N2O is a promising green propellant and exhibits great potential for satellite propulsion systems. It is difficult for catalytic decomposition, which is an important way to initiate the propulsion process, to occur at...N2O is a promising green propellant and exhibits great potential for satellite propulsion systems. It is difficult for catalytic decomposition, which is an important way to initiate the propulsion process, to occur at temperatures below 600 °C due to the high activation energy of N2O. In this work, we report an Ir supported on rutile TiO2(Ir/r-TiO2) catalyst which exhibits a fairly high activity for high-concentration N2O decomposition. HAADF-STEM, H2-TPR, and XPS results indicate that highly dispersed Ir particles and improved oxygen mobility on the Ir/r-TiO2 could facilitate the decompo-sition of N2O and desorption of the adsorbed oxygen. Bridge-bonded peroxide intermediates were observed with in-situ DRIFT and herein, a detailed decomposition route is proposed.展开更多
Three kinds of Pt/alumina catalysts were prepared by impregnation-hydrogen reduction, impregnation-hydrazine reduction and electroless plating methods. Their differences in the structures, specific areas and particle ...Three kinds of Pt/alumina catalysts were prepared by impregnation-hydrogen reduction, impregnation-hydrazine reduction and electroless plating methods. Their differences in the structures, specific areas and particle sizes were characterized by XRD, BET and TEM, respectively. Furthermore, their catalytic activities for the hydrogen iodide (HI) decomposition were evaluated in a fixed bed reactor. The results show that the catalyst 5%Pt/Al2O3 prepared by the electroless plating has the optimum catalytic properties for HI decomposition owing to the high dispersion of the platinum nano-particles (〈5 nm) on the alumina supports.展开更多
Catalytic decomposition of methylene chloride in air below 300℃ was studied. Sulfated titania was very effective in converting 959ppm methylene chloride selectively to CO, C02 and HCl. Complete decomposition of methy...Catalytic decomposition of methylene chloride in air below 300℃ was studied. Sulfated titania was very effective in converting 959ppm methylene chloride selectively to CO, C02 and HCl. Complete decomposition of methylene chloride was achieved at low temperature (275℃ ). It was found that the acidic property of catalyst was a determinant factor for the catalytic activity. The presence of water vapor in the feed stream remarkably reduced the catalytic activity, which could be due to the blockage of acidic sites on the surface of catalyst by water molecules. A bifunctional catalyst comprising copper oxide was developed to improve the selectivity of catalytic oxidation , which indicated that copper oxide can promote the deep oxidation of methylene chloride. The crystal form of TiO2 imposes an important influence upon the catalytic oxidation.展开更多
A new dual-composition catalyst based on Ni-Mo/MgO with high efficiency of producing carbon nanotubes (CNTs) from methane was reported recently. In the present article, with this type of catalyst, the impact of such...A new dual-composition catalyst based on Ni-Mo/MgO with high efficiency of producing carbon nanotubes (CNTs) from methane was reported recently. In the present article, with this type of catalyst, the impact of such experimental parameters as reaction temperature, reaction time, concentration of H2, flow rate ratio of CH4 to H2 on yield and graphitization were investigated, leading to the following optimal growth conditions: reaction time 60min, reaction temperature 900℃, CH4:H2 about 100:20mL/min, under which high-yield multi-walled CNTs bundles were synthesized. Raman measurement indicated that the as-synthesized product was well-graphitized, and the purity was estimated over 95% by TG-DSC analysis. In terms of the above results, an explanation of high-efficiency formation of CNTs bundles and the co-catalysis mechanism of Ni-Mo/MgO were suggested. 2007 Chinese Societv of Particuology and Institute of Process Engineering, Chinese Academy of Sciences. Published by Elsevier B.V.展开更多
A new energetic complex,[Co(3,3?-Hbpt)(Htm)]·H_2O(1,3,3?-Hbpt = 3,5-bis(3-pyridyl)-1H-1,2,4-triazole and H_3tm = trimesic acid),has been synthesized by hydrothermal reactions and characterized by single...A new energetic complex,[Co(3,3?-Hbpt)(Htm)]·H_2O(1,3,3?-Hbpt = 3,5-bis(3-pyridyl)-1H-1,2,4-triazole and H_3tm = trimesic acid),has been synthesized by hydrothermal reactions and characterized by single-crystal X-ray diffraction,elementary analysis,IR spectroscopy,thermogravimetric analysis and X-ray powder diffraction. Single-crystal X-ray diffraction indicates that the complex belongs to triclinic system,space group P 1 with a = 10.0911(1),b = 10.2573(1),c = 10.6393(1) ?,α = 103.793(2),β = 101.041(2),γ = 107.918(3)o,V = 974.9(2) ?~3,Z = 2,D_c = 1.732 g·cm-3,μ = 0.941 mm^(-1),M_r = 508.31,F(000) = 518,the final R = 0.0523 and wR = 0.0935 with I 〉 2σ(I). In the title complex,Co(Ⅱ) ions are connected by Htm2-anions generating 1D ladder-like chains which are linked by 3,3?-Hbpt to form 1D cages. In addition,the thermal decomposition of ammonium perchlorate(AP) with complex 1 was explored by differential scanning calorimetry(DSC). AP is completely decomposed in a shorter time in the presence of complex 1,and the decomposition heat of the mixture is 2.531 kJ·g^(-1),significantly higher than that of pure AP. By Kissinger's method,the ratio of Ea/ln(A) is 11.05 for the mixture,which indicates that complex 1 shows good catalytic activity toward the AP decomposition.展开更多
