The further development of catalytic elements has been plagued by activation and binary problems.The automatic shift model that has emerged in recent years helps components achieve full range.However,the detection dat...The further development of catalytic elements has been plagued by activation and binary problems.The automatic shift model that has emerged in recent years helps components achieve full range.However,the detection data still remains unstable in the shift area(7%∼13%).This paper proposes a Catalytic Combustion and Thermal Conductivity(CCTC)model for the specified range,which can be explained fromtwo aspects based on the existing methods.On the one hand,it uses iterative location search to process heterogeneous data,judges the prediction position of data points,and then givesweight evaluation.On the other hand,it corrects the abnormal points,determines the abnormal points in the horizontal direction,and gives the replacement value through the data of adjacent points.The experimental results show that the CCTC model reduces the sum of variance from 17 of the automatic shift model to 13,and the comparison of experimental variance is reduced by 23%.In the full-scale real-time data,the experimental variance of CCTC model and automatic shift model is reduced by 18%.In conclusion,CCTC is a cross section stability framework for full-scale methane measurement,in which the specified heterogeneous combination and anomaly point correction methods improve the stability.展开更多
Composite solid propellants(CSPs) have widely been used as main energy source for propelling the rockets in both space and military applications. Internal ballistic parameters of rockets like characteristic exhaust ve...Composite solid propellants(CSPs) have widely been used as main energy source for propelling the rockets in both space and military applications. Internal ballistic parameters of rockets like characteristic exhaust velocity, specific impulse, thrust, burning rate etc., are measured to assess and control the performance of rocket motors. The burn rate of solid propellants has been considered as most vital parameter for design of solid rocket motors to meet specific mission requirements. The burning rate of solid propellants can be tailored by using different constituents, extent of oxidizer loading and its particle size and more commonly by incorporating suitable combustion catalysts. Various metal oxides(MOs),complexes, metal powders and metal alloys have shown positive catalytic behaviour during the combustion of CSPs. These are usually solid-state catalysts that play multiple roles in combustion of CSPs such as reduction in activation energy, enhancement of rate of reaction, modification of sequences in reaction-phase, influence on condensed-phase combustion and participation in combustion process in gas-phase reactions. The application of nanoscale catalysts in CSPs has increased considerably in recent past due to their superior catalytic properties as compared to their bulk-sized counterparts. A large surface-to-volume ratio and quantum size effect of nanocatalysts are considered to be plausible reasons for improving the combustion characteristics of propellants. Several efforts have been made to produce nanoscale combustion catalysts for advanced propellant formulations to improve their energetics. The work done so far is largely scattered. In this review, an effort has been made to introduce various combustion catalysts having at least a metallic entity. Recent developments of nanoscale combustion catalysts with their specific merits are discussed. The combustion chemistry of a typical CSP is briefly discussed for providing a better understanding on role of combustion catalysts in burning rate enhancement. Available information on different types of combustion nanocatalysts is also presented with critical comments.展开更多
LaMnO3was prepared by citrate sol‐gel,coprecipitation,hard template,and hydrothermal methods,respectively,and its catalytic performance for the combustion of vinyl chloride was investigated.N2adsorption‐desorption,X...LaMnO3was prepared by citrate sol‐gel,coprecipitation,hard template,and hydrothermal methods,respectively,and its catalytic performance for the combustion of vinyl chloride was investigated.N2adsorption‐desorption,X‐ray diffraction(XRD),Raman spectroscopy(Raman),O2temperature programmed desorption(O2‐TPD),H2temperature programmed surface reaction(H2‐TPR)and X‐ray photoelectron spectroscopy(XPS)were used to characterize the physicochemical properties of the LaMnO3samples.The preparation methods had obvious effects on the distribution of oxygen and manganese species on the catalyst surface.The reaction followed the suprafacial mechanism;the activity corresponded with the high amount of Mn4+and adsorbed oxygen species.LaMnO3prepared by the citrate sol‐gel method had the best performance for vinyl chloride combustion with T90of182°C.The optimal activity was attributed to the improved redox capability of Mn4+/Mn3+.More available adsorbed oxygen and Mn4+species on the surface were mainly responsible for the remarkable enhancement of the catalytic activity.展开更多
The nano ZrO2-supported copper-based catalysts for methane combustion were investigated by means of N2 adsorption, TEM, XRD, H2-TPR techniques and the test of methane oxidation. Two kinds of ZrO2 were used as support,...The nano ZrO2-supported copper-based catalysts for methane combustion were investigated by means of N2 adsorption, TEM, XRD, H2-TPR techniques and the test of methane oxidation. Two kinds of ZrO2 were used as support, one (ZrO2-1) was obtained from the commercial ZrO2 and the other (ZrO2-2) was issued from the thermal decomposition of zirconium nitrate. It was found that the CuO/ZrO2-2 catalyst was more active than CuO/ZrO2-1. N2 adsorption, H2-TPR and XRD measurements showed that larger surface area, better reduction property, presence of tetragonal ZrO2 and higher dispersion of active component for CuO/ZrO2-2 than that of CuO/ZrO2-1. These factors could be the dominating reasons for its higher activity for methane combustion.展开更多
