In this study, reduction and desorption of oxides of nitrogen (NOx) were conducted using an electrical discharge plasma technique. The study was carried out using a simulated gas mixture to explore the possibility o...In this study, reduction and desorption of oxides of nitrogen (NOx) were conducted using an electrical discharge plasma technique. The study was carried out using a simulated gas mixture to explore the possibility of re-generation of used adsorbents by a nonthermal plasma desorption technique. Three different types of corona electrodes, namely, pipe, helical wire, and straight wire, were used for analyzing their effectiveness in NOx reduction/desorption. The pipe- type corona electrode exhibited a nitric oxide (NO) conversion of 50%, which is 1.5 times that of the straight-wire-type electrode at an energy density of 175 J/L. The helical-wire-type corona electrode exhibited a NOx desorption efficiency almost 4 times that of the pipe-type electrode, indicating the possibility that corona-generated species play a crucial role in desorption.展开更多
As the emission control regulations get stricter,the NO;reduction in the sintering process becomes an important environmental concern owing to its role in the formation of photochemical smog and acid rain.The NOxemiss...As the emission control regulations get stricter,the NO;reduction in the sintering process becomes an important environmental concern owing to its role in the formation of photochemical smog and acid rain.The NOxemissions from the sintering machine account for 48% of total amount from the iron and steel industry.Thus,it is essential to reduce NO;emissions from the sintering machine,for the achievement of clean production of sinter.Ca-Fe oxides,serving as the main binding phase in the sinter,are therefore used as additives into the sintering mixture to reduce NOxemissions.The results show that the NO;reduction ratio achieves 27.76% with 8% Ca-Fe oxides additives since the Ca-Fe oxides can advance the ignition and inhibit the nitrogen oxidation compared with the conventional condition.Meanwhile,the existence of Ca-Fe oxides was beneficial to the sinter quality since they were typical low melting point compounds.The optimal mass fraction of Ca-Fe oxides additives should be less than 8%since the permeability of sintering bed was significantly decreased with a further increase of the Ca-Fe oxides fines,inhibiting the mineralization reaction of sintering mixture.Additionally,the appropriate particle size can be obtained when mixing an equal amount of Ca-Fe oxides additives of-0.5 mm and 0.5-3.0 mm in size.展开更多
NOx storage and reduction(NSR)technology has been regarded as one of the most promising strategies for the removal of nitric oxides(NOx)from lean-burn engines,and the potential of the plasma catalysis method for NOx r...NOx storage and reduction(NSR)technology has been regarded as one of the most promising strategies for the removal of nitric oxides(NOx)from lean-burn engines,and the potential of the plasma catalysis method for NOx reduction has been confirmed in the past few decades.This work reports the NSR of nitric oxide(NO)by combining non-thermal plasma(NTP)and Co/Pt/Ba/γ-Al2O3(Co/PBA)catalyst using methane as a reductant.The experimental results reveal that the NOx conversion of NSR assisted by NTP is notably enhanced compared to the catalytic efficiency obtained from NSR in the range of 150°C–350°C,and NOx conversion of the 8%Co/PBA catalyst reaches 96.8%at 350°C.Oxygen(O_(2))has a significant effect on the removal of NOx,and the NOx conversion increases firstly and then decreases when the O_(2)concentration ranges from 2%to 10%.Water vapor reduces the NOx storage capacity of Co/PBA catalysts on account of the competition for adsorption sites on the surface of Co/PBA catalysts.There is a negative correlation between sulfur dioxide(SO_(2))and NOx conversion in the NTP system,and the 8%Co/PBA catalyst exhibits higher NOx conversion compared to other catalysts,which shows that Co has a certain SO_(2)resistance.展开更多