A series of mixed oxide catalysts with different composition of Co-M-Al and Co-M-Ce- Al (M=Zn, Ni, Cu) were prepared by co-precipitation method from hydrotalcite-like compounds. The experimental results revealed the...A series of mixed oxide catalysts with different composition of Co-M-Al and Co-M-Ce- Al (M=Zn, Ni, Cu) were prepared by co-precipitation method from hydrotalcite-like compounds. The experimental results revealed the catalytic activity of Co-Ni-Al is slightly higher than that of Co-Zn-Al and much higher than that of Co-Cu-Al for direct decomposition of N2O. Moreover, addition of small amounts of Ce02 improved the catalytic activity signif- icantly and made the decomposition temperatures at which the N2O conversion was 50% and 90% (T50 and Tgo) both decreased 80 ℃ than those of Co-M-Al catalysts without CeO2 added. Further, potassium-load also promoted the catalytic activity, and the decomposi- tion temperatures of T50 and T90 both decreased approximately 50 ℃. It is significant for decomposing N2O from industries and reducing carbon emission from atmosphere.展开更多
It has been generally unclear over the mechanism of inhibitory influence of silicate on structural rearrangement or solely physical adsorption onto manganese dioxide (MnO2) about the decomposition of hydrogen peroxi...It has been generally unclear over the mechanism of inhibitory influence of silicate on structural rearrangement or solely physical adsorption onto manganese dioxide (MnO2) about the decomposition of hydrogen peroxide (H2O2). Consequently, several experiments were carried out by using MnO2 as a catalyst for the decomposition of H2O2 in a concentration series under certain concentrations of silicates. The silicates were analyzed by using a molybdenum blue colorimetric method. The results showed that the determination of silicates was inhibited by H2O2, whose inhibitory effect was greatly increased by increasing its concentration, but not limited by pH. SEM-EDX (scanning electron microscopy-energy dispersive x-ray spectrometry) results showed that the adsorption of silicates onto the surface of MnO2 was not purely via a structural rearrangement, with increasing Mn atoms protruding on the outer surface by covering oxygen and silicon atoms. XRD (X-ray diffraction) and FTIR (Fourier transform infrared) spectra results further revealed no significant total crystal structural changes in MnO2 after the adsorption of silicates, but only a small shift of 0.21° at 2e from 56.36° to 56.15° , and a FTIR vibration showed at around 1 050 cm-1. The results, therefore, showed that silicate adsorption onto MnO2 took place via both surface adsorption and structural rearrangement by interfacial reaction.展开更多
The catalytic hydrolysis of dichlorodifluoromethane (CFC-12) was investigated over solid acid Ti(SO_4)_2. The catalytic activity decreased with the calcination temperature. When space velocity was 6 1 h^(-1) g-cat^(-1...The catalytic hydrolysis of dichlorodifluoromethane (CFC-12) was investigated over solid acid Ti(SO_4)_2. The catalytic activity decreased with the calcination temperature. When space velocity was 6 1 h^(-1) g-cat^(-1). the CPC-12 conversion at 310C over Ti(SO_4)_2 calcined at 350C remained about 98.5% during 360 h on stream. and the selectivity to by-products remained zero. The findings enlarged the scope of traditional catalyst systems for the CFCs decomposition.展开更多
Ammonium dinitramide(ADN)based liquid monopropellants have been identified as environmentally benign substitutes for hydrazine monopropellant.However,new catalysts are to be developed for making ADN monopropellants co...Ammonium dinitramide(ADN)based liquid monopropellants have been identified as environmentally benign substitutes for hydrazine monopropellant.However,new catalysts are to be developed for making ADN monopropellants cold-start capable.In the present study,performance of Co and Ba doped CuCr_2O_4 nanocatalysts prepared by hydrothermal method was evaluated on the decomposition of aqueous ADN solution and ADN liquid monopropellant(LMP103X).The catalysts were characterized by PXRD(Powder X-ray Diffraction),FTIR(Fourier Transform Infrared spectroscopy),SEM(Scanning Electron Microscopy),TEM(Transmission Electron Microscopy),EDS(Energy Dispersive X-ray Spectroscopy),and XPS(X-ray Photoelectron Spectroscopy).The nanosize was confirmed by SEM and TEM,while the nanoflake morphology was confirmed by the SEM analysis.Further,we obtained the elemental composition from the EDS analysis.We investigated the catalytic activity of the catalysts by thermogravimetric(TG)analysis and the developed catalysts lowered the decomposition temperature of ADN monopropellant by about 55℃.The XPS analysis confirmed the presence of metal ions with different chemical states.Apparently,increase in the surface area of the catalysts and the mixed active sites as well as the development of oxygen vacancy on the catalyst surface introduced by metal doping are influencing the decomposition temperature of ADN samples.展开更多
The catalytic reaction of NO with CO and decomposition of NO over metal modified ACFs were investigated and compared with other carriers supported catalysts. It is demonstrated that Pd/ACF and Pd/Cu/ACF have high cata...The catalytic reaction of NO with CO and decomposition of NO over metal modified ACFs were investigated and compared with other carriers supported catalysts. It is demonstrated that Pd/ACF and Pd/Cu/ACF have high catalytic activity for the reaction of NO/CO, while Pt/ACF, Pt/Cu/ACF and Co/Cu/ACF have very low catalytic activity in similar circumstance. Pd-modified ACF possesses high catalytic decomposition of NO at 300℃. Pd/CB and Pd/GAC present good catalytic decomposition ability for NO only at low flowrate. Pd/G, Pd/ZMS and Pd/A however, do not show any catalytic activity for NO decomposition even at 400℃. Catalytic temperature, NO flowrate and loading of metal components affect the decomposition rate of NO. The coexistence of Cu with Pd on Cu/Pd/ACF leads to crystalline of palladium to more unperfected so as to that increase the catalytic activity.展开更多