Nanostructure K2NiF4 type oxides La2-xKxCuO4 complex oxides were prepared using the Sol-Gel method, characterized by X-Ray Diffraction (XRD), Fourier Transform Infrared (FT-IR), and Scanning Electron Microscopy (...Nanostructure K2NiF4 type oxides La2-xKxCuO4 complex oxides were prepared using the Sol-Gel method, characterized by X-Ray Diffraction (XRD), Fourier Transform Infrared (FT-IR), and Scanning Electron Microscopy (SEM). The catalytic activity for soot combustion was evaluated by the Temperature-Programmed Reaction (TPO) technique. The results demonstrated that the substitution quality of K^+ for La^3+ at the A-site would increase the catalytic activities of La2-xKxCuO4 for soot combustion greatly; the substitution quality affected the structure and catalytic activity obviously. The La1.8K0.2CuO4 complex oxides with tetrahedral structures had the best catalytic activity for soot combustion, and the ignition temperature of soot combustion was lowered from 490 to 320 ℃.展开更多
The copper based catalysts, CuO/T-Al2O3, CuO/y-Al2O3-cordierite (Cord) and CuO/Cord, were prepared by impregnation method. The catalytic activity of the catalysts was tested in absence and presence of water vapor,an...The copper based catalysts, CuO/T-Al2O3, CuO/y-Al2O3-cordierite (Cord) and CuO/Cord, were prepared by impregnation method. The catalytic activity of the catalysts was tested in absence and presence of water vapor,and the catalysts were characterized. Temperature program desorption (TPD) experiments or toluene and water on the catalysts were carried out. The influence of water vapor on the activity of the catalysts was discussed. Results showed that addition of the water vapor has a significant negative effect on the catalytic activity of the catalysts.The higher the concentration of the Water vapor in feed steam was, the lower the catalytic activity of the copper based catalysts became, which could be mainly ascribed to the competition of water molecules with toluene molecules for adsorption on the catalyst surfaces. TPD experiments showed that the strength of the interaction between water molecules and three catalysts followed the order: CuO/γ-Al2O3〉CuO/γ-Al2O3-Cord〉CuO/Cord. As a consequence of that, the degree of degradation in the catalytic activity of these three catalysts by the water vapor followed the order: CuO/γ-Al2O3〉CuO/y-Al2O3-Cord〉CuO/Cord. However, the negative effect of the water vapor was reversible.展开更多
Perovskite oxide LaCoO_3 methane catalytic material was synthesized with citric acid complexation and bubbling method. The effect of doped cerium was studied on the series of La_(1-x)Ce_xCoO_(3+δ) materials by means...Perovskite oxide LaCoO_3 methane catalytic material was synthesized with citric acid complexation and bubbling method. The effect of doped cerium was studied on the series of La_(1-x)Ce_xCoO_(3+δ) materials by means of BET, XRD and SEM techniques. Their catalytic behaviors were studied with methane catalytic complete combustion as probe reaction. The results show that doped cerium has great effect on crystal phase formation. When doped cerium is less than 0.3 ((molar) ratio), the crystal phase of oxide has little changed. When doped cerium is up to 0.5, Co_3O_4 phase is obviously discovered and the perfectibility of LaCoO_3 perovskite crystal phase is deteriorated. When x is over 0.7, perovskite crystal phase is weakened or completely disappeared. Considering the crystal phase of oxides, the optimum doped cerium is about 0.3. The perovskite oxides can be formed at a low calcinations temperature of 700 ℃. When x is 0.3, the highest catalytic activity of T_(10%) (390 ℃) and T_(90%) (603 ℃) is obtained on the series of La_(1-x)Ce_xCoO_(3+δ) materials calcined at 800 ℃.展开更多
Catalytic combustion of CH4/air in monolith reactor is simulated using a commercial computational fluid dy-namic code. The user subroutines to describe the heterogeneous reaction at the channel wall in a single channe...Catalytic combustion of CH4/air in monolith reactor is simulated using a commercial computational fluid dy-namic code. The user subroutines to describe the heterogeneous reaction at the channel wall in a single channel and at the channel walls in the whole reactor are incorporated into the program. The correctness of the method is verified by com-paring the simulation results with the experimental data for the whole reactor. Furthermore, it is observed that the model based on the whole reactor is more reasonable than that based on a single channel. Therefore, using the former, the effects of operating conditions such as inlet gas velocity, temperature, concentration and catalyst loading on methane conversion are investigated.展开更多
Changes are needed to improve the efficiency and lower the CO_(2)emissions of traditional coal-fired power generation,which is the main source of global CO_(2)emissions.The integrated gasification fuel cell(IGFC)proce...Changes are needed to improve the efficiency and lower the CO_(2)emissions of traditional coal-fired power generation,which is the main source of global CO_(2)emissions.The integrated gasification fuel cell(IGFC)process,which combines coal gasification and high-temperature fuel cells,was proposed in 2017 to improve the efficiency of coal-based power generation and reduce CO_(2)emissions.Supported by the National Key R&D Program of China,the IGFC for nearzero CO_(2)emissions program was enacted with the goal of achieving near-zero CO_(2)emissions based on(1)catalytic combustion of the flue gas from solid oxide fuel cell(SOFC)stacks and(2)CO_(2)conversion using solid oxide electrolysis cells(SOECs).In this work,we investigated a kW-level catalytic combustion burner and SOEC stack,evaluated the electrochemical performance of the SOEC stack in H2O electrolysis and H2O/CO_(2)co-electrolysis,and established a multiscale and multi-physical coupling simulation model of SOFCs and SOECs.The process developed in this work paves the way for the demonstration and deployment of IGFC technology in the future.展开更多