The selective catalytic reduction (SCR) of NOx with NH3 has been proven to be an efficient technology for NOx conversion to N2. However, the catalysts used for SCR usually suffer from the problem of sulfur poisoning...The selective catalytic reduction (SCR) of NOx with NH3 has been proven to be an efficient technology for NOx conversion to N2. However, the catalysts used for SCR usually suffer from the problem of sulfur poisoning which seriously limits their practical application. This review summarized sulfur poisoning mechanisms of various SCR deNG catalysts and strategies to reduce deactivation caused by SO2 such as doping metals, controlling the structures and morphologies of the catalysts, and selecting appropriate supports. The methods and procedures of catalysts preparation and the reaction conditions also have effect on SO2-resistance of the catalysts. Several novel catalyst systems that exhibited good SO2 resistance are also introduced. This paper could provide guidance for the development of highly efficient sulfur-tolerant deNOx catalysts.展开更多
Pulverized coal reburning, ammonia injection and advanced reburning in a pilot scale drop tube furnace were inves- tigated. Premix of petroleum gas, air and NH3 were burned in a porous gas burner to generate the neede...Pulverized coal reburning, ammonia injection and advanced reburning in a pilot scale drop tube furnace were inves- tigated. Premix of petroleum gas, air and NH3 were burned in a porous gas burner to generate the needed flue gas. Four kinds of pulverized coal were fed as reburning fuel at constant rate of 1g/min. The coal reburning process parameters including 15%~25% reburn heat input, temperature range from 1100 °C to 1400 °C and also the carbon in fly ash, coal fineness, reburn zone stoichiometric ratio, etc. were investigated. On the condition of 25% reburn heat input, maximum of 47% NO reduction with Yanzhou coal was obtained by pure coal reburning. Optimal temperature for reburning is about 1300 °C and fuel-rich stoichiometric ratio is essential; coal fineness can slightly enhance the reburning ability. The temperature window for ammonia injection is about 700 °C^1100 °C. CO can improve the NH3 ability at lower temperature. During advanced reburning, 72.9% NO reduction was measured. To achieve more than 70% NO reduction, Selective Non-catalytic NOx Reduction (SNCR) should need NH3/NO stoichiometric ratio larger than 5, while advanced reburning only uses common dose of ammonia as in conventional SNCR technology. Mechanism study shows the oxidization of CO can improve the decomposition of H2O, which will rich the radical pools igniting the whole reactions at lower temperatures.展开更多
In this study,to prepare a series of activated carbon-supported metals for the catalytic reduction of NO_x to N_2 in excess O_2,activated carbons derived from lignocellulosic and herbaceous biomasses were selected as ...In this study,to prepare a series of activated carbon-supported metals for the catalytic reduction of NO_x to N_2 in excess O_2,activated carbons derived from lignocellulosic and herbaceous biomasses were selected as the reducing agents,and alkali and transition metals were used as the catalytic active phases.The effects of the type of biomass,carbonization temperature and catalyst composition on NO_x reduction efficiency were analyzed in a fixed-bed flow reactor.The results showed that two temperature regimes are present for the NO_x-carbon reaction:at temperatures below 250°C,the NO_x adsorption process on the carbon surface was predominant,whereas true NO_x reduction by carbon occurred at temperatures above 250°C,producing N_2,CO_2 and CO.The influence of the carbonization temperature on carbon reactivity depended on the effect of the carbonization temperature on the carbon surface area and the reduction of the metal species on carbon.All studied metals catalyzed both NO_xand O_2reduction by carbon,and potassium could strongly enhance the C-NO_x reaction without substantial carbon consumption by O_2.Moreover,the potassium supported by sawdust-derived activated carbon exhibited higher selectivity and capacity towards NO_x reduction than did its previously reported coal-derived counterparts.These properties were ascribed to the high dispersion of the active potassium species on the carbon surface,as observed through the comparison of X-ray photoelectron spectroscopy and powder X-ray diffraction results for the carbons made from biomass and coal-based precursors.展开更多