Numerous researchers in the energy field are engaged in a competitive race to advance hydrogen as a clean and environmentally friendly fuel.Studies have been conducted on the different aspects of hydrogen,including it...Numerous researchers in the energy field are engaged in a competitive race to advance hydrogen as a clean and environmentally friendly fuel.Studies have been conducted on the different aspects of hydrogen,including its production,storage,transportation and utilization.The catalytic methane decomposition technique for hydrogen production is an environmentally friendly process that avoids generating carbon dioxide gas,which contributes to the greenhouse effect.Catalysts play a crucial role in facilitating rapid,cost-effective and efficient production of hydrogen using this technique.In this study,reactive molecular dynamics simulations were employed to examine the impact of Pt_(7) cluster decoration on the surface of a Ni(110)catalyst,referred to as Pt_(7)-Ni(110),on the rates of methane dissociation and molecular hydrogen production.The reactive force field was employed to model the atomic interactions that enabled the formation and dissociation of chemical bonds.Our reactive molecular dynamics simulations using the Pt_(7)-Ni(110)catalyst revealed a notable decrease in the number of methane molecules,specifically~11.89 molecules per picosecond.The rate was approximately four times higher than that of the simulation system utilizing a Ni(110)catalyst and approximately six times higher than that of the pure methane,no-catalyst system.The number of hydrogen molecules generated during a simulation period of 150000 fs was greater on the Pt_(7)-Ni(110)surface than in both the Ni(110)and pure methane systems.This was due to the presence of numerous dissociated hydrogen atoms on the Pt_(7)-Ni(110)surface.展开更多
The preparation of immobilizing-catalysts for decomposing ozone by using dipping method was studied. XRD, XPS and TEM were used to characterize the catalysts. The three kinds of catalysts were selected preferentially,...The preparation of immobilizing-catalysts for decomposing ozone by using dipping method was studied. XRD, XPS and TEM were used to characterize the catalysts. The three kinds of catalysts were selected preferentially, and their catalytic activities were investigated. The results showed that the catalyst with activated carbon dipping acetate(active components are Mn:Cu=3:2, active component proportion in catalyst is 15%, calcination temperature is 200℃) has the best catalytic activity for ozone decomposing. One gram of catalyst can decompose 17.6 g ozone at initial ozone concentration of 2.5 g/m 3 and the residence time in reactor of 0.1 s. The experimental results also indicated that humidity of reaction system had negative effect on catalytic activity.展开更多
Intrinsic data of N2O catalytic decomposition over a K-promoted Co-Mn-Al mixed oxide prepared by the thermal treatment of a layered double hydroxide was used for the design of a pilot reactor for the abatement of N2O ...Intrinsic data of N2O catalytic decomposition over a K-promoted Co-Mn-Al mixed oxide prepared by the thermal treatment of a layered double hydroxide was used for the design of a pilot reactor for the abatement of N2O emissions from the off-gases in HNO3 production.A pseudo-homogeneous one-dimensional model of an ideal plug flow reactor under an isothermal regime(450°C)was used for reactor design.A catalyst particle diameter of 3 mm is a compromise size because increasing the size of the catalyst particle leads to a decrease in the reaction rate because of an internal diffusion limitation,and particles with a smaller diameter cause a large pressure drop.A catalyst bed of 11.5 m 3 was estimated for the target N2O conversion of 90%upon the treatment of 30000 m 3 /h of exhaust gas(0.1 mol%N2O,0.005 mol% NO,0.9 mol%H2O,5 mol%O2)at 450°C and 130 kPa.展开更多
To control contamination of flue gas emission NOx, the author mixcd method of preparing new magnesia base catalyst and researched on denitrificating fine gas by directness catalytic decomposition. Usually removal rate...To control contamination of flue gas emission NOx, the author mixcd method of preparing new magnesia base catalyst and researched on denitrificating fine gas by directness catalytic decomposition. Usually removal rate of NO is regarded on the main evaluation criteria. The author analyzed calcination temperature of catalyzer manufacturing process, the temperature of flue gas desorption tower, bed height and efficiency denitrification of NO concentration. And discussed the result of both denitrate lore-and-aft of FT-IR and XRD. The experiment indicates that magnesia base catalyst is available to directness catalytic decomposition denitrificate flue gas. Through denitrification rate is from 85% to 95%. The ingredient of magnesia base catalyst is made from magnesia, firming agent, addition agent. Height denitration bed was 4 cm- 5 cm, deuitration reaction temperature is 130℃-170℃, through the analyses above, presumed that magnesia base catalyst exist activating of vice, and analyzed this vice preliminarily.展开更多
