The traditional automotive catalytic converter using commercial ceramic honeycomb carriers has many problems such as high back pressure,low engine efficiency,and high usage of precious metals.This study proposes a fou...The traditional automotive catalytic converter using commercial ceramic honeycomb carriers has many problems such as high back pressure,low engine efficiency,and high usage of precious metals.This study proposes a four-channel catalytic micro-reactor based on alumina hollow fiber membrane,which uses phase inversion method for structural molding and regulation.Due to the advantages of its carrier,it can achieve lower ignition temperature under low noble metal loading.With Pd/CeO_(2) at a loading rate of 2.3%(mass),the result showed that the reaction ignition temperature is even less than 160℃,which is more than 90℃ lower than the data of commercial ceramic substrates under similar catalyst loading and airspeed conditions.The technology in turn significantly reduces the energy consumption of the reaction.And stability tests were conducted under constant conditions for 1000 h,which proved that this catalytic converter has high catalytic efficiency and stability,providing prospects for the design of innovative catalytic converters in the future.展开更多
The effect of Na-excess content in the precursor on the structural and electrochemical performances of sodium nickel manganese oxide(NNMO)prepared by sol-gel and electrospinning methods is investigated in this paper.X...The effect of Na-excess content in the precursor on the structural and electrochemical performances of sodium nickel manganese oxide(NNMO)prepared by sol-gel and electrospinning methods is investigated in this paper.X-ray diffraction results of the prepared NNMO without adding Na-excess content indicate sodium loss,while the mixed phase of P2/O′3-type layered NNMO presented after adding Na-excess content.Compared with the sol-gel method,the secondary phase of NiO is more suppressed by using the electrospinning method,which is further confirmed by field emission scanning electron microscope images.N_(2) adsorption-desorption isotherms show no remarkably difference in specific surface areas between different preparation methods and Na-excess contents.The analysis of X-ray absorption near edge structure indicates that the oxidation states of Ni and Mn are+2 and+4,respectively.For the electrochemical properties,superior electrochemical performance is observed in the NNMO electrode with a low Na-excess content of 5wt%.The highest specific capacitance is 36.07 F·g^(-1)at0.1 A·g^(-1)in the NNMO electrode prepared by using the sol-gel method.By contrast,the NNMO electrode prepared using the electrospinning method with decreased Na-excess content shows excellent cycling stability of 100%after charge-discharge measurements for 300 cycles.Therefore,controlling the Na excess in the precursor together with the preparation method is important for improving the electrochemical performance of Na-based electrode materials in supercapacitors.展开更多
Influence of three different preparation methods, i.e. impregnation, coprecipitation, and inverse coprecipitation, on the preferential oxidation of CO in excess hydrogen (PROX) over CuO-CeO2 catalysts has been inves...Influence of three different preparation methods, i.e. impregnation, coprecipitation, and inverse coprecipitation, on the preferential oxidation of CO in excess hydrogen (PROX) over CuO-CeO2 catalysts has been investigated and CuO-CeO2 catalysts are characterized using BET, XPS, XRD, UV Raman, and TPR techniques. The results show that the catalysts prepared by coprecipitation have smaller particle sizes, well-dispersed CuOx species, more oxygen vacancies, and are more active in the PROX than those prepared by the other methods. However. the inverse coprecipitation depresses the catalytic performance of CuO-CeO2 catalysts and causes the growth of CuO-CeO2 because of different pH value in the precipitation process.展开更多
A series of SnO2‐based catalysts modified by Mn, Zr, Ti and Pb oxides with a Sn/M (M=Mn, Zr, Ti and Pb) molar ratio of 9/1 were prepared by a co‐precipitation method and used for CH4 and CO oxidation. The Mn3+, ...A series of SnO2‐based catalysts modified by Mn, Zr, Ti and Pb oxides with a Sn/M (M=Mn, Zr, Ti and Pb) molar ratio of 9/1 were prepared by a co‐precipitation method and used for CH4 and CO oxidation. The Mn3+, Zr4+, Ti4+and Pb4+cations are incorporated into the lattice of tetragonal rutile SnO2 to form a solid solution structure. As a consequence, the surface area and thermal stability of the catalysts are improved. Moreover, the oxygen species of the modified catalysts become easier to be reduced. Therefore, the oxidation activity over the catalysts was improved, except for the one modified by Pb oxide. Manganese oxide demonstrates the best promotional effects for SnO2. Using an X‐ray diffraction extrapolation method, the lattice capacity of SnO2 for Mn2O3 was 0.135 g Mn2O3/g SnO2, which indicates that to form stable solid solution, only 21%Sn4+cations in the lattice can be maximally replaced by Mn3+. If the amount of Mn3+cations is over the capacity, Mn2O3 will be formed, which is not favorable for the activity of the catalysts. The Sn rich samples with only Sn‐Mn solid solution phase show higher activity than the ones with excess Mn2O3 species.展开更多
The Cu-Zr-Ce-O catalysts prepared using the coprecipitation method exhibited better catalytic performance for CO selective oxidation. The Cu-Zr-Ce-O catalysts pretreated with different methods were studied by CO-TPR a...The Cu-Zr-Ce-O catalysts prepared using the coprecipitation method exhibited better catalytic performance for CO selective oxidation. The Cu-Zr-Ce-O catalysts pretreated with different methods were studied by CO-TPR and XPS techniques. The results showed that the Cu-Zr-Ce-O catalyst pretreated with oxygen exhibited the best catalytic performance and had the widest operating temperature window, with CO conversion above 99% from 160 to 200 ℃. The O2 pretreatment caused an enrichment of the oxygen storaged on the Cu active species and promoted the conversion of adsorbed oxygen into surface lattice oxygen. It also improved the amount of Cu+/Cu^2+ ionic pair, and then facilitated the formation of CuO active species on the catalyst for selective CO oxidation.展开更多
