluene at low temperature under the heating rate of 5℃/min.When the heating rate is 1℃/min,the catalyst has a complete macroporous structure(>250 nm),which is beneficial to the exchange of macromolecular substances during the catalytic reaction and the catalyst has a high concentration of lattice oxygen suitable for the catalysis of toluene in high temperature flue gas combustion.
基金Supported by the National Natural Science Foundation of China (Grant No. 20635020)
文摘A novel type of glucose sensor was fabricated based on a glucose oxidase(GOD)-N,N-dimethtylformamide(DMF)-[BMIm][BF4] composites modified three-dimensional ordered macroporous(3DOM) gold film electrode.The immobilized GOD exhibits a pair of well-defined reversible peaks in 50 mM pH 7.0 phosphate buffer solutions(PBS),which could be attributed to the redox of flavin adenine dinucleotide(FAD) in GOD.The research results show that ionic liquid([BMIm][BF4]),DMF and 3DOM gold film are crucial for GOD to exhibit a pair of stable and reversible peaks.It is believed that the large active area of 3DOM gold film can increase the amount of immobilized GOD.Simultaneously,the application of IL enhances the stability of GOD and facilitates the electron transfer between GOD and the electrode.The synergetic effect of DMF can help the GOD to maintain its bioactivity better.GOD immobilized on the electrode exhibits the favorable electrocatalytic property to glucose,and the prepared sensor has a linear range from 10 to 125 nM with a detection limit of 3.3 nM at a signal-to-noise ratio of 3σ.The apparent Km(Michaelis-Menten constant) for the enzymatic reaction is 0.018 mM.