Given their unique and excellent properties,metal-organic frameworks(MOFs)materials have been used in many scientific fields.EMOFs use energetic materials as ligands,which can provide part of the energy for the system...Given their unique and excellent properties,metal-organic frameworks(MOFs)materials have been used in many scientific fields.EMOFs use energetic materials as ligands,which can provide part of the energy for the system while catalyzing ammonium perchlorate.The energetic material 1.1'-dihydroxyazotetrazole(H_(2)AzTO),as a high-energy nitrogen-rich material,was selected as a ligand.Five kinds of La^(3+),Ce^(3+),Pr^(3+),Nd^(3+),and Sm^(3+)lanthanide EMOFs were synthesized and obtained.Single crystal X-ray diffraction tests were conducted to obtain the crystal structures of EMOFs 1-5,which indicate that they have similar crystal structures.The thermal stabilities of EMOFs 1-5,which are obtained by differential scanning calorimetry(DSC)tests,are improved compa red with that of the ligand.The results of thermicdecomposition of ammonium perchlorate(AP)and AP mixtures with 10 wt%EMOFs 1-5 show that except for AP mixed with 10 wt%co mpound 2,the high-temperature decomposition peak tempe rature of AP mixed with other compounds is significantly advanced(up to 59.3-88.3 K),and the decomposition of AP is continuous and violent.EMOFs 3-5 have good application prospects for the catalytic thermicdecomposition of AP.展开更多
An alumina-supported cobalt aerogel catalyst prepared from a sol-gel and a supercritical drying method was used in the catalytic decomposition of methane. The physical-chemical properties of the catalyst were characte...An alumina-supported cobalt aerogel catalyst prepared from a sol-gel and a supercritical drying method was used in the catalytic decomposition of methane. The physical-chemical properties of the catalyst were characterized and its activity for methane decomposition was investigated. The effects of calcination and reaction temperatures on the activity of the catalyst and the morphology of the carbon nanotubes produced were discussed. A CoAl2O4 spinel structure formed in the calcined catalyst. The quantity of the nanotubes produced in the reaction increases with the amount of cobalt in the reduced catalyst. A higher reaction temperature leads to a higher reaction rate, though faster deactivation of the catalyst occurs with the change. The carbon nanotubes grown on the catalyst have smooth walls and uniform di-ameter distribution.展开更多
Magnetic TS-1 was synthesized thesis and solvent vaporation method. The with nanosized nickelferrite particles prepared samples were characterized as nuclei via the hydrothermal syn- with N2 adsorption-desorption iso-...Magnetic TS-1 was synthesized thesis and solvent vaporation method. The with nanosized nickelferrite particles prepared samples were characterized as nuclei via the hydrothermal syn- with N2 adsorption-desorption iso- therms, FTIR spectrometry, Raman spectrometry, X-ray diffraction, Ultraviolet-visible spectroscopy and Vibrating sample magnetometry. The results show that the composite obtained was composed of TS-1 with MFI structure and NiFe204 with spinel structure, its specific surface area was about 316 m2/g, pore volume was 0.12 cm3/g and pore size distribution was in the range of 0.5-0.7 nm. The catalytic activity of the composite was also investigated by its catalyzing the decomposition of rhodamine B oxidized by H2O2 in aqueous solution. In this case Rhodamine B pollutant could be completely degraded within 150 min. Magnetic TS-1 exhibited high photocatalytic efficiency and super paramagnetic nature for cleaning polluted water with the help of magnetic separation.展开更多
Three groups of cobalt mixed oxide catalysts(Mg/Zn-Co, Mg/Zn-Ce-C, K/Na-Mg/Zn-Ce-Co)were prepared by sol-gel or impregnation methods. The synergistic effects of transition metal, rare earth metal and alkali metal on...Three groups of cobalt mixed oxide catalysts(Mg/Zn-Co, Mg/Zn-Ce-C, K/Na-Mg/Zn-Ce-Co)were prepared by sol-gel or impregnation methods. The synergistic effects of transition metal, rare earth metal and alkali metal on cobalt mixed catalysts for nitrous oxide(N2O)decomposing to N2 and O2were investigated. The experimental results revealed that the catalytic activity for N2 O decomposition was promoted as Co2+was replaced partially by Zn2+/Mg2+, moreover, the characterization analysis by XRD and XPS showed that Zn2+/Mg2+replaced Co2+successfully into the spinel structure of Co3O4 and promoted significantly the catalytic activity. Especially, the addition of CeO2 and K2O/Na2O decreased the binding energy and resulted in an increase in the density of the electron cloud around Co and an improvement of the catalytic activity. Of the investigated cobalt mixed catalysts, the best catalytic activity was shown by 2% K-Zn0.5-Ce0.05-Co catalyst.展开更多
FeCe nanocomposite catalysts with different iron contents were synthesized by a facile co-precipitation method.The as-prepared materials were characterized by various techniques including powder X-ray diffraction(XRD)...FeCe nanocomposite catalysts with different iron contents were synthesized by a facile co-precipitation method.The as-prepared materials were characterized by various techniques including powder X-ray diffraction(XRD),N2 adsorption/desorption and high-resolution transmission electron microscopy(HRTEM).Catalyst with the highest iron content(90 FeCe) shows the best activity for the hydrogen generation via ammonia decomposition.83% NH3 conversion is achieved at 550℃ and nearly full conversion of NH3 is realized at 600℃ with a GHSV of 24000 cm3/(gcat·h).The large content and small size crystal particles of iron species are responsible for the good catalytic performance.Temperatureprogrammed reduction by hydrogen(H2-TPR) was performed to investigate the interaction between cerium and iron species.It is found that slight cerium can exert strong interaction with iron compound thus effectively prevent the self-aggregation of active iron species,so as to improve the catalytic activity for ammonia decomposition.展开更多