In order to enhance catalytic combustion efficiency, a premixed hydrogen /air combustion model of the micro turbine engine is established under different excess air ratio, inlet velocity and heat transfer coefficient....In order to enhance catalytic combustion efficiency, a premixed hydrogen /air combustion model of the micro turbine engine is established under different excess air ratio, inlet velocity and heat transfer coefficient. And effects of inlet velocity, excess air coefficient and heat transfer coefficient on the catalytic combustion efficiency of the hydrogen have been analyzed by the FLUENT with CHEMKIN reaction mechanisms and the fuzzy grey relation theory. It is showed that inlet velocity has a more intuitive influence on the catalytic combustion efficiency of the hydrogen. A higher efficiency can be obtained with a lower inlet velocity. The optimum excess air coefficient is in the range of 0.94 to 1.0, the catalytic combustion efficiency of the hydrogen will be declined if the excess air coefficient exceeded 1.0. The effect of heat transfer coefficient on the catalytic combustion efficiency of the hydrogen mainly embodies in the case of the excess air coefficient exceeded 1.0, however, the effect will be declined if the heat transfer coefficient exceeded 4.0. The fuzzy grey relation degrees of the inlet velocity, heat transfer coefficient and excess air coefficient on the catalytic combustion efficiency of the hydrogen are 0.640945, 0.633214 and 0.547892 respectively.展开更多
Five monolithic catalysts with low noble metal content were prepared by irnmerge method (Pt/γ=Al2O3, Pt/La-Al2O3, Pt/YSZ-AI203, Pt+Pd/La-Al2O3 and Pd/La-Al2O3) and their activity measurements were carried out in a...Five monolithic catalysts with low noble metal content were prepared by irnmerge method (Pt/γ=Al2O3, Pt/La-Al2O3, Pt/YSZ-AI203, Pt+Pd/La-Al2O3 and Pd/La-Al2O3) and their activity measurements were carried out in a conventional fixed-bed flow reactor. The results show that La-Al2O3 can promote activity of the prepared catalysts and can decrease the complete conversion temperature of cooking fume. The Pt/La-Al2O3 catalyst has the highest activity and can be applied in wide range of gas hourly space velocity (GHSV). Some characterizations (XRD, TPR) were carried out with the objective to explain differences in catalytic behaviors. The prepared catalyst showed a great potential for application.展开更多
Silicalite-1(S1)foam was functionalized by supporting manganese-cobalt(Mn-Co)mixed oxides to develop the structured hierarchical catalyst(Mn-Co@SlF)for catalytic combustion for the first time.The self-supporting S1 fo...Silicalite-1(S1)foam was functionalized by supporting manganese-cobalt(Mn-Co)mixed oxides to develop the structured hierarchical catalyst(Mn-Co@SlF)for catalytic combustion for the first time.The self-supporting S1 foam with hierarchical porosity was prepared via hydrothermal synthesis with polyurethane(PU)foam as the template.Subsequently,Mn-Co oxide nano sheets were uniformly grown on the surface of S1 foams under hydrothermal conditions to prepare the structured hierarchical catalyst with specific surface area of 354 m^2·g^-1,micropore volume of 0.141 cm^3·g^-1 and total pore volume of 0.217 cm3·g^-1,as well as a good capacity to adsorb toluene(1.7 mmol·g^-1 at p/p0=0.99).Comparative catalytic combustion of toluene of over developed structured catalyst Mn-Co@SlF was performed against the control catalysts of bulk Mn-Co@S1(i.e.,the crushed Mn-Co@SlF)and unsupported Mn-Co oxides(i.e.,Mn-Co).Mn-Co@SlF exhibited comparatively the best catalytic performance,that is,complete and stable toluene conversion at 2480 C over 65 h due to the synergy between Mn-Co oxides and S1 foam,which provided a large number of oxygen vacancies,high redox capacity.In addition,the hierarchical porous structure also improved the accessibility of active sites and facilitated the global mass transfer across the catalyst bed,being beneficial to the catalysis and catalyst longevity.展开更多
Supported manganese oxide catalysts were prepared by incipient wetness impregnation method for methane catalytic combustion, and effects of the support (Al2O3, SiO2 and TiO2) and Mn loading were investigated. These ...Supported manganese oxide catalysts were prepared by incipient wetness impregnation method for methane catalytic combustion, and effects of the support (Al2O3, SiO2 and TiO2) and Mn loading were investigated. These catalysts were characterized with N2 adsorption, X-ray diffraction, X-ray photoelectron spectroscopy and temperature-programmed reduction techniques. Methane conversion varied in a large range depending on supports or Mn loading. Al2O3 supported 15% Mn catalyst exhibited better activity toward methane catalytic oxidation. The manganese state and oxygen species played an important role in the catalytic performance,展开更多
MnO_x/Al_2O_3 and MnO_x/ZrO_2-Al_2O_3 catalysts were prepared by incipientwetness impregnation of Mn(CH_3COO)_2 on the corresponding supports, followed by thecharacterization using X-ray diffraction (XRD), temperature...MnO_x/Al_2O_3 and MnO_x/ZrO_2-Al_2O_3 catalysts were prepared by incipientwetness impregnation of Mn(CH_3COO)_2 on the corresponding supports, followed by thecharacterization using X-ray diffraction (XRD), temperature programmed reduction (TPR) and BETsurface area techniques. The result shows the BET surface area of ZrO_2-Al_2O_3 is lower than thatof Al_2O_3 due to the loading of ZrO_2. However the resulted MnO_x/ZrO_2-Al_2O_3 catalyst exhibitshigher activity for methane combustion than MnO_x/Al_2O_3, because the addition of ZrO_2 ontoAl_2O_3 is beneficial for the dispersion of Mn species and the improvement of the lattice oxygenactivity in MnO_x, subsequently the activation of methane during combustion. The optimum loading ofZr in MnO_x/ZrO_2-Al_2O_3 is in the range of 5%-10% correlated with the calcination temperatures ofcatalyst supports.展开更多