Commercial V_(2)O_(5)-based catalysts have been successfully applied in NH_(3) selective catalytic reduction(NH_(3)-SCR)of NO_(x) from power stations,but their poor alkali-resistance restrains the wider application in...Commercial V_(2)O_(5)-based catalysts have been successfully applied in NH_(3) selective catalytic reduction(NH_(3)-SCR)of NO_(x) from power stations,but their poor alkali-resistance restrains the wider application in nonelectrical industries.In this study,NO_(x) reduction against alkali poisoning over V_(2)O_(5)/TiO_(2) is greatly improved via Ce(SO_(4))_(2) modification.It has been originally demonstrated that Ce^(4+)-SO_(4)^(2−)pair sites play crucial roles in improving NO_(x) reduction against alkali poisoning over V_(2)O_(5)/TiO_(2) catalysts.The strong interaction between V species and Ce sites of Ce^(4+)-SO_(4)^(2−)pairs triggers the reaction between NH_(4)^(+) species and gaseous NO via Eley-Rideal(E-R)reaction pathway.After K-poisoning,the SO_(4)^(2−)sites of Ce^(4+)-SO_(4)^(2−)pairs as protective sites strongly bond with K and thus maintain the high reaction efficiency via the E-R reaction pathway.This work demonstrates an effective strategy to enhance NO_(x) reduction against alkali poisoning over catalysts via constructing Ce^(4+)-SO_(4)^(2−)pair sites,contributing to developing alkali-resistant SCR catalysts for practical application in nonelectrical industries.展开更多
With the excessive use of fossil fuels leading to significant CO_(2)emissions,and the continuous increase of NOx in water bodies and soils,the use of electrochemical methods for the conversion of CO_(2)and NOx has gar...With the excessive use of fossil fuels leading to significant CO_(2)emissions,and the continuous increase of NOx in water bodies and soils,the use of electrochemical methods for the conversion of CO_(2)and NOx has garnered widespread attention as a green chemical approach due to its advantages of being environmentally friendly,low-carbon,and straightforward.C—N bonds are widely present in many value-added chemicals,such as urea,amides,and oximes.However,traditional methods for constructing C—N bonds typically involve thermochemical processes.Therefore,using electrochemical methods to catalyze the reduction of CO_(2)and NOx for C—N bond formation has emerged as a green and sustainable alternative.This paper summarizes the research progress of electrochemical C—N bond construction involving CO_(2)and NOx from the perspectives of reaction mechanisms and catalytic system construction,reviews the electrochemical synthesis of urea,amines,amides,and oximes through electrochemical C—N bond construction,and finally analyzes the current problems and challenges in the field,providing prospects for its future development.展开更多
Fully formulated lean NOx trap(LNT)catalysts of the type Pt/Rh/BaO/Al2O3 were prepared with and without incorporation of CeO2-ZrO2 in the washcoat,and their NOx reduction behavior was evaluated in steady-state,continu...Fully formulated lean NOx trap(LNT)catalysts of the type Pt/Rh/BaO/Al2O3 were prepared with and without incorporation of CeO2-ZrO2 in the washcoat,and their NOx reduction behavior was evaluated in steady-state,continuous flow experiments.In the fresh state, the CeO2-ZrO2 addition was found to exert little effect on NOx reduction activity using H2,CO,and NH3 as the reductants.However,after simulated road aging,NOx reduction activity was significantly impaired for the CeO2-ZrO2-free catalyst,whereas the performance of the CeO2-ZrO2-containing analog was affected to only a minor degree.These differences are explained on the basis of high-resolution transmission electron microscopy measurements showing that Pt supported on CeO2-ZrO2 remained highly dispersed after aging,whereas Pt supported on BaO/Al2O3 underwent significant sintering.In addition,the Pt/CeO2-ZrO2 component did not accumulate sulfur during aging, unlike Pt/BaO/Al2O3 for which significant sulfation of the Ba phase occurred.For both catalysts,selectivity to NH3 in NO and NO2 reduction by H2 increased after the catalyst aging,indicative of a change in the relative surface coverages of N and H ad-atoms on the precious metal sites.展开更多