The removal of hydrogen sulfide from gas plays an important role in rational utilization of resources and environ- mental protection. In this paper, the process of hydrogen sulfide removal by wet oxidation method in a...The removal of hydrogen sulfide from gas plays an important role in rational utilization of resources and environ- mental protection. In this paper, the process of hydrogen sulfide removal by wet oxidation method in a rotating packed bed was investigated in a scale for treating 10 000 Nm3/h of gas. On the basis of studying the influence of the species and con- centration of alkali source, the liquid/gas volume ratio, the high gravity factor, and the hydrogen sulfide content in feed gas on the desulfurization effect, the suitable technological conditions were obtained. The hydrogen sulfide removal efficiency could reach 98.0% under these conditions. The results of continuous operation of process facilities showed that the high gravity method has many merits including higher desulfurization rate, good stability in operation, lower liquid/gas volume ratio, greater operation elasticity, and apparent energy saving effects.展开更多
The reduced sealing difficulty of tubular solid oxide fuel cells(SOFCs)makes the stacking of tubular cell groups relatively easy,and the thermal stress constraints during stack operation are smaller,which helps the st...The reduced sealing difficulty of tubular solid oxide fuel cells(SOFCs)makes the stacking of tubular cell groups relatively easy,and the thermal stress constraints during stack operation are smaller,which helps the stack to operate stably for a long time.The special design of tubular SOFC structures can completely solve the problem of high-temperature sealing,especially in the design of multiple single-cell series integrated into one tube,where each cell tube is equivalent to a small electric stack,with unique characteristics of high voltage and low current output,which can significantly reduce the ohmic polarization loss of tubular cells.This paper provides an overview of typical tubular SOFC structural designs both domestically and internationally.Based on the geometric structure of tubular SOFCs,they can be divided into bamboo tubes,bamboo flat tubes,single-section tubes,and single-section flat tube structures.Meanwhile,this article provides an overview of commonly used materials and preparation methods for tubular SOFCs,including commonly used materials and preparation methods for support and functional layers,as well as a comparison of commonly used preparation methods for microtubule SOFCs,It introduced the three most important parts of building a fuel cell stack:manifold,current collector,and ceramic adhesive,and also provided a detailed introduction to the power generation systems of different tubular SOFCs,Finally,the development prospects of tubular SOFCs were discussed.展开更多
The CuO-CeO2 catalyst prepared by chelating method has a superior catalytic performance for the preferential oxidation of CO in rich hydrogen, compared with the CuO-CeO2 catalyst prepared by coprecipitation method. Th...The CuO-CeO2 catalyst prepared by chelating method has a superior catalytic performance for the preferential oxidation of CO in rich hydrogen, compared with the CuO-CeO2 catalyst prepared by coprecipitation method. The CO conversions over these catalysts, at 120 ℃ and 120000 ml/(g-h) in the absence of CO2 and H2O, are 99.6% and 88.6%, respectively, and the selectivity of O2 over these catalysts is very close (i.e. 51.3% and 55.8%, respectively). The influence of certain factors such as hydrogen concentration, carbon monoxide concentration, H2O, O2/CO ratios, and space velocity on the catalytic performance of CuO-CeO2 catalyst prepared by chelating method is also studied. The results show that the addition of hydrogen and H2O has a negative effect on the catalytic performance of CuO-CeO2 catalyst, however, the variation of space velocity and the O2/CO ratio causes a comparatively slight influence.展开更多
High-temperature oxidation is an important property to evaluate thermal protection materials. However, since oxidation is a complex process involving microstructure evolution, its quantitative analysis has always been...High-temperature oxidation is an important property to evaluate thermal protection materials. However, since oxidation is a complex process involving microstructure evolution, its quantitative analysis has always been a challenge. In this work, a phase field method (PFM) based on the thermodynamics theory is developed to simulate the oxidation behavior and oxidation induced growth stress. It involves microstructure evolution and solves the problem of quantitatively computational analysis for the oxidation behavior and growth stress. Employing this method, the diffusion process, oxidation performance, and stress evolution axe predicted for Fe-Cr-A1-Y alloys. The numerical results agree well with the experimental data. The linear relationship between the maximum growth stress and the environment oxygen concentration is found. PFM provides a powerful tool to investigate high-temperature oxidation in complex environments.展开更多
The influence of different cooking and smoking methods (boiling, frying, frying + boiling, hot and cold smoking) on oxidation and fatty acid composition of catfish (Arius maculatus) commercialized on the Wouri river c...The influence of different cooking and smoking methods (boiling, frying, frying + boiling, hot and cold smoking) on oxidation and fatty acid composition of catfish (Arius maculatus) commercialized on the Wouri river coast was evaluated including commonly used analytical indexes (peroxide and acid values)and physical analysis by Fourier transform infrared (FTIR) spectroscopy. The mean moisture, protein, ash and fat contents of raw fish were 75.88 ± 0.55;64.24 ± 0.14;10.98 ± 0.31 and 23.02 ± 0.88 respectively. All these treatments provoke the modification of the quality indexes. Lipid deterioration, thermolysis and lipid oxidation occurred throughout the treatment. Peroxide value decreased for all cooked and smoked catfish, while free fatty acids of smoked sample increased. The FTIR applied to evaluate lipid oxidation in extracted lipid clearly provided a better picture of the oxidation progress and led to a similar conclusion with chemical analysis. Boiled, bleaching hot and bleaching cold smoking were found to be the suitable treatment methods for catfish because they gave it a high nutritive value compared to other smoking methods.展开更多