This work is focused on the performance prediction of pilot scale catalytic reverse flow reactors used for combustion of lean methane-air mixtures. An unsteady one-dimensional heterogeneous model for the reactor was e...This work is focused on the performance prediction of pilot scale catalytic reverse flow reactors used for combustion of lean methane-air mixtures. An unsteady one-dimensional heterogeneous model for the reactor was established to account for the influence of the reactor wall on the heat transfer. Results of the simulation indicate that feed concentration, switch time and compensatory temperature impose important influence on the performance of the reactor. The amount of the heat extracted from the mid-section of the reactor can be optimized via adjusting the parameters mentioned above. At the optimal operating conditions, Le. switching time of 400 s, feed concentration of 1% (by volume), and insulation layer temperature of 343 K, the axial temperature of the reactor revealed a comparatively symmetrical "saddle" distribution, indicating a favorable operating status of the catalytic reverse flow reactor.展开更多
In this paper the premixed catalytic combustion emissions such as CO, unburned hydrocarbon (UHC), NOx and the temperature distribution in the catalytic monolith with ultra low concentration of Pd were studied. Three t...In this paper the premixed catalytic combustion emissions such as CO, unburned hydrocarbon (UHC), NOx and the temperature distribution in the catalytic monolith with ultra low concentration of Pd were studied. Three types of monoliths were used for experiments and the temperature of preheated air was respectively 50℃ , 100℃ and 200℃ . The results showed that preheated air made radial temperature in the catalytic monolith uniform which helped to avoid local hot spots so as to decrease NOx emission. The experiment also proved that the shorter monolith showed much better catalytic combustion performance than longer one and the temperature at the exit of the shorter monolith was relatively lower. On the contrary, the temperature was higher in the longer monolith and the lethal NOx emission was slightly increased.展开更多
The catalytic activity of Cu-ZSM-5 in trichloroethylene (TCE) combustion increases with the increasing skeletal Cu amount and however decreases with the increase of surface amorphous CuO, which is detected by infrar...The catalytic activity of Cu-ZSM-5 in trichloroethylene (TCE) combustion increases with the increasing skeletal Cu amount and however decreases with the increase of surface amorphous CuO, which is detected by infrared spectroscopy (IR) and diffuse reflectance ultraviolet-visible spectroscopy (DRS-UV-vis), therefore the skeletal Cu species are concluded to be the active sites for the TCE combustion.展开更多
A natural montmorillonite, produced from Laiyang of Shandong Province, was pillared by Tipolyeations to form Ti-pillared clay (Ti-PILC), and characterized by BET surface area, infrared spectra and thermal analysis. Th...A natural montmorillonite, produced from Laiyang of Shandong Province, was pillared by Tipolyeations to form Ti-pillared clay (Ti-PILC), and characterized by BET surface area, infrared spectra and thermal analysis. The characterization results show that Ti-PILC has a larger surface area and more hydroxyl groups than that of the natural clay, thus was used as the catalytic carriers to prepare supported Cu catalysts (Cu/Ti-PILC). The 20%Cu/Ti-PILC with 10mmol/g of Ti/clay shows a high catalytic performance of methane combustion in the temperature range of 400 500℃.展开更多
The K2NiF4 type oxides, La2-x KxCuO4 complex oxides with nanometric size were prepared by sol-gel method. The characters of these samples were analyzed by H2-TPR, XRD, FT-IR and SEM. The catalytic activity for soot co...The K2NiF4 type oxides, La2-x KxCuO4 complex oxides with nanometric size were prepared by sol-gel method. The characters of these samples were analyzed by H2-TPR, XRD, FT-IR and SEM. The catalytic activity for soot combustion was evaluated by temperature-programmed reaction (TPO) technique. The results demonstrate that the substitution of K^+ for La^3+ at A-site will increase the catalytic activities of La2-xKxCuO4 to soot combustion greatly, and the substitution quantity affects the structure and catalytic activity obviously. The La1.8 K0.2 CuO4 complex oxides with tetrahedral structure has the best catalytic activity for soot removal reaction, the ignition temperature of soot combustion is decreased from 490 to 320℃.展开更多
Ce0.6Mn0.4O2 catalysts with different sources of manganese and Ce0.6-xZrxMn0.4O2 mixed oxide catalysts were prepared by coprecipitation method and were characterized by N2 adsorption-desorption,TPR,XRD,and XPS techniq...Ce0.6Mn0.4O2 catalysts with different sources of manganese and Ce0.6-xZrxMn0.4O2 mixed oxide catalysts were prepared by coprecipitation method and were characterized by N2 adsorption-desorption,TPR,XRD,and XPS techniques.The activities of the prepared catalysts for ethyl acetate combustion,and the effects of calcination temperature and space velocity on catalytic activity were investigated.The results showed that partial replacement of Mn(NO3)2 with KMnO4 as sources of manganese could improve activities of catalysts.Ce0.45Zr0.15Mn0.4O2 catalyst exhibited the best catalytic activity and high thermal stability,e.g.,T90 could be still below 210℃ even if space velocity was up to 20000h-1.展开更多
基金supported by Major Science and Technology Project of Sichuan Province[No.2022YFG0315,2022YFG0174]Sichuan Gas Turbine Research Institute stability support project of China Aero Engine Group Co.,Ltd[GJCZ-2019-59]Key project of Chengdu[No.2019-YF09-00044-CG].