Oxy fuel combustion and conventional cycle(currently working cycle) in Kazeroon plant are modeled using commercial thermodynamic modeling software. Economic evaluation of the two models regarding the resources of tran...Oxy fuel combustion and conventional cycle(currently working cycle) in Kazeroon plant are modeled using commercial thermodynamic modeling software. Economic evaluation of the two models regarding the resources of transport and injection of carbon dioxide into oil fields at Gachsaran for enhanced oil recovery in the various oil price indices is conducted and indices net present value(NPV) and internal rate of return on investment(IRR) are calculated. The results of the two models reveal that gross efficiency of the oxy fuel cycle is more than reference cycle(62% compared to 49.03%), but the net efficiency is less(41.85% compared to 47.92%) because of the high-energy consumption of the components, particularly air separation unit(ASU) in the oxy fuel cycle. In this model, pure carbon dioxide with pressure of 20×105 Pa and purity of 96.84% was captured. NOX emissions also decrease by 4289.7 tons per year due to separation of nitrogen in ASU. In this model, none of the components of oxy fuel cycle is a major engineering challenge. With increasing oil price, economic justification of oxy fuel combustion model increases. With the price of oil at $ 80 per barrel in mind and $ 31 per ton fines for emissions of carbon dioxide in the atmosphere, IRR is the same for both models.展开更多
In the present study reduction of nitrogen oxides using reburning technology, during combustion of sewage sludge (fuel I) and the mixture of sewage sludge, wasted bleaching earth and CaO (fuel II), was carried out. Th...In the present study reduction of nitrogen oxides using reburning technology, during combustion of sewage sludge (fuel I) and the mixture of sewage sludge, wasted bleaching earth and CaO (fuel II), was carried out. The experimental works were conducted in a laboratory-scale fluidized bed reactor (power up to 10 kW) with application of two types of beds: chemically inert bed (sand) and chemically active bed (CaO). The second combustion (reburning) zone in the reactor was formed by dosing into an area above the bed, additional gaseous fuel (propane). Obtained reduction in emissions of nitrogen oxides in both types of beds was at a level 70% - 79%. Additionally bed of CaO has the desulfurizing effect and also reduces the CO concentration in the exhaust fumes. A significant drawback of active bed is the adverse effect on increase of the primary NO which enters the second combustion zone. The result of this fact is higher NOx emission during combustion of the same fuel in bed of CaO in comparison to the combustion of this fuel in the sand bed, when the same maximum degree of reduction of NOx will be obtained for both types of beds.展开更多
In order to study the combustion characteristics,NOx emission and NH3 slip in a new trinal-sprayed precalciner,the simulations of combustion and aqueous urea solution based selective non-catalytic reduction(SNCR)proce...In order to study the combustion characteristics,NOx emission and NH3 slip in a new trinal-sprayed precalciner,the simulations of combustion and aqueous urea solution based selective non-catalytic reduction(SNCR)process were conducted by computational fluid dynamics in this precalciner,the effects of different injection heights,different injection flow rates and stratified injection under different flow rates on SNCR process were studied.The results showed that the flow field was symmetrically distributed in the precalciner,and the flue gas from the rotary kiln formed the recirculation region on both sides of the cone body,which increased the residence time of the solid particles.The temperature was mainly between 1100 K and 1250 K in the middle and upper column of the precalciner,which met the demand of the pulverized coal combustion and raw material decomposition.The concentration of NO at the outlet of the precalciner was 559 ppm,moreover,different injection heights and different injection flow rates had a strong influence on NOX removal efficiency and NH3 slip.The aqueous urea solution should be injected at SNCR-1 to prolong the residence time of NH3,and injection flow rate had an optimal flow rate but not the higher the better.When the injection flow rate under stratified injection was 0.019 kg/s,which could play a better optimization role on NO removal efficiency on the basic of the injection flow rate.In consideration of cost effective,a stratified injection with an injection flow rate of 0.019 kg/s and an injection height of 20 m,25 m and 30 m was suggested as a compromise of a satisfactory NOx reduction rates and reasonable NH3 slip.Under this condition,numerical simulation result showed that NOx concentration at the outlet of precalciner was 297.27 mg/Nm3 and NH3 slip was 4.67 mg/Nm3,meeting emission standard.展开更多