基金supported by the National Natural Science Foundation of China (21476229, 21376236, 21503264)~~
文摘N2O is a promising green propellant and exhibits great potential for satellite propulsion systems. It is difficult for catalytic decomposition, which is an important way to initiate the propulsion process, to occur at temperatures below 600 °C due to the high activation energy of N2O. In this work, we report an Ir supported on rutile TiO2(Ir/r-TiO2) catalyst which exhibits a fairly high activity for high-concentration N2O decomposition. HAADF-STEM, H2-TPR, and XPS results indicate that highly dispersed Ir particles and improved oxygen mobility on the Ir/r-TiO2 could facilitate the decompo-sition of N2O and desorption of the adsorbed oxygen. Bridge-bonded peroxide intermediates were observed with in-situ DRIFT and herein, a detailed decomposition route is proposed.
基金the Foundational Research Project of National Defence(No.A1420080145)for thefinancial support.
文摘Three kinds of Pt/alumina catalysts were prepared by impregnation-hydrogen reduction, impregnation-hydrazine reduction and electroless plating methods. Their differences in the structures, specific areas and particle sizes were characterized by XRD, BET and TEM, respectively. Furthermore, their catalytic activities for the hydrogen iodide (HI) decomposition were evaluated in a fixed bed reactor. The results show that the catalyst 5%Pt/Al2O3 prepared by the electroless plating has the optimum catalytic properties for HI decomposition owing to the high dispersion of the platinum nano-particles (〈5 nm) on the alumina supports.
文摘Catalytic decomposition of methylene chloride in air below 300℃ was studied. Sulfated titania was very effective in converting 959ppm methylene chloride selectively to CO, C02 and HCl. Complete decomposition of methylene chloride was achieved at low temperature (275℃ ). It was found that the acidic property of catalyst was a determinant factor for the catalytic activity. The presence of water vapor in the feed stream remarkably reduced the catalytic activity, which could be due to the blockage of acidic sites on the surface of catalyst by water molecules. A bifunctional catalyst comprising copper oxide was developed to improve the selectivity of catalytic oxidation , which indicated that copper oxide can promote the deep oxidation of methylene chloride. The crystal form of TiO2 imposes an important influence upon the catalytic oxidation.
基金This work was supported financially by the National Natural Science Foundation of China (No. 20506010) Beijing Novel Program (2006A74)Natural Science Fund of Shanxi Province (No. 20063004).
文摘A new dual-composition catalyst based on Ni-Mo/MgO with high efficiency of producing carbon nanotubes (CNTs) from methane was reported recently. In the present article, with this type of catalyst, the impact of such experimental parameters as reaction temperature, reaction time, concentration of H2, flow rate ratio of CH4 to H2 on yield and graphitization were investigated, leading to the following optimal growth conditions: reaction time 60min, reaction temperature 900℃, CH4:H2 about 100:20mL/min, under which high-yield multi-walled CNTs bundles were synthesized. Raman measurement indicated that the as-synthesized product was well-graphitized, and the purity was estimated over 95% by TG-DSC analysis. In terms of the above results, an explanation of high-efficiency formation of CNTs bundles and the co-catalysis mechanism of Ni-Mo/MgO were suggested. 2007 Chinese Societv of Particuology and Institute of Process Engineering, Chinese Academy of Sciences. Published by Elsevier B.V.
基金Supported by the National Natural Science Foundation of China(No.21263019 and 21467022)
文摘A new energetic complex,[Co(3,3?-Hbpt)(Htm)]·H_2O(1,3,3?-Hbpt = 3,5-bis(3-pyridyl)-1H-1,2,4-triazole and H_3tm = trimesic acid),has been synthesized by hydrothermal reactions and characterized by single-crystal X-ray diffraction,elementary analysis,IR spectroscopy,thermogravimetric analysis and X-ray powder diffraction. Single-crystal X-ray diffraction indicates that the complex belongs to triclinic system,space group P 1 with a = 10.0911(1),b = 10.2573(1),c = 10.6393(1) ?,α = 103.793(2),β = 101.041(2),γ = 107.918(3)o,V = 974.9(2) ?~3,Z = 2,D_c = 1.732 g·cm-3,μ = 0.941 mm^(-1),M_r = 508.31,F(000) = 518,the final R = 0.0523 and wR = 0.0935 with I 〉 2σ(I). In the title complex,Co(Ⅱ) ions are connected by Htm2-anions generating 1D ladder-like chains which are linked by 3,3?-Hbpt to form 1D cages. In addition,the thermal decomposition of ammonium perchlorate(AP) with complex 1 was explored by differential scanning calorimetry(DSC). AP is completely decomposed in a shorter time in the presence of complex 1,and the decomposition heat of the mixture is 2.531 kJ·g^(-1),significantly higher than that of pure AP. By Kissinger's method,the ratio of Ea/ln(A) is 11.05 for the mixture,which indicates that complex 1 shows good catalytic activity toward the AP decomposition.