The oil oxidation characteristics of the whole temperature regions from 30 ℃ to 600 ℃ during oil reservoir air injection were revealed by experiments. The whole oil oxidation temperature regions were divided into fo...The oil oxidation characteristics of the whole temperature regions from 30 ℃ to 600 ℃ during oil reservoir air injection were revealed by experiments. The whole oil oxidation temperature regions were divided into four different parts: dissolving and inflation region, low temperature oxidation region, medium temperature oxidation region and high temperature oxidation region. The reaction mechanisms of different regions were explained. Based on the oil oxidation characteristics and filed tests results, light oil reservoirs air injection development methods were divided into two types: oxygen-reducing air flooding and air flooding;heavy oil reservoirs air injection in-situ combustion development methods were divided into two types: medium temperature in-situ combustion and high temperature in-situ combustion. When the reservoir temperature is lower than 120 ℃, oxygen-reducing air flooding should be used for light oil reservoir development. When the reservoir temperature is higher than 120 ℃, air flooding method should be used for light oil reservoir development. For a normal heavy oil reservoir, when the combustion front temperature is lower than 400 ℃, the development method is medium temperature in-situ combustion. For a heavy oil reservoir with high oil resin and asphalting contents, when the combustion front temperature is higher than 450 ℃, the development method at this condition is high temperature in-situ combustion. Ten years field tests of air injection carried out by PetroChina proved that air has advantages in technical, economical and gas source aspects compared with other gas agents for oilfield gas injection development. Air injection development can be used in low/super-low permeability light oil reservoirs, medium and high permeability light oil reservoirs and heavy oil reservoirs. Air is a very promising gas flooding agent.展开更多
The hydrothermal synthesis of In_(2)O_(3)and CeO_(2)–In_(2)O_(3)is investigated as well as the properties of sensor layers based on these compounds.During the synthesis of In_(2)O_(3),intermediate products In(OH)_(3)...The hydrothermal synthesis of In_(2)O_(3)and CeO_(2)–In_(2)O_(3)is investigated as well as the properties of sensor layers based on these compounds.During the synthesis of In_(2)O_(3),intermediate products In(OH)_(3)and InOOH are formed,which are the precursors of stable cubic(c-In_(2)O_(3))and metastable rhombohedral(rh-In_(2)O_(3))phases,respectively.A transition from c-In_(2)O_(3)to rh-In_(2)O_(3)is observed with the addition of CeO_(2).The introduction of cerium into rh-In_(2)O_(3)results in a decrease in the sensor response to hydrogen,while it increases in composites based on c-In_(2)O_(3).The data on the sensor activity of the composites correlate with XPS results in which CeO_(2)causes a decrease in the concentrations of chemisorbed oxygen and oxygen vacancies in rh-In_(2)O_(3).The reverse situation is observed in composites based on c-In_(2)O_(3).Compared to In_(2)O_(3)and CeO_(2)–In_(2)O_(3)obtained by other methods,the synthesized composites demonstrate maximum response to H_(2)at low temperatures by 70–100℃,and have short response time(0.2–0.5 s),short recovery time(6–7 s),and long-term stability.A model is proposed for the dependence of sensitivity on the direction of electron transfer between In_(2)O_(3)and CeO_(2).展开更多
For present solid oxide fuel cells(SOFCs),rapid performance degradation is observed in the initial aging process,and the dis-cussion of the degradation mechanism necessitates quantitative analysis.Herein,focused ion b...For present solid oxide fuel cells(SOFCs),rapid performance degradation is observed in the initial aging process,and the dis-cussion of the degradation mechanism necessitates quantitative analysis.Herein,focused ion beam-scanning electron microscopy was em-ployed to characterize and reconstruct the ceramic microstructures of SOFC anodes.The lattice Boltzmann method(LBM)simulation of multiphysical and electrochemical processes in the reconstructed models was performed.Two samples collected from industrial-size cells were characterized,including a reduced reference cell and a cell with an initial aging process.Statistical parameters of the reconstructed microstructures revealed a significant decrease in the active triple-phase boundary and Ni connectivity in the aged cell compared with the reference cell.The LBM simulation revealed that activity degradation is dominant compared with microstructural degradation during the initial aging process,and the electrochemical reactions spread to the support layer in the aged cell.The microstructural and activity de-gradations are attributed to Ni migration and coarsening.展开更多
The systematic method for constructing Lewis representations is a method for representing chemical bonds between atoms in a molecule. It uses symbols to represent the valence electrons of the atoms involved in the bon...The systematic method for constructing Lewis representations is a method for representing chemical bonds between atoms in a molecule. It uses symbols to represent the valence electrons of the atoms involved in the bond. Using a number of rules in a defined order, it is often better suited to complicated cases than the Lewis representation of atoms. This method allows us to determine the formal charge and oxidation number of each atom in the edifice more efficiently than other methods.展开更多