Herein,we report the high De-NOx performance of the A-site defective perovskite-based Pd/La_(0.5)Sr_(0.3)MnO_(3) catalyst.The formation of the defective perovskite structure can be proved by both the increased Mn^(4+)...Herein,we report the high De-NOx performance of the A-site defective perovskite-based Pd/La_(0.5)Sr_(0.3)MnO_(3) catalyst.The formation of the defective perovskite structure can be proved by both the increased Mn^(4+)/Mn^(3+) ratio and serious lattice contraction due to cationic nonstoichiometry.It promotes the Sr doping into perovskite lattice and reduces the formation of the SrCO_(3) phase.Our results demonstrate that below 300℃ the A-site defective perovskite can be more efficiently regenerated than the SrCO_(3) phase as NOx storage sites due to the latter’s stronger basicity,and also exhibits the higher NO oxidation ability than the A-site stoichiometric and excessive catalysts.Both factors promote the lowtemperature De-NOx activity of the Pd/La_(0.5)Sr_(0.3)MnO_(3) catalyst through improving its NOx trapping efficiency.Nevertheless,above 300℃,the NOx reduction becomes the determinant of the De-NOx activity of the perovskite-based catalysts.A-site defects can weaken the interactions between perovskite and Pd,inducing activation of Pd sites by in-situ transformation from PdO to metallic Pd in the alternative leanburn/fuel-rich atmospheric alternations,which boosts the De-NOx activity of the Pd/La_(0.5)Sr_(0.3)MnO_(3) catalyst.The Pd/L_(0.5)Sr_(0.3)MnO_(3) catalyst exhibits the high sulfur tolerance as well.These findings provide insight into optimizing the structural properties and catalytic activities of the perovskite-based catalysts via tuning formulation,and have potential to be applied for various related catalyst systems.展开更多
Contaminants(K,Na,Ca,and Mg)were introduced into Cu-SAPO-18 via incipient wetness impregnation to investigate their effect on the selective catalytic reduction of NOx with NH3(NH3-SCR)over Cu-SAPO-18.After the introdu...Contaminants(K,Na,Ca,and Mg)were introduced into Cu-SAPO-18 via incipient wetness impregnation to investigate their effect on the selective catalytic reduction of NOx with NH3(NH3-SCR)over Cu-SAPO-18.After the introduction of contaminants into Cu-SAPO-18,the quantity of acidic sites and Cu^2+ species in catalyst decreases owing to the replacement of H^+ and Cu^2+ by K^+,Na^+,Ca^2+,and Mg^2+.Furthermore,the loss of isolated Cu^2+ induces the generation of CuO and CuAl2O4-like phases,which causes further loss in the Brunauer-Emmett-Teller surface area of the catalyst.Consequently,the deNOx performance of the contaminated Cu-SAPO-18 catalysts drops.Such decline in NH3-SCR performance becomes more pronounced by increasing the contaminant contents from 0.5 to 1.0 mmol/gcatal.In addition,the deactivation influence of the contaminants on Cu-SAPO-18 is presented in the order of K>Na>Ca>Mg,which is consistent with the order of reduction of acidic sites.To a certain degree,the effect of the acidic sites on the deactivation of Cu-SAPO-18 might be more significant than that of isolated Cu2+ and the catalyst framework.Moreover,kinetic analysis of NH3-SCR was conducted,and the results indicate that there is no influence of contaminants on the NH3-SCR mechanism.展开更多
N2O is a powerful greenhouse gas and plays an important role in destructing the ozone layer. This present work investigated the effects of Pd doping on N2O formation over Pt/BaO/Al2O3 catalyst. Three types of catalyst...N2O is a powerful greenhouse gas and plays an important role in destructing the ozone layer. This present work investigated the effects of Pd doping on N2O formation over Pt/BaO/Al2O3 catalyst. Three types of catalysts, Pt/BaO/Al2O3, Pt/Pd mechanical mixing catalyst (Pt/BaO/Al203 + Pd/Al2O3) and Pt-Pd co-impregnation catalyst (Pt-Pd/BaO/Al2O3) were prepared by incipient wetness imoreenation method. These catalysts were first evaluated in NSR activity tests using H2/CO as reductants and then carefully characterized by BET, CO chemisorption, CO-DRIFTs and H2-TPR techniques. In addition, temperature programmed reactions of NO with H2/CO were conducted to obtain