文摘The further development of catalytic elements has been plagued by activation and binary problems.The automatic shift model that has emerged in recent years helps components achieve full range.However,the detection data still remains unstable in the shift area(7%∼13%).This paper proposes a Catalytic Combustion and Thermal Conductivity(CCTC)model for the specified range,which can be explained fromtwo aspects based on the existing methods.On the one hand,it uses iterative location search to process heterogeneous data,judges the prediction position of data points,and then givesweight evaluation.On the other hand,it corrects the abnormal points,determines the abnormal points in the horizontal direction,and gives the replacement value through the data of adjacent points.The experimental results show that the CCTC model reduces the sum of variance from 17 of the automatic shift model to 13,and the comparison of experimental variance is reduced by 23%.In the full-scale real-time data,the experimental variance of CCTC model and automatic shift model is reduced by 18%.In conclusion,CCTC is a cross section stability framework for full-scale methane measurement,in which the specified heterogeneous combination and anomaly point correction methods improve the stability.
文摘Composite solid propellants(CSPs) have widely been used as main energy source for propelling the rockets in both space and military applications. Internal ballistic parameters of rockets like characteristic exhaust velocity, specific impulse, thrust, burning rate etc., are measured to assess and control the performance of rocket motors. The burn rate of solid propellants has been considered as most vital parameter for design of solid rocket motors to meet specific mission requirements. The burning rate of solid propellants can be tailored by using different constituents, extent of oxidizer loading and its particle size and more commonly by incorporating suitable combustion catalysts. Various metal oxides(MOs),complexes, metal powders and metal alloys have shown positive catalytic behaviour during the combustion of CSPs. These are usually solid-state catalysts that play multiple roles in combustion of CSPs such as reduction in activation energy, enhancement of rate of reaction, modification of sequences in reaction-phase, influence on condensed-phase combustion and participation in combustion process in gas-phase reactions. The application of nanoscale catalysts in CSPs has increased considerably in recent past due to their superior catalytic properties as compared to their bulk-sized counterparts. A large surface-to-volume ratio and quantum size effect of nanocatalysts are considered to be plausible reasons for improving the combustion characteristics of propellants. Several efforts have been made to produce nanoscale combustion catalysts for advanced propellant formulations to improve their energetics. The work done so far is largely scattered. In this review, an effort has been made to introduce various combustion catalysts having at least a metallic entity. Recent developments of nanoscale combustion catalysts with their specific merits are discussed. The combustion chemistry of a typical CSP is briefly discussed for providing a better understanding on role of combustion catalysts in burning rate enhancement. Available information on different types of combustion nanocatalysts is also presented with critical comments.
基金supported by the National Basic Research Program of China (2013CB933201)the National Natural Science Foundation of China (21207037,21577035)the Commission of Science and Technology of Shanghai Municipality (15DZ1205305)~~
文摘LaMnO3was prepared by citrate sol‐gel,coprecipitation,hard template,and hydrothermal methods,respectively,and its catalytic performance for the combustion of vinyl chloride was investigated.N2adsorption‐desorption,X‐ray diffraction(XRD),Raman spectroscopy(Raman),O2temperature programmed desorption(O2‐TPD),H2temperature programmed surface reaction(H2‐TPR)and X‐ray photoelectron spectroscopy(XPS)were used to characterize the physicochemical properties of the LaMnO3samples.The preparation methods had obvious effects on the distribution of oxygen and manganese species on the catalyst surface.The reaction followed the suprafacial mechanism;the activity corresponded with the high amount of Mn4+and adsorbed oxygen species.LaMnO3prepared by the citrate sol‐gel method had the best performance for vinyl chloride combustion with T90of182°C.The optimal activity was attributed to the improved redox capability of Mn4+/Mn3+.More available adsorbed oxygen and Mn4+species on the surface were mainly responsible for the remarkable enhancement of the catalytic activity.