文摘A series of mixed oxide catalysts with different composition of Co-M-Al and Co-M-Ce- Al (M=Zn, Ni, Cu) were prepared by co-precipitation method from hydrotalcite-like compounds. The experimental results revealed the catalytic activity of Co-Ni-Al is slightly higher than that of Co-Zn-Al and much higher than that of Co-Cu-Al for direct decomposition of N2O. Moreover, addition of small amounts of Ce02 improved the catalytic activity signif- icantly and made the decomposition temperatures at which the N2O conversion was 50% and 90% (T50 and Tgo) both decreased 80 ℃ than those of Co-M-Al catalysts without CeO2 added. Further, potassium-load also promoted the catalytic activity, and the decomposi- tion temperatures of T50 and T90 both decreased approximately 50 ℃. It is significant for decomposing N2O from industries and reducing carbon emission from atmosphere.
基金Supported by the Provincial Basic Research Program of Hebei Education Department(ZD2015110)the National Special Project on Key Technologies and Demonstration of Wetland Ecological Restoration in the Haihe River Basin(2014ZX07203008)
文摘It has been generally unclear over the mechanism of inhibitory influence of silicate on structural rearrangement or solely physical adsorption onto manganese dioxide (MnO2) about the decomposition of hydrogen peroxide (H2O2). Consequently, several experiments were carried out by using MnO2 as a catalyst for the decomposition of H2O2 in a concentration series under certain concentrations of silicates. The silicates were analyzed by using a molybdenum blue colorimetric method. The results showed that the determination of silicates was inhibited by H2O2, whose inhibitory effect was greatly increased by increasing its concentration, but not limited by pH. SEM-EDX (scanning electron microscopy-energy dispersive x-ray spectrometry) results showed that the adsorption of silicates onto the surface of MnO2 was not purely via a structural rearrangement, with increasing Mn atoms protruding on the outer surface by covering oxygen and silicon atoms. XRD (X-ray diffraction) and FTIR (Fourier transform infrared) spectra results further revealed no significant total crystal structural changes in MnO2 after the adsorption of silicates, but only a small shift of 0.21° at 2e from 56.36° to 56.15° , and a FTIR vibration showed at around 1 050 cm-1. The results, therefore, showed that silicate adsorption onto MnO2 took place via both surface adsorption and structural rearrangement by interfacial reaction.
文摘The catalytic hydrolysis of dichlorodifluoromethane (CFC-12) was investigated over solid acid Ti(SO_4)_2. The catalytic activity decreased with the calcination temperature. When space velocity was 6 1 h^(-1) g-cat^(-1). the CPC-12 conversion at 310C over Ti(SO_4)_2 calcined at 350C remained about 98.5% during 360 h on stream. and the selectivity to by-products remained zero. The findings enlarged the scope of traditional catalyst systems for the CFCs decomposition.
基金financial support by DST-SERB (Grant No.SRG/2021/001182)DRDO (Grant No.ARMREB/HEM/2021/241)is gratefully acknowledged。
文摘Ammonium dinitramide(ADN)based liquid monopropellants have been identified as environmentally benign substitutes for hydrazine monopropellant.However,new catalysts are to be developed for making ADN monopropellants cold-start capable.In the present study,performance of Co and Ba doped CuCr_2O_4 nanocatalysts prepared by hydrothermal method was evaluated on the decomposition of aqueous ADN solution and ADN liquid monopropellant(LMP103X).The catalysts were characterized by PXRD(Powder X-ray Diffraction),FTIR(Fourier Transform Infrared spectroscopy),SEM(Scanning Electron Microscopy),TEM(Transmission Electron Microscopy),EDS(Energy Dispersive X-ray Spectroscopy),and XPS(X-ray Photoelectron Spectroscopy).The nanosize was confirmed by SEM and TEM,while the nanoflake morphology was confirmed by the SEM analysis.Further,we obtained the elemental composition from the EDS analysis.We investigated the catalytic activity of the catalysts by thermogravimetric(TG)analysis and the developed catalysts lowered the decomposition temperature of ADN monopropellant by about 55℃.The XPS analysis confirmed the presence of metal ions with different chemical states.Apparently,increase in the surface area of the catalysts and the mixed active sites as well as the development of oxygen vacancy on the catalyst surface introduced by metal doping are influencing the decomposition temperature of ADN samples.
基金Major Natural Science Foundation of Guangdong Province, The Team Project of Guangdong Province and the Talent Training Program Foundation of the Higher Education Department of Gangdong Province.