further information about NzO formation mechanism. Compared with Pt/BaO/Al2O3 (Pt/BaO/Al2O3 + Pd/Al2O3) produced less N2O and more NH3 during NOx storage and reduction process, while an opposite trend was found over (Pt-Pd/BaO/Al2O3 + Al2O3). Temperature programmed reactions of NO with H2/CO results showed that Pd/Al2O3 component in (Pt/BaO/Al2O3 + Pd/Al2O3) played an important role in NO reduction to NH3, and the formed NH3 could reduce NOx to N2 leading to a decrease in N2O formation. Most of N2O formed over (Pt-Pd/BaO/Al2O3 + Al2O3) was originated from Pd/BaO/Al2O3 component. H2-TPR results indicated Pd-Ba interaction resulted in more difficult- to-reduce PdOx species over Pd/BaO/Al2O3, which inhibits the NO dissociation and thus drives the selectivity to N2O in NO reduction.展开更多
NH_(3)-SCR was one of the most promising de NO_x technologies and it has been widely applied in industrial NO_x reduction.However,with the further development of energy transformation in power generation sector,the de...NH_(3)-SCR was one of the most promising de NO_x technologies and it has been widely applied in industrial NO_x reduction.However,with the further development of energy transformation in power generation sector,the development of NH_(3)-SCR catalysts is facing some new challenges.It is becoming an urgent problem to solve low catalytic activity and stability of NH_(3)-SCR catalysts at the working condition of ultra-low temperature(≤200℃)and high concentrations of H_(2)O+SO_(2) due to the gradual deployment of new energy power plants.Furthermore,the traditional coal-fired power plants would need flexible operation with the increasing share of renewable energy generation.The NH_(3)-SCR catalysts which were applied in coal-fired power industry would be requested to work in a wide temperature window from 200℃ to 500℃ in the near future.Therefore,in this review,we summarized the progress of NH_(3)-SCR catalysts in solving these different industrial problems in recent years.And the research directions which were deserved to be focused on the development of NH_(3)-SCR catalysts for the energy transition of power generation sector are proposed.展开更多
A series of WO3/CeO2 (WOx/CeO2) catalysts were synthesized by wet impregnation of ammonium metatungstate on a CeO2 support. The resulting solid acid catalysts were characterized by X-ray diffraction (XRD), UV-Vis ...A series of WO3/CeO2 (WOx/CeO2) catalysts were synthesized by wet impregnation of ammonium metatungstate on a CeO2 support. The resulting solid acid catalysts were characterized by X-ray diffraction (XRD), UV-Vis spectroscopy (UV-Vis), Raman spectroscopy (Raman), in-situ Fourier transform infrared spectroscopy (in-situ FT-IR) of ammonia adsorption, NH3-TPD, H2 temperature- programmed reduction (H2-TPR), NH3/NO oxidation and activity measurements for NOx reduction by NH3 (NH3-SCR). The results show that polytungstate (WOx) species are the main species of tungsten oxide on the surface of ceria. The addition of tungsten oxide enhances the BriSnsted acidity of ceria catalysts remarkably and decreases the amount of surface oxygen on celia, with strong interaction between CeO2 and WOx. As a result, the N2 selectivity of NH3 oxidation and NH3-SCR at high temperatures (〉 300℃) is enhanced. Therefore, a wide working temperature window in which NOx conversion exceeds 80% (NOx conversion 〉 80%) from 200 to 450℃, is achieved over 10 wt.% WOx/CeO2 catalyst. A tentative model of the NH3-SCR reaction route on WOx/CeO2 catalysts is presented.展开更多
Three dimensional numerical simulation of bituminous coal reburning in a full-scale tangentially fired boiler was conducted with CFD method to study the effects of reburn zone length, the height of reburn nozzles, the...Three dimensional numerical simulation of bituminous coal reburning in a full-scale tangentially fired boiler was conducted with CFD method to study the effects of reburn zone length, the height of reburn nozzles, the stoichiometric ratio in reburn zone, the reburn fuel fraction and the reburn coal fineness on NOx reduction efficiency and unburned carbon in fly ash. The results indicate that the NOx reduction efficiency reaches the largest value when the relative height of reburn nozzles is about 0.21 and the stoichiometric ratio is between 0.8 and 0.9 in reburn zone; NOx reduction efficiency increases with reburn zone length, reburn fuel fraction and the decrease of reburn coal particle size; the smaller the coal particle size is, the better the burnout performance of coal is.展开更多