Recent advances in utilizing ^(17)O isotopic labeling methods for solid-state nuclear magnetic resonance(NMR)investigations of metal oxides for lithium-ion batteries have yielded extensive insights into their structur...Recent advances in utilizing ^(17)O isotopic labeling methods for solid-state nuclear magnetic resonance(NMR)investigations of metal oxides for lithium-ion batteries have yielded extensive insights into their structural and dynamic details.Herein,we commence with a brief introduction to recent research on lithium-ion battery oxide materials studied using ^(17)O solid-state NMR spectroscopy.Then we delve into a review of ^(17)O isotopic labeling methods for tagging oxygen sites in both the bulk and surfaces of metal oxides.At last,the unresolved problems and the future research directions for advancing the ^(17)O labeling technique are discussed.展开更多
Co3O4 catalysts prepared with different precipitants(NH3·H2O,KOH,NH4HCO3,K2CO3 and KHCO3)were investigated for the oxidation of formaldehyde(HCHO).Among these,KHCO3-precipitated Co3O4(KHCO3-Co) was the most...Co3O4 catalysts prepared with different precipitants(NH3·H2O,KOH,NH4HCO3,K2CO3 and KHCO3)were investigated for the oxidation of formaldehyde(HCHO).Among these,KHCO3-precipitated Co3O4(KHCO3-Co) was the most active low-temperature catalyst,and was able to completely oxidize HCHO at the 100-ppm level to CO2 at 90℃.In situ diffuse reflectance infrared spectroscopy demonstrated that hydroxyl groups on the catalyst surface were regenerated by K~+ and CO3^(2-),thus promoting the oxidation of HCHO.Moreover,H2-temperature programmed reduction and X-ray photoelectron spectroscopy showed that employing KHCO3 as the precipitant increased the Co^3+/Co^2+molar ratio on the surface of the Co3O4 catalyst,thus further promoting oxidation.Structural characterization revealed that catalysts precipitated with carbonate or bicarbonate reagents exhibited greater specific surface areas and pore volumes.Overall,these data suggest that the high activity observed during the Co3O4 catalyzed oxidation of HCHO can be primarily attributed to the presence of K~+ and CO3^(2-) on the Co3O4 surface and the favorable Co^3+/Co^2+ ratio.展开更多
A molten salt method was developed to prepare porous La1‐xSrxMn0.8Fe0.2O3 (0≤ x ≤ 0.6) micro‐spheres using hierarchical porous δ‐MnO2 microspheres as a template in eutectic NaNO3‐KNO3. X‐ray diffraction patt...A molten salt method was developed to prepare porous La1‐xSrxMn0.8Fe0.2O3 (0≤ x ≤ 0.6) micro‐spheres using hierarchical porous δ‐MnO2 microspheres as a template in eutectic NaNO3‐KNO3. X‐ray diffraction patterns showed that single phase LaMn0.8Fe0.2O3 with good crystallinity was syn‐thesized at 450℃ after 4 h. Transmission electron microscope images exhibited that the LaMn0.8Fe0.2O3 sample obtained at 450?? after 4 h possessed a porous spherical morphology com‐posed of aggregated nanocrystallites. Field emission scanning electron microscope images indicated that the growth of the porous LaMn0.8Fe0.2O3 microspheres has two stages. SEM pictures showed that a higher calcination temperature than 450?? had an adverse effect on the formation of a po‐rous spherical structure. The LaMn0.8Fe0.2O3 sample obtained at 450?? after 4 h displayed a high BET surface area of 55.73 m2/g with a pore size of 9.38 nm. Fourier transform infrared spectra suggested that Sr2+ions entered the A sites and induced a decrease of the binding energy between Mn and O. The CO conversion with the La1‐xSrxMn0.8Fe0.2O3 (0≤x≤0.6) samples indicated that the La0.4Sr0.6Mn0.8Fe0.2O3 sample had the best catalytic activity and stability. Further analysis by X‐ray photoelectron spectroscopy demonstrated that Sr2+doping altered the content of Mn4+ions, oxygen vacancies and adsorbed oxygen species on the surface, which affected the catalytic performance for CO oxidation.展开更多
A series of rare earth hydroxide and oxide nanoparticles have been prepared by precipitation method with alcohol as the dispersive and protective reagent. Transmission electron microscope (TEM) images indicate that ...A series of rare earth hydroxide and oxide nanoparticles have been prepared by precipitation method with alcohol as the dispersive and protective reagent. Transmission electron microscope (TEM) images indicate that the particles are spherical in shape and smaller than 100 nm in size. The crystallite sizes of cubic Ln2O3 have lanthanide shrinking effect, while average crystal lattice distortion rates possess lanthanide swelling effect. The diffraction peak intensity of heavy rare earth oxide nanometer powders is remarkably stronger than that of light rare earth oxide nanometer powders. The variation of diffraction intensity with atomic number presents an inverted W type, forming a double peak structure. Fourier transform infrared (FTIR) spectrums reveal that Ln2O3 nanopowders have higher surface activity than that of ordinary Ln2O3 powders. The UV-vis spectra show that Ln-O bond of these particles is slightly blue-shifted, and its absorption intensity decreases.展开更多
A carbon supported Pd(Pd/C) catalyst used as the anodic catalyst in the direct formic acid fuel cells(DFAFC) was prepared via the improved complex reduction method with sodium ethylenediamine tetracetate(EDTA) a...A carbon supported Pd(Pd/C) catalyst used as the anodic catalyst in the direct formic acid fuel cells(DFAFC) was prepared via the improved complex reduction method with sodium ethylenediamine tetracetate(EDTA) as stabilizer and complexing agent. This method is very simple. The average size of the Pd particles in the Pd/C catalyst prepared with the improved complex reduction method is as small as about 2.1 nm and the Pd particles in the Pd/C catalyst possess an excellent uniformity. The Pd/C catalyst shows a high electrocatalytic activity and stability for the formic acid oxidation.展开更多