文摘The catalytic reaction of NO with CO and decomposition of NO over metal modified ACFs were investigated and compared with other carriers supported catalysts. It is demonstrated that Pd/ACF and Pd/Cu/ACF have high catalytic activity for the reaction of NO/CO, while Pt/ACF, Pt/Cu/ACF and Co/Cu/ACF have very low catalytic activity in similar circumstance. Pd-modified ACF possesses high catalytic decomposition of NO at 300℃. Pd/CB and Pd/GAC present good catalytic decomposition ability for NO only at low flowrate. Pd/G, Pd/ZMS and Pd/A however, do not show any catalytic activity for NO decomposition even at 400℃. Catalytic temperature, NO flowrate and loading of metal components affect the decomposition rate of NO. The coexistence of Cu with Pd on Cu/Pd/ACF leads to crystalline of palladium to more unperfected so as to that increase the catalytic activity.
基金funded by a PFR 2023 research grant from the Ministry of Education,Culture,Research,and Technology of the Republic of Indonesia(contract number 183/E5/PG/02.00.PL/2023).
文摘Numerous researchers in the energy field are engaged in a competitive race to advance hydrogen as a clean and environmentally friendly fuel.Studies have been conducted on the different aspects of hydrogen,including its production,storage,transportation and utilization.The catalytic methane decomposition technique for hydrogen production is an environmentally friendly process that avoids generating carbon dioxide gas,which contributes to the greenhouse effect.Catalysts play a crucial role in facilitating rapid,cost-effective and efficient production of hydrogen using this technique.In this study,reactive molecular dynamics simulations were employed to examine the impact of Pt_(7) cluster decoration on the surface of a Ni(110)catalyst,referred to as Pt_(7)-Ni(110),on the rates of methane dissociation and molecular hydrogen production.The reactive force field was employed to model the atomic interactions that enabled the formation and dissociation of chemical bonds.Our reactive molecular dynamics simulations using the Pt_(7)-Ni(110)catalyst revealed a notable decrease in the number of methane molecules,specifically~11.89 molecules per picosecond.The rate was approximately four times higher than that of the simulation system utilizing a Ni(110)catalyst and approximately six times higher than that of the pure methane,no-catalyst system.The number of hydrogen molecules generated during a simulation period of 150000 fs was greater on the Pt_(7)-Ni(110)surface than in both the Ni(110)and pure methane systems.This was due to the presence of numerous dissociated hydrogen atoms on the Pt_(7)-Ni(110)surface.
文摘The preparation of immobilizing-catalysts for decomposing ozone by using dipping method was studied. XRD, XPS and TEM were used to characterize the catalysts. The three kinds of catalysts were selected preferentially, and their catalytic activities were investigated. The results showed that the catalyst with activated carbon dipping acetate(active components are Mn:Cu=3:2, active component proportion in catalyst is 15%, calcination temperature is 200℃) has the best catalytic activity for ozone decomposing. One gram of catalyst can decompose 17.6 g ozone at initial ozone concentration of 2.5 g/m 3 and the residence time in reactor of 0.1 s. The experimental results also indicated that humidity of reaction system had negative effect on catalytic activity.
基金supported by the Czech Science Foundation(106/09/1664)the Ministry of Education,Youth and Sports of the CzechRepublic(NPV II 2B06068)
文摘Intrinsic data of N2O catalytic decomposition over a K-promoted Co-Mn-Al mixed oxide prepared by the thermal treatment of a layered double hydroxide was used for the design of a pilot reactor for the abatement of N2O emissions from the off-gases in HNO3 production.A pseudo-homogeneous one-dimensional model of an ideal plug flow reactor under an isothermal regime(450°C)was used for reactor design.A catalyst particle diameter of 3 mm is a compromise size because increasing the size of the catalyst particle leads to a decrease in the reaction rate because of an internal diffusion limitation,and particles with a smaller diameter cause a large pressure drop.A catalyst bed of 11.5 m 3 was estimated for the target N2O conversion of 90%upon the treatment of 30000 m 3 /h of exhaust gas(0.1 mol%N2O,0.005 mol% NO,0.9 mol%H2O,5 mol%O2)at 450°C and 130 kPa.
文摘To control contamination of flue gas emission NOx, the author mixcd method of preparing new magnesia base catalyst and researched on denitrificating fine gas by directness catalytic decomposition. Usually removal rate of NO is regarded on the main evaluation criteria. The author analyzed calcination temperature of catalyzer manufacturing process, the temperature of flue gas desorption tower, bed height and efficiency denitrification of NO concentration. And discussed the result of both denitrate lore-and-aft of FT-IR and XRD. The experiment indicates that magnesia base catalyst is available to directness catalytic decomposition denitrificate flue gas. Through denitrification rate is from 85% to 95%. The ingredient of magnesia base catalyst is made from magnesia, firming agent, addition agent. Height denitration bed was 4 cm- 5 cm, deuitration reaction temperature is 130℃-170℃, through the analyses above, presumed that magnesia base catalyst exist activating of vice, and analyzed this vice preliminarily.