In this work, the effectiveness of V2O5-WO3/TiO2 catalysts modified with different CeO2 contents by impregnation and co-precipitation methods on the selective catalytic reduction of NOxby NH3 have been studied compara...In this work, the effectiveness of V2O5-WO3/TiO2 catalysts modified with different CeO2 contents by impregnation and co-precipitation methods on the selective catalytic reduction of NOxby NH3 have been studied comparatively by various experimental techniques. The results showed that the NO conversion of V2O5-WO3/CeO2-TiO2 catalysts modified by co-precipitation method obviously increased with the Ce doping contents in the studied range below 20%(All Ce contents are in mass fractions), but the NO conversion of V2O5-WO3/CeO2/TiO2 catalysts modified by impregnation methods was lower than V2O5-WO3/CeO2-TiO2 catalysts especially beyond 2.5% Ce doping contents. The V2O5-WO3/CeO2-TiO2 catalysts showed better SCR activity, wider reaction window, and higher sulfur and water resistance. The characterization results elucidated that the modified catalysts by co-precipitation method exhibited higher specific surface area, much better dispersity of Ce component, more Ce^(3+)species and more Br?nsted acid sites than that by impregnation. The vacancies caused by more Ce^(3+)species were favorable for more NO oxidation to NO2, and the interaction between Ce species and WOxspecies generated more Br?nsted acid sites. It could be supposed that dispersed Ce Oxspecies and WOxspecies offered more second active centers respectively to adsorb oxygen and activate ammonia as co-catalysis to the primary active center of V ions, thus facilitated the better SCR activity of modified V2O5-WO3/CeO2-TiO2 catalysts by coprecipitation methods. The co-precipitation methods with Ce component were more suitable for production of modified commercial V2O5-WO3/TiO2 catalysts.展开更多
A series of meso-microporous Cu-SAPO-34 catalysts were successfully synthesized by a one-pot hydrothermal crystallization method, and these catalysts exhibited excellent NH3-SCR performance at low temperature. Their s...A series of meso-microporous Cu-SAPO-34 catalysts were successfully synthesized by a one-pot hydrothermal crystallization method, and these catalysts exhibited excellent NH3-SCR performance at low temperature. Their structure and physic chemical properties were characterized by means of X-ray diffraction patterns (XRD), Scanning electron microscopy (SEM), Transmission electron microscopy (TEM), N2 sorption-desorption, nuclear magnetic resonance (NMR), Inductively Coupled Plasma-Atomic Emission spectrometer (ICP-AES), X-ray absorption spectroscopy (XPS), Temperature-programmed desorption of ammonia (NH3-TPD), Ultraviolet visible diffuse reflectance spectroscopy (UV-Vis DRS) and Temperature programmed reduction (TPR). The analysis results indicate that the high activities of Cu-SAPO-34 catalysts could be attributed to the enhancement of redox property, the formation of mesopores and the more acid sites. Furthermore, the kinetic results verify that the formation of mesopores remarkably reduces diffusion resistance and then improves the accessibility of reactants to catalytically active sites. The 1.0-Cu-SAPO-34 catalyst exhibited the high NO conversion (〉90%) among the wide activity temperature window in the range of 150- 425℃.展开更多
文摘In this study, reduction and desorption of oxides of nitrogen (NOx) were conducted using an electrical discharge plasma technique. The study was carried out using a simulated gas mixture to explore the possibility of re-generation of used adsorbents by a nonthermal plasma desorption technique. Three different types of corona electrodes, namely, pipe, helical wire, and straight wire, were used for analyzing their effectiveness in NOx reduction/desorption. The pipe- type corona electrode exhibited a nitric oxide (NO) conversion of 50%, which is 1.5 times that of the straight-wire-type electrode at an energy density of 175 J/L. The helical-wire-type corona electrode exhibited a NOx desorption efficiency almost 4 times that of the pipe-type electrode, indicating the possibility that corona-generated species play a crucial role in desorption.