The orthogonal test was used to optimize the reaction conditions of roasting zinc oxide ore with NaOH aiming to comprehensively utilize zinc oxide ore.The optimized reaction conditions were molar ratio of NaOH to zinc...The orthogonal test was used to optimize the reaction conditions of roasting zinc oxide ore with NaOH aiming to comprehensively utilize zinc oxide ore.The optimized reaction conditions were molar ratio of NaOH to zinc oxide ore 6:1,roasting temperature 450°C,holding time 150 min.The molar ratio of NaOH to zinc oxide ore was the most predominant factor affecting the extraction ratios of zinc oxide and silica.The mineral phase transformations were investigated by testing the phases of specimens obtained at different temperatures.The process was that silica reacted with molten NaOH to form Na_2SiO_3 at first,then transformed into Na_4SiO_4 with temperature rising.ZnCO_3 and its decomposing product ZnO reacted with NaOH to form Na_2ZnO_2.Na_2ZnSiO_4was also obtained.The reaction rate was investigated using unreacted shrinking core model.Two models used were chemical reaction at the particle surface and diffusion through the product layer.The results indicated that the reaction rate was combine-controlled by two models.The activation energy and frequency factor were obtained as 24.12 k J/mol and 0.0682,respectively.展开更多
基金funded by the Natural Science Foundation of Jiangsu Province(BK20210252)。
文摘The traditional automotive catalytic converter using commercial ceramic honeycomb carriers has many problems such as high back pressure,low engine efficiency,and high usage of precious metals.This study proposes a four-channel catalytic micro-reactor based on alumina hollow fiber membrane,which uses phase inversion method for structural molding and regulation.Due to the advantages of its carrier,it can achieve lower ignition temperature under low noble metal loading.With Pd/CeO_(2) at a loading rate of 2.3%(mass),the result showed that the reaction ignition temperature is even less than 160℃,which is more than 90℃ lower than the data of commercial ceramic substrates under similar catalyst loading and airspeed conditions.The technology in turn significantly reduces the energy consumption of the reaction.And stability tests were conducted under constant conditions for 1000 h,which proved that this catalytic converter has high catalytic efficiency and stability,providing prospects for the design of innovative catalytic converters in the future.
基金financially supported by (i) Suranaree University of Technology,(ii) Thailand Science Research and Innovation,and (iii) National Science,Research and Innovation Fund(project codes 90464 and 160363)。
文摘The effect of Na-excess content in the precursor on the structural and electrochemical performances of sodium nickel manganese oxide(NNMO)prepared by sol-gel and electrospinning methods is investigated in this paper.X-ray diffraction results of the prepared NNMO without adding Na-excess content indicate sodium loss,while the mixed phase of P2/O′3-type layered NNMO presented after adding Na-excess content.Compared with the sol-gel method,the secondary phase of NiO is more suppressed by using the electrospinning method,which is further confirmed by field emission scanning electron microscope images.N_(2) adsorption-desorption isotherms show no remarkably difference in specific surface areas between different preparation methods and Na-excess contents.The analysis of X-ray absorption near edge structure indicates that the oxidation states of Ni and Mn are+2 and+4,respectively.For the electrochemical properties,superior electrochemical performance is observed in the NNMO electrode with a low Na-excess content of 5wt%.The highest specific capacitance is 36.07 F·g^(-1)at0.1 A·g^(-1)in the NNMO electrode prepared by using the sol-gel method.By contrast,the NNMO electrode prepared using the electrospinning method with decreased Na-excess content shows excellent cycling stability of 100%after charge-discharge measurements for 300 cycles.Therefore,controlling the Na excess in the precursor together with the preparation method is important for improving the electrochemical performance of Na-based electrode materials in supercapacitors.
文摘Influence of three different preparation methods, i.e. impregnation, coprecipitation, and inverse coprecipitation, on the preferential oxidation of CO in excess hydrogen (PROX) over CuO-CeO2 catalysts has been investigated and CuO-CeO2 catalysts are characterized using BET, XPS, XRD, UV Raman, and TPR techniques. The results show that the catalysts prepared by coprecipitation have smaller particle sizes, well-dispersed CuOx species, more oxygen vacancies, and are more active in the PROX than those prepared by the other methods. However. the inverse coprecipitation depresses the catalytic performance of CuO-CeO2 catalysts and causes the growth of CuO-CeO2 because of different pH value in the precipitation process.
基金supported by the National Natural Science Foundation of China (21263015,21567016 and 21503106)the Education Department Foundation of Jiangxi Province (KJLD14005 and GJJ150016)the Natural Science Foundation of Jiangxi Province (20142BAB213013 and 20151BBE50006),which are greatly acknowledged by the authors~~
文摘A series of SnO2‐based catalysts modified by Mn, Zr, Ti and Pb oxides with a Sn/M (M=Mn, Zr, Ti and Pb) molar ratio of 9/1 were prepared by a co‐precipitation method and used for CH4 and CO oxidation. The Mn3+, Zr4+, Ti4+and Pb4+cations are incorporated into the lattice of tetragonal rutile SnO2 to form a solid solution structure. As a consequence, the surface area and thermal stability of the catalysts are improved. Moreover, the oxygen species of the modified catalysts become easier to be reduced. Therefore, the oxidation activity over the catalysts was improved, except for the one modified by Pb oxide. Manganese oxide demonstrates the best promotional effects for SnO2. Using an X‐ray diffraction extrapolation method, the lattice capacity of SnO2 for Mn2O3 was 0.135 g Mn2O3/g SnO2, which indicates that to form stable solid solution, only 21%Sn4+cations in the lattice can be maximally replaced by Mn3+. If the amount of Mn3+cations is over the capacity, Mn2O3 will be formed, which is not favorable for the activity of the catalysts. The Sn rich samples with only Sn‐Mn solid solution phase show higher activity than the ones with excess Mn2O3 species.
基金supported by the National Nature Science Foundation of China (Project No.20576023)the Natural Science Foundation of Guangdong Province (Project No.06025660).