基金Project supported by the National Natural Science Foundation of China(21875192)the Basic Research Project of Sichuan Province for Science and Technology Development(2019YJ0355)+1 种基金Outstanding Youth Science and Technology Talents Program of Sichuan(19JCQN0085)the Project of State Key Laboratory of Environment-friendly Energy Materials,Southwest University of Science and Technology(20fksy04)。
文摘Given their unique and excellent properties,metal-organic frameworks(MOFs)materials have been used in many scientific fields.EMOFs use energetic materials as ligands,which can provide part of the energy for the system while catalyzing ammonium perchlorate.The energetic material 1.1'-dihydroxyazotetrazole(H_(2)AzTO),as a high-energy nitrogen-rich material,was selected as a ligand.Five kinds of La^(3+),Ce^(3+),Pr^(3+),Nd^(3+),and Sm^(3+)lanthanide EMOFs were synthesized and obtained.Single crystal X-ray diffraction tests were conducted to obtain the crystal structures of EMOFs 1-5,which indicate that they have similar crystal structures.The thermal stabilities of EMOFs 1-5,which are obtained by differential scanning calorimetry(DSC)tests,are improved compa red with that of the ligand.The results of thermicdecomposition of ammonium perchlorate(AP)and AP mixtures with 10 wt%EMOFs 1-5 show that except for AP mixed with 10 wt%co mpound 2,the high-temperature decomposition peak tempe rature of AP mixed with other compounds is significantly advanced(up to 59.3-88.3 K),and the decomposition of AP is continuous and violent.EMOFs 3-5 have good application prospects for the catalytic thermicdecomposition of AP.
基金supports from a 973 Program of the Chinese Ministry of Science and Technology under contract number G199902240National Natural Science Foundation of China under contract numbers 20006072,29792079-2 and 29876032 are gratefully acknowledged.
文摘An alumina-supported cobalt aerogel catalyst prepared from a sol-gel and a supercritical drying method was used in the catalytic decomposition of methane. The physical-chemical properties of the catalyst were characterized and its activity for methane decomposition was investigated. The effects of calcination and reaction temperatures on the activity of the catalyst and the morphology of the carbon nanotubes produced were discussed. A CoAl2O4 spinel structure formed in the calcined catalyst. The quantity of the nanotubes produced in the reaction increases with the amount of cobalt in the reduced catalyst. A higher reaction temperature leads to a higher reaction rate, though faster deactivation of the catalyst occurs with the change. The carbon nanotubes grown on the catalyst have smooth walls and uniform di-ameter distribution.
文摘Magnetic TS-1 was synthesized thesis and solvent vaporation method. The with nanosized nickelferrite particles prepared samples were characterized as nuclei via the hydrothermal syn- with N2 adsorption-desorption iso- therms, FTIR spectrometry, Raman spectrometry, X-ray diffraction, Ultraviolet-visible spectroscopy and Vibrating sample magnetometry. The results show that the composite obtained was composed of TS-1 with MFI structure and NiFe204 with spinel structure, its specific surface area was about 316 m2/g, pore volume was 0.12 cm3/g and pore size distribution was in the range of 0.5-0.7 nm. The catalytic activity of the composite was also investigated by its catalyzing the decomposition of rhodamine B oxidized by H2O2 in aqueous solution. In this case Rhodamine B pollutant could be completely degraded within 150 min. Magnetic TS-1 exhibited high photocatalytic efficiency and super paramagnetic nature for cleaning polluted water with the help of magnetic separation.
基金supported by the Hi-Tech Research and Development Program (863) of China (No. 2012AA062501)the Natural Science Foundation of Hubei Province (No. 2009CDB246)the Postgraduates Innovation Foundation of Huazhong University of Science and Technology of China (No. HF-08-11-2011-261)
文摘Three groups of cobalt mixed oxide catalysts(Mg/Zn-Co, Mg/Zn-Ce-C, K/Na-Mg/Zn-Ce-Co)were prepared by sol-gel or impregnation methods. The synergistic effects of transition metal, rare earth metal and alkali metal on cobalt mixed catalysts for nitrous oxide(N2O)decomposing to N2 and O2were investigated. The experimental results revealed that the catalytic activity for N2 O decomposition was promoted as Co2+was replaced partially by Zn2+/Mg2+, moreover, the characterization analysis by XRD and XPS showed that Zn2+/Mg2+replaced Co2+successfully into the spinel structure of Co3O4 and promoted significantly the catalytic activity. Especially, the addition of CeO2 and K2O/Na2O decreased the binding energy and resulted in an increase in the density of the electron cloud around Co and an improvement of the catalytic activity. Of the investigated cobalt mixed catalysts, the best catalytic activity was shown by 2% K-Zn0.5-Ce0.05-Co catalyst.
基金Project supported by the Natural Science Foundation of Jiangsu Province (BK20170232,BK20170238)National Natural Science Foundation of China (51908256)。
文摘FeCe nanocomposite catalysts with different iron contents were synthesized by a facile co-precipitation method.The as-prepared materials were characterized by various techniques including powder X-ray diffraction(XRD),N2 adsorption/desorption and high-resolution transmission electron microscopy(HRTEM).Catalyst with the highest iron content(90 FeCe) shows the best activity for the hydrogen generation via ammonia decomposition.83% NH3 conversion is achieved at 550℃ and nearly full conversion of NH3 is realized at 600℃ with a GHSV of 24000 cm3/(gcat·h).The large content and small size crystal particles of iron species are responsible for the good catalytic performance.Temperatureprogrammed reduction by hydrogen(H2-TPR) was performed to investigate the interaction between cerium and iron species.It is found that slight cerium can exert strong interaction with iron compound thus effectively prevent the self-aggregation of active iron species,so as to improve the catalytic activity for ammonia decomposition.