文摘The nano ZrO2-supported copper-based catalysts for methane combustion were investigated by means of N2 adsorption, TEM, XRD, H2-TPR techniques and the test of methane oxidation. Two kinds of ZrO2 were used as support, one (ZrO2-1) was obtained from the commercial ZrO2 and the other (ZrO2-2) was issued from the thermal decomposition of zirconium nitrate. It was found that the CuO/ZrO2-2 catalyst was more active than CuO/ZrO2-1. N2 adsorption, H2-TPR and XRD measurements showed that larger surface area, better reduction property, presence of tetragonal ZrO2 and higher dispersion of active component for CuO/ZrO2-2 than that of CuO/ZrO2-1. These factors could be the dominating reasons for its higher activity for methane combustion.
基金Beijing Municipal Education Committee Program (KM200710017006)
文摘Nanostructure K2NiF4 type oxides La2-xKxCuO4 complex oxides were prepared using the Sol-Gel method, characterized by X-Ray Diffraction (XRD), Fourier Transform Infrared (FT-IR), and Scanning Electron Microscopy (SEM). The catalytic activity for soot combustion was evaluated by the Temperature-Programmed Reaction (TPO) technique. The results demonstrated that the substitution quality of K^+ for La^3+ at the A-site would increase the catalytic activities of La2-xKxCuO4 for soot combustion greatly; the substitution quality affected the structure and catalytic activity obviously. The La1.8K0.2CuO4 complex oxides with tetrahedral structures had the best catalytic activity for soot combustion, and the ignition temperature of soot combustion was lowered from 490 to 320 ℃.
基金Supported by the National-Natural Science Foundation of China (20936001), the Natural Science Foundation of Guangdong Province, and the State Key Lab of Subtropical Building Science, South China University of Technology (x2yj C709028Z).
文摘The copper based catalysts, CuO/T-Al2O3, CuO/y-Al2O3-cordierite (Cord) and CuO/Cord, were prepared by impregnation method. The catalytic activity of the catalysts was tested in absence and presence of water vapor,and the catalysts were characterized. Temperature program desorption (TPD) experiments or toluene and water on the catalysts were carried out. The influence of water vapor on the activity of the catalysts was discussed. Results showed that addition of the water vapor has a significant negative effect on the catalytic activity of the catalysts.The higher the concentration of the Water vapor in feed steam was, the lower the catalytic activity of the copper based catalysts became, which could be mainly ascribed to the competition of water molecules with toluene molecules for adsorption on the catalyst surfaces. TPD experiments showed that the strength of the interaction between water molecules and three catalysts followed the order: CuO/γ-Al2O3〉CuO/γ-Al2O3-Cord〉CuO/Cord. As a consequence of that, the degree of degradation in the catalytic activity of these three catalysts by the water vapor followed the order: CuO/γ-Al2O3〉CuO/y-Al2O3-Cord〉CuO/Cord. However, the negative effect of the water vapor was reversible.
文摘Perovskite oxide LaCoO_3 methane catalytic material was synthesized with citric acid complexation and bubbling method. The effect of doped cerium was studied on the series of La_(1-x)Ce_xCoO_(3+δ) materials by means of BET, XRD and SEM techniques. Their catalytic behaviors were studied with methane catalytic complete combustion as probe reaction. The results show that doped cerium has great effect on crystal phase formation. When doped cerium is less than 0.3 ((molar) ratio), the crystal phase of oxide has little changed. When doped cerium is up to 0.5, Co_3O_4 phase is obviously discovered and the perfectibility of LaCoO_3 perovskite crystal phase is deteriorated. When x is over 0.7, perovskite crystal phase is weakened or completely disappeared. Considering the crystal phase of oxides, the optimum doped cerium is about 0.3. The perovskite oxides can be formed at a low calcinations temperature of 700 ℃. When x is 0.3, the highest catalytic activity of T_(10%) (390 ℃) and T_(90%) (603 ℃) is obtained on the series of La_(1-x)Ce_xCoO_(3+δ) materials calcined at 800 ℃.
基金Supported by the National Natural Science Foundation of China (No.20136010 and No.20376005).
文摘Catalytic combustion of CH4/air in monolith reactor is simulated using a commercial computational fluid dy-namic code. The user subroutines to describe the heterogeneous reaction at the channel wall in a single channel and at the channel walls in the whole reactor are incorporated into the program. The correctness of the method is verified by com-paring the simulation results with the experimental data for the whole reactor. Furthermore, it is observed that the model based on the whole reactor is more reasonable than that based on a single channel. Therefore, using the former, the effects of operating conditions such as inlet gas velocity, temperature, concentration and catalyst loading on methane conversion are investigated.
基金This work was financially supported by the National Key R&D Program of China(2017YFB0601904).
文摘Changes are needed to improve the efficiency and lower the CO_(2)emissions of traditional coal-fired power generation,which is the main source of global CO_(2)emissions.The integrated gasification fuel cell(IGFC)process,which combines coal gasification and high-temperature fuel cells,was proposed in 2017 to improve the efficiency of coal-based power generation and reduce CO_(2)emissions.Supported by the National Key R&D Program of China,the IGFC for nearzero CO_(2)emissions program was enacted with the goal of achieving near-zero CO_(2)emissions based on(1)catalytic combustion of the flue gas from solid oxide fuel cell(SOFC)stacks and(2)CO_(2)conversion using solid oxide electrolysis cells(SOECs).In this work,we investigated a kW-level catalytic combustion burner and SOEC stack,evaluated the electrochemical performance of the SOEC stack in H2O electrolysis and H2O/CO_(2)co-electrolysis,and established a multiscale and multi-physical coupling simulation model of SOFCs and SOECs.The process developed in this work paves the way for the demonstration and deployment of IGFC technology in the future.