文摘The Cu-Zr-Ce-O catalysts prepared using the coprecipitation method exhibited better catalytic performance for CO selective oxidation. The Cu-Zr-Ce-O catalysts pretreated with different methods were studied by CO-TPR and XPS techniques. The results showed that the Cu-Zr-Ce-O catalyst pretreated with oxygen exhibited the best catalytic performance and had the widest operating temperature window, with CO conversion above 99% from 160 to 200 ℃. The O2 pretreatment caused an enrichment of the oxygen storaged on the Cu active species and promoted the conversion of adsorbed oxygen into surface lattice oxygen. It also improved the amount of Cu+/Cu^2+ ionic pair, and then facilitated the formation of CuO active species on the catalyst for selective CO oxidation.
基金the Shanxi Provin-cial Youth Science and Technology Research Fund (No.2008021009-2) for the financial support to this project
文摘The removal of hydrogen sulfide from gas plays an important role in rational utilization of resources and environ- mental protection. In this paper, the process of hydrogen sulfide removal by wet oxidation method in a rotating packed bed was investigated in a scale for treating 10 000 Nm3/h of gas. On the basis of studying the influence of the species and con- centration of alkali source, the liquid/gas volume ratio, the high gravity factor, and the hydrogen sulfide content in feed gas on the desulfurization effect, the suitable technological conditions were obtained. The hydrogen sulfide removal efficiency could reach 98.0% under these conditions. The results of continuous operation of process facilities showed that the high gravity method has many merits including higher desulfurization rate, good stability in operation, lower liquid/gas volume ratio, greater operation elasticity, and apparent energy saving effects.
基金financially supported by the National Key Research and Development Program of China (No.2021YFB4001400)。
文摘The reduced sealing difficulty of tubular solid oxide fuel cells(SOFCs)makes the stacking of tubular cell groups relatively easy,and the thermal stress constraints during stack operation are smaller,which helps the stack to operate stably for a long time.The special design of tubular SOFC structures can completely solve the problem of high-temperature sealing,especially in the design of multiple single-cell series integrated into one tube,where each cell tube is equivalent to a small electric stack,with unique characteristics of high voltage and low current output,which can significantly reduce the ohmic polarization loss of tubular cells.This paper provides an overview of typical tubular SOFC structural designs both domestically and internationally.Based on the geometric structure of tubular SOFCs,they can be divided into bamboo tubes,bamboo flat tubes,single-section tubes,and single-section flat tube structures.Meanwhile,this article provides an overview of commonly used materials and preparation methods for tubular SOFCs,including commonly used materials and preparation methods for support and functional layers,as well as a comparison of commonly used preparation methods for microtubule SOFCs,It introduced the three most important parts of building a fuel cell stack:manifold,current collector,and ceramic adhesive,and also provided a detailed introduction to the power generation systems of different tubular SOFCs,Finally,the development prospects of tubular SOFCs were discussed.
基金The work was supported by the National Basic Research Program of China (973 Program, No. 2004CB719504)
文摘The CuO-CeO2 catalyst prepared by chelating method has a superior catalytic performance for the preferential oxidation of CO in rich hydrogen, compared with the CuO-CeO2 catalyst prepared by coprecipitation method. The CO conversions over these catalysts, at 120 ℃ and 120000 ml/(g-h) in the absence of CO2 and H2O, are 99.6% and 88.6%, respectively, and the selectivity of O2 over these catalysts is very close (i.e. 51.3% and 55.8%, respectively). The influence of certain factors such as hydrogen concentration, carbon monoxide concentration, H2O, O2/CO ratios, and space velocity on the catalytic performance of CuO-CeO2 catalyst prepared by chelating method is also studied. The results show that the addition of hydrogen and H2O has a negative effect on the catalytic performance of CuO-CeO2 catalyst, however, the variation of space velocity and the O2/CO ratio causes a comparatively slight influence.
基金Project supported by the National Natural Science Foundation of China (Nos. 90505015 and10702035)
文摘High-temperature oxidation is an important property to evaluate thermal protection materials. However, since oxidation is a complex process involving microstructure evolution, its quantitative analysis has always been a challenge. In this work, a phase field method (PFM) based on the thermodynamics theory is developed to simulate the oxidation behavior and oxidation induced growth stress. It involves microstructure evolution and solves the problem of quantitatively computational analysis for the oxidation behavior and growth stress. Employing this method, the diffusion process, oxidation performance, and stress evolution axe predicted for Fe-Cr-A1-Y alloys. The numerical results agree well with the experimental data. The linear relationship between the maximum growth stress and the environment oxygen concentration is found. PFM provides a powerful tool to investigate high-temperature oxidation in complex environments.
文摘The influence of different cooking and smoking methods (boiling, frying, frying + boiling, hot and cold smoking) on oxidation and fatty acid composition of catfish (Arius maculatus) commercialized on the Wouri river coast was evaluated including commonly used analytical indexes (peroxide and acid values)and physical analysis by Fourier transform infrared (FTIR) spectroscopy. The mean moisture, protein, ash and fat contents of raw fish were 75.88 ± 0.55;64.24 ± 0.14;10.98 ± 0.31 and 23.02 ± 0.88 respectively. All these treatments provoke the modification of the quality indexes. Lipid deterioration, thermolysis and lipid oxidation occurred throughout the treatment. Peroxide value decreased for all cooked and smoked catfish, while free fatty acids of smoked sample increased. The FTIR applied to evaluate lipid oxidation in extracted lipid clearly provided a better picture of the oxidation progress and led to a similar conclusion with chemical analysis. Boiled, bleaching hot and bleaching cold smoking were found to be the suitable treatment methods for catfish because they gave it a high nutritive value compared to other smoking methods.