基金Project(51776062) supported by the National Natural Science Foundation of ChinaProject(201208430262) supported by the National Studying Abroad Foundation Project of the China Scholarship Council
文摘In order to enhance catalytic combustion efficiency, a premixed hydrogen /air combustion model of the micro turbine engine is established under different excess air ratio, inlet velocity and heat transfer coefficient. And effects of inlet velocity, excess air coefficient and heat transfer coefficient on the catalytic combustion efficiency of the hydrogen have been analyzed by the FLUENT with CHEMKIN reaction mechanisms and the fuzzy grey relation theory. It is showed that inlet velocity has a more intuitive influence on the catalytic combustion efficiency of the hydrogen. A higher efficiency can be obtained with a lower inlet velocity. The optimum excess air coefficient is in the range of 0.94 to 1.0, the catalytic combustion efficiency of the hydrogen will be declined if the excess air coefficient exceeded 1.0. The effect of heat transfer coefficient on the catalytic combustion efficiency of the hydrogen mainly embodies in the case of the excess air coefficient exceeded 1.0, however, the effect will be declined if the heat transfer coefficient exceeded 4.0. The fuzzy grey relation degrees of the inlet velocity, heat transfer coefficient and excess air coefficient on the catalytic combustion efficiency of the hydrogen are 0.640945, 0.633214 and 0.547892 respectively.
基金Project supported by the National Basic Research Program of China(No.G1999022407).
文摘Five monolithic catalysts with low noble metal content were prepared by irnmerge method (Pt/γ=Al2O3, Pt/La-Al2O3, Pt/YSZ-AI203, Pt+Pd/La-Al2O3 and Pd/La-Al2O3) and their activity measurements were carried out in a conventional fixed-bed flow reactor. The results show that La-Al2O3 can promote activity of the prepared catalysts and can decrease the complete conversion temperature of cooking fume. The Pt/La-Al2O3 catalyst has the highest activity and can be applied in wide range of gas hourly space velocity (GHSV). Some characterizations (XRD, TPR) were carried out with the objective to explain differences in catalytic behaviors. The prepared catalyst showed a great potential for application.
基金financial support from the Key Projects of Natural Science Foundation of Liaoning Province(2018010047-301)the Shenyang National Laboratory for Materials Science for his research(Y8L6641161)+1 种基金financial support from the National Key R&D Program of China(2016YFB0501303)funding from European Union's Horizon 2020 research and innovation programme under grant agreement No.872102。
文摘Silicalite-1(S1)foam was functionalized by supporting manganese-cobalt(Mn-Co)mixed oxides to develop the structured hierarchical catalyst(Mn-Co@SlF)for catalytic combustion for the first time.The self-supporting S1 foam with hierarchical porosity was prepared via hydrothermal synthesis with polyurethane(PU)foam as the template.Subsequently,Mn-Co oxide nano sheets were uniformly grown on the surface of S1 foams under hydrothermal conditions to prepare the structured hierarchical catalyst with specific surface area of 354 m^2·g^-1,micropore volume of 0.141 cm^3·g^-1 and total pore volume of 0.217 cm3·g^-1,as well as a good capacity to adsorb toluene(1.7 mmol·g^-1 at p/p0=0.99).Comparative catalytic combustion of toluene of over developed structured catalyst Mn-Co@SlF was performed against the control catalysts of bulk Mn-Co@S1(i.e.,the crushed Mn-Co@SlF)and unsupported Mn-Co oxides(i.e.,Mn-Co).Mn-Co@SlF exhibited comparatively the best catalytic performance,that is,complete and stable toluene conversion at 2480 C over 65 h due to the synergy between Mn-Co oxides and S1 foam,which provided a large number of oxygen vacancies,high redox capacity.In addition,the hierarchical porous structure also improved the accessibility of active sites and facilitated the global mass transfer across the catalyst bed,being beneficial to the catalysis and catalyst longevity.
基金supported by the New Century Excellent Talent Project of China (NCET-05-0783).
文摘Supported manganese oxide catalysts were prepared by incipient wetness impregnation method for methane catalytic combustion, and effects of the support (Al2O3, SiO2 and TiO2) and Mn loading were investigated. These catalysts were characterized with N2 adsorption, X-ray diffraction, X-ray photoelectron spectroscopy and temperature-programmed reduction techniques. Methane conversion varied in a large range depending on supports or Mn loading. Al2O3 supported 15% Mn catalyst exhibited better activity toward methane catalytic oxidation. The manganese state and oxygen species played an important role in the catalytic performance,
基金This work was financially supported by Shandong Provincial Department of Science and Technology(project number:981206403)and the State Key Laboratory of Coal Conversion at Institute of Coal Chemistry of CAS(2002-2003)
文摘MnO_x/Al_2O_3 and MnO_x/ZrO_2-Al_2O_3 catalysts were prepared by incipientwetness impregnation of Mn(CH_3COO)_2 on the corresponding supports, followed by thecharacterization using X-ray diffraction (XRD), temperature programmed reduction (TPR) and BETsurface area techniques. The result shows the BET surface area of ZrO_2-Al_2O_3 is lower than thatof Al_2O_3 due to the loading of ZrO_2. However the resulted MnO_x/ZrO_2-Al_2O_3 catalyst exhibitshigher activity for methane combustion than MnO_x/Al_2O_3, because the addition of ZrO_2 ontoAl_2O_3 is beneficial for the dispersion of Mn species and the improvement of the lattice oxygenactivity in MnO_x, subsequently the activation of methane during combustion. The optimum loading ofZr in MnO_x/ZrO_2-Al_2O_3 is in the range of 5%-10% correlated with the calcination temperatures ofcatalyst supports.
基金Supported by the National High Technology Research and Development Program of China(2006AA030201)
文摘This work is focused on the performance prediction of pilot scale catalytic reverse flow reactors used for combustion of lean methane-air mixtures. An unsteady one-dimensional heterogeneous model for the reactor was established to account for the influence of the reactor wall on the heat transfer. Results of the simulation indicate that feed concentration, switch time and compensatory temperature impose important influence on the performance of the reactor. The amount of the heat extracted from the mid-section of the reactor can be optimized via adjusting the parameters mentioned above. At the optimal operating conditions, Le. switching time of 400 s, feed concentration of 1% (by volume), and insulation layer temperature of 343 K, the axial temperature of the reactor revealed a comparatively symmetrical "saddle" distribution, indicating a favorable operating status of the catalytic reverse flow reactor.
基金Supported by the Key Project of the National 973 Program of China (No.2005CB724201)the Natural Science Foundation ofBeijing (No.06C0002)the Beijing Education Commission Key Laboratory of Heat Transfer and Energy Conversion Fund(No.05005790200406).
文摘In this paper the premixed catalytic combustion emissions such as CO, unburned hydrocarbon (UHC), NOx and the temperature distribution in the catalytic monolith with ultra low concentration of Pd were studied. Three types of monoliths were used for experiments and the temperature of preheated air was respectively 50℃ , 100℃ and 200℃ . The results showed that preheated air made radial temperature in the catalytic monolith uniform which helped to avoid local hot spots so as to decrease NOx emission. The experiment also proved that the shorter monolith showed much better catalytic combustion performance than longer one and the temperature at the exit of the shorter monolith was relatively lower. On the contrary, the temperature was higher in the longer monolith and the lethal NOx emission was slightly increased.
基金financially supported by the developing & scientific foundation of Chengdu University of Information Technology (No.KYTZ20060902)Sichuan Provincial Department of Education (No.2006C032).
文摘The catalytic activity of Cu-ZSM-5 in trichloroethylene (TCE) combustion increases with the increasing skeletal Cu amount and however decreases with the increase of surface amorphous CuO, which is detected by infrared spectroscopy (IR) and diffuse reflectance ultraviolet-visible spectroscopy (DRS-UV-vis), therefore the skeletal Cu species are concluded to be the active sites for the TCE combustion.
基金This work was financially supported by the Scientific Research Found ationfor the Returned Overseas Chinese Scholars,State Education Ministry(2004-527)and the StateKey Laboratory of Coal Conversion at Institute of Coal Chemistry of CAS(04-603).
文摘A natural montmorillonite, produced from Laiyang of Shandong Province, was pillared by Tipolyeations to form Ti-pillared clay (Ti-PILC), and characterized by BET surface area, infrared spectra and thermal analysis. The characterization results show that Ti-PILC has a larger surface area and more hydroxyl groups than that of the natural clay, thus was used as the catalytic carriers to prepare supported Cu catalysts (Cu/Ti-PILC). The 20%Cu/Ti-PILC with 10mmol/g of Ti/clay shows a high catalytic performance of methane combustion in the temperature range of 400 500℃.
文摘The K2NiF4 type oxides, La2-x KxCuO4 complex oxides with nanometric size were prepared by sol-gel method. The characters of these samples were analyzed by H2-TPR, XRD, FT-IR and SEM. The catalytic activity for soot combustion was evaluated by temperature-programmed reaction (TPO) technique. The results demonstrate that the substitution of K^+ for La^3+ at A-site will increase the catalytic activities of La2-xKxCuO4 to soot combustion greatly, and the substitution quantity affects the structure and catalytic activity obviously. The La1.8 K0.2 CuO4 complex oxides with tetrahedral structure has the best catalytic activity for soot removal reaction, the ignition temperature of soot combustion is decreased from 490 to 320℃.
基金supported by the National Natural Science Foundation of China (No. 20773090)the National High Technology Research and Development Program of China (863 Program,No. 2006AA06Z347)the Youth Fund of Sichuan University (No. 2008119)
文摘Ce0.6Mn0.4O2 catalysts with different sources of manganese and Ce0.6-xZrxMn0.4O2 mixed oxide catalysts were prepared by coprecipitation method and were characterized by N2 adsorption-desorption,TPR,XRD,and XPS techniques.The activities of the prepared catalysts for ethyl acetate combustion,and the effects of calcination temperature and space velocity on catalytic activity were investigated.The results showed that partial replacement of Mn(NO3)2 with KMnO4 as sources of manganese could improve activities of catalysts.Ce0.45Zr0.15Mn0.4O2 catalyst exhibited the best catalytic activity and high thermal stability,e.g.,T90 could be still below 210℃ even if space velocity was up to 20000h-1.