文摘The oil oxidation characteristics of the whole temperature regions from 30 ℃ to 600 ℃ during oil reservoir air injection were revealed by experiments. The whole oil oxidation temperature regions were divided into four different parts: dissolving and inflation region, low temperature oxidation region, medium temperature oxidation region and high temperature oxidation region. The reaction mechanisms of different regions were explained. Based on the oil oxidation characteristics and filed tests results, light oil reservoirs air injection development methods were divided into two types: oxygen-reducing air flooding and air flooding;heavy oil reservoirs air injection in-situ combustion development methods were divided into two types: medium temperature in-situ combustion and high temperature in-situ combustion. When the reservoir temperature is lower than 120 ℃, oxygen-reducing air flooding should be used for light oil reservoir development. When the reservoir temperature is higher than 120 ℃, air flooding method should be used for light oil reservoir development. For a normal heavy oil reservoir, when the combustion front temperature is lower than 400 ℃, the development method is medium temperature in-situ combustion. For a heavy oil reservoir with high oil resin and asphalting contents, when the combustion front temperature is higher than 450 ℃, the development method at this condition is high temperature in-situ combustion. Ten years field tests of air injection carried out by PetroChina proved that air has advantages in technical, economical and gas source aspects compared with other gas agents for oilfield gas injection development. Air injection development can be used in low/super-low permeability light oil reservoirs, medium and high permeability light oil reservoirs and heavy oil reservoirs. Air is a very promising gas flooding agent.
基金supported by the Russian Science Foundation(grant No.22-19-00037),https://rscf.ru/project/22-19-00037/.
文摘The hydrothermal synthesis of In_(2)O_(3)and CeO_(2)–In_(2)O_(3)is investigated as well as the properties of sensor layers based on these compounds.During the synthesis of In_(2)O_(3),intermediate products In(OH)_(3)and InOOH are formed,which are the precursors of stable cubic(c-In_(2)O_(3))and metastable rhombohedral(rh-In_(2)O_(3))phases,respectively.A transition from c-In_(2)O_(3)to rh-In_(2)O_(3)is observed with the addition of CeO_(2).The introduction of cerium into rh-In_(2)O_(3)results in a decrease in the sensor response to hydrogen,while it increases in composites based on c-In_(2)O_(3).The data on the sensor activity of the composites correlate with XPS results in which CeO_(2)causes a decrease in the concentrations of chemisorbed oxygen and oxygen vacancies in rh-In_(2)O_(3).The reverse situation is observed in composites based on c-In_(2)O_(3).Compared to In_(2)O_(3)and CeO_(2)–In_(2)O_(3)obtained by other methods,the synthesized composites demonstrate maximum response to H_(2)at low temperatures by 70–100℃,and have short response time(0.2–0.5 s),short recovery time(6–7 s),and long-term stability.A model is proposed for the dependence of sensitivity on the direction of electron transfer between In_(2)O_(3)and CeO_(2).
基金the National Key R&D Program of China(No.2018YFB1502201)the Guangdong Basic and Applied Basic Research Foundation,China(No.2020A1515010551).
文摘For present solid oxide fuel cells(SOFCs),rapid performance degradation is observed in the initial aging process,and the dis-cussion of the degradation mechanism necessitates quantitative analysis.Herein,focused ion beam-scanning electron microscopy was em-ployed to characterize and reconstruct the ceramic microstructures of SOFC anodes.The lattice Boltzmann method(LBM)simulation of multiphysical and electrochemical processes in the reconstructed models was performed.Two samples collected from industrial-size cells were characterized,including a reduced reference cell and a cell with an initial aging process.Statistical parameters of the reconstructed microstructures revealed a significant decrease in the active triple-phase boundary and Ni connectivity in the aged cell compared with the reference cell.The LBM simulation revealed that activity degradation is dominant compared with microstructural degradation during the initial aging process,and the electrochemical reactions spread to the support layer in the aged cell.The microstructural and activity de-gradations are attributed to Ni migration and coarsening.
文摘The systematic method for constructing Lewis representations is a method for representing chemical bonds between atoms in a molecule. It uses symbols to represent the valence electrons of the atoms involved in the bond. Using a number of rules in a defined order, it is often better suited to complicated cases than the Lewis representation of atoms. This method allows us to determine the formal charge and oxidation number of each atom in the edifice more efficiently than other methods.
基金supported by National Key R&D Program of China(2021YFA1502803)the National Natural Science Foundation of China(NSFC)(21972066,91745202)+3 种基金NSFC-Royal Society Joint Program(21661130149)L.P.thanks the Royal Society and Newton Fund for a Royal Society-Newton Advanced Fellowshipsupported by the Research Funds for the Frontiers Science Centre for Critical Earth Material Cycling,Nanjing Universitya Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions.
文摘Recent advances in utilizing ^(17)O isotopic labeling methods for solid-state nuclear magnetic resonance(NMR)investigations of metal oxides for lithium-ion batteries have yielded extensive insights into their structural and dynamic details.Herein,we commence with a brief introduction to recent research on lithium-ion battery oxide materials studied using ^(17)O solid-state NMR spectroscopy.Then we delve into a review of ^(17)O isotopic labeling methods for tagging oxygen sites in both the bulk and surfaces of metal oxides.At last,the unresolved problems and the future research directions for advancing the ^(17)O labeling technique are discussed.
基金supported by the National Natural Science Foundation of China(21577088)~~
文摘Co3O4 catalysts prepared with different precipitants(NH3·H2O,KOH,NH4HCO3,K2CO3 and KHCO3)were investigated for the oxidation of formaldehyde(HCHO).Among these,KHCO3-precipitated Co3O4(KHCO3-Co) was the most active low-temperature catalyst,and was able to completely oxidize HCHO at the 100-ppm level to CO2 at 90℃.In situ diffuse reflectance infrared spectroscopy demonstrated that hydroxyl groups on the catalyst surface were regenerated by K~+ and CO3^(2-),thus promoting the oxidation of HCHO.Moreover,H2-temperature programmed reduction and X-ray photoelectron spectroscopy showed that employing KHCO3 as the precipitant increased the Co^3+/Co^2+molar ratio on the surface of the Co3O4 catalyst,thus further promoting oxidation.Structural characterization revealed that catalysts precipitated with carbonate or bicarbonate reagents exhibited greater specific surface areas and pore volumes.Overall,these data suggest that the high activity observed during the Co3O4 catalyzed oxidation of HCHO can be primarily attributed to the presence of K~+ and CO3^(2-) on the Co3O4 surface and the favorable Co^3+/Co^2+ ratio.
基金supported by the National Science Foundation for Young Scientists of China (51202171)~~
文摘A molten salt method was developed to prepare porous La1‐xSrxMn0.8Fe0.2O3 (0≤ x ≤ 0.6) micro‐spheres using hierarchical porous δ‐MnO2 microspheres as a template in eutectic NaNO3‐KNO3. X‐ray diffraction patterns showed that single phase LaMn0.8Fe0.2O3 with good crystallinity was syn‐thesized at 450℃ after 4 h. Transmission electron microscope images exhibited that the LaMn0.8Fe0.2O3 sample obtained at 450?? after 4 h possessed a porous spherical morphology com‐posed of aggregated nanocrystallites. Field emission scanning electron microscope images indicated that the growth of the porous LaMn0.8Fe0.2O3 microspheres has two stages. SEM pictures showed that a higher calcination temperature than 450?? had an adverse effect on the formation of a po‐rous spherical structure. The LaMn0.8Fe0.2O3 sample obtained at 450?? after 4 h displayed a high BET surface area of 55.73 m2/g with a pore size of 9.38 nm. Fourier transform infrared spectra suggested that Sr2+ions entered the A sites and induced a decrease of the binding energy between Mn and O. The CO conversion with the La1‐xSrxMn0.8Fe0.2O3 (0≤x≤0.6) samples indicated that the La0.4Sr0.6Mn0.8Fe0.2O3 sample had the best catalytic activity and stability. Further analysis by X‐ray photoelectron spectroscopy demonstrated that Sr2+doping altered the content of Mn4+ions, oxygen vacancies and adsorbed oxygen species on the surface, which affected the catalytic performance for CO oxidation.
文摘A series of rare earth hydroxide and oxide nanoparticles have been prepared by precipitation method with alcohol as the dispersive and protective reagent. Transmission electron microscope (TEM) images indicate that the particles are spherical in shape and smaller than 100 nm in size. The crystallite sizes of cubic Ln2O3 have lanthanide shrinking effect, while average crystal lattice distortion rates possess lanthanide swelling effect. The diffraction peak intensity of heavy rare earth oxide nanometer powders is remarkably stronger than that of light rare earth oxide nanometer powders. The variation of diffraction intensity with atomic number presents an inverted W type, forming a double peak structure. Fourier transform infrared (FTIR) spectrums reveal that Ln2O3 nanopowders have higher surface activity than that of ordinary Ln2O3 powders. The UV-vis spectra show that Ln-O bond of these particles is slightly blue-shifted, and its absorption intensity decreases.
基金Supported by the "863" Program of Science and Technology Ministry of China(Nos.2006AA05Z137, 2007AA05Z143 and 2007AA05Z159)National Natural Science Foundation of China(Nos.20433060, 20473038, 20573057 and 20703043)the Natural Science Foundation of Jiangsu Province, China(No.BK2006224).
文摘A carbon supported Pd(Pd/C) catalyst used as the anodic catalyst in the direct formic acid fuel cells(DFAFC) was prepared via the improved complex reduction method with sodium ethylenediamine tetracetate(EDTA) as stabilizer and complexing agent. This method is very simple. The average size of the Pd particles in the Pd/C catalyst prepared with the improved complex reduction method is as small as about 2.1 nm and the Pd particles in the Pd/C catalyst possess an excellent uniformity. The Pd/C catalyst shows a high electrocatalytic activity and stability for the formic acid oxidation.
基金Projects(51774070,51204054)supported by the National Natural Science Foundation of ChinaProject(N150204009)supported by the Ministry of Education Basic Scientific Research Business Expenses,ChinaProject(2007CB613603)supported by the National Basic Research Program of China
文摘The orthogonal test was used to optimize the reaction conditions of roasting zinc oxide ore with NaOH aiming to comprehensively utilize zinc oxide ore.The optimized reaction conditions were molar ratio of NaOH to zinc oxide ore 6:1,roasting temperature 450°C,holding time 150 min.The molar ratio of NaOH to zinc oxide ore was the most predominant factor affecting the extraction ratios of zinc oxide and silica.The mineral phase transformations were investigated by testing the phases of specimens obtained at different temperatures.The process was that silica reacted with molten NaOH to form Na_2SiO_3 at first,then transformed into Na_4SiO_4 with temperature rising.ZnCO_3 and its decomposing product ZnO reacted with NaOH to form Na_2ZnO_2.Na_2ZnSiO_4was also obtained.The reaction rate was investigated using unreacted shrinking core model.Two models used were chemical reaction at the particle surface and diffusion through the product layer.The results indicated that the reaction rate was combine-controlled by two models.The activation energy and frequency factor were obtained as 24.12 k J/mol and 0.0682,respectively.