文摘As the emission control regulations get stricter,the NO;reduction in the sintering process becomes an important environmental concern owing to its role in the formation of photochemical smog and acid rain.The NOxemissions from the sintering machine account for 48% of total amount from the iron and steel industry.Thus,it is essential to reduce NO;emissions from the sintering machine,for the achievement of clean production of sinter.Ca-Fe oxides,serving as the main binding phase in the sinter,are therefore used as additives into the sintering mixture to reduce NOxemissions.The results show that the NO;reduction ratio achieves 27.76% with 8% Ca-Fe oxides additives since the Ca-Fe oxides can advance the ignition and inhibit the nitrogen oxidation compared with the conventional condition.Meanwhile,the existence of Ca-Fe oxides was beneficial to the sinter quality since they were typical low melting point compounds.The optimal mass fraction of Ca-Fe oxides additives should be less than 8%since the permeability of sintering bed was significantly decreased with a further increase of the Ca-Fe oxides fines,inhibiting the mineralization reaction of sintering mixture.Additionally,the appropriate particle size can be obtained when mixing an equal amount of Ca-Fe oxides additives of-0.5 mm and 0.5-3.0 mm in size.
基金by the National Engineering Laboratory for Mobile Source Emission Control Technology(No.NELMS2019A13)the National Key Research and Development Project of China(No.2019YFC1805505)+2 种基金the Shanxi Province Bidding Project(No.20191101007)the Major Science and Technology Projects of Shanxi Province(No.20181102017)State Key Laboratory of Organic Geochemistry(No.SKLOG-201909)。
文摘NOx storage and reduction(NSR)technology has been regarded as one of the most promising strategies for the removal of nitric oxides(NOx)from lean-burn engines,and the potential of the plasma catalysis method for NOx reduction has been confirmed in the past few decades.This work reports the NSR of nitric oxide(NO)by combining non-thermal plasma(NTP)and Co/Pt/Ba/γ-Al2O3(Co/PBA)catalyst using methane as a reductant.The experimental results reveal that the NOx conversion of NSR assisted by NTP is notably enhanced compared to the catalytic efficiency obtained from NSR in the range of 150°C–350°C,and NOx conversion of the 8%Co/PBA catalyst reaches 96.8%at 350°C.Oxygen(O_(2))has a significant effect on the removal of NOx,and the NOx conversion increases firstly and then decreases when the O_(2)concentration ranges from 2%to 10%.Water vapor reduces the NOx storage capacity of Co/PBA catalysts on account of the competition for adsorption sites on the surface of Co/PBA catalysts.There is a negative correlation between sulfur dioxide(SO_(2))and NOx conversion in the NTP system,and the 8%Co/PBA catalyst exhibits higher NOx conversion compared to other catalysts,which shows that Co has a certain SO_(2)resistance.
基金Supported by the Scientific Research Foundation for the Returned Overseas Chinese Scholars,State Education Ministrythe National Natural Science Foundation of China(21506150)
文摘The selective catalytic reduction (SCR) of NOx with NH3 has been proven to be an efficient technology for NOx conversion to N2. However, the catalysts used for SCR usually suffer from the problem of sulfur poisoning which seriously limits their practical application. This review summarized sulfur poisoning mechanisms of various SCR deNG catalysts and strategies to reduce deactivation caused by SO2 such as doping metals, controlling the structures and morphologies of the catalysts, and selecting appropriate supports. The methods and procedures of catalysts preparation and the reaction conditions also have effect on SO2-resistance of the catalysts. Several novel catalyst systems that exhibited good SO2 resistance are also introduced. This paper could provide guidance for the development of highly efficient sulfur-tolerant deNOx catalysts.
文摘Pulverized coal reburning, ammonia injection and advanced reburning in a pilot scale drop tube furnace were inves- tigated. Premix of petroleum gas, air and NH3 were burned in a porous gas burner to generate the needed flue gas. Four kinds of pulverized coal were fed as reburning fuel at constant rate of 1g/min. The coal reburning process parameters including 15%~25% reburn heat input, temperature range from 1100 °C to 1400 °C and also the carbon in fly ash, coal fineness, reburn zone stoichiometric ratio, etc. were investigated. On the condition of 25% reburn heat input, maximum of 47% NO reduction with Yanzhou coal was obtained by pure coal reburning. Optimal temperature for reburning is about 1300 °C and fuel-rich stoichiometric ratio is essential; coal fineness can slightly enhance the reburning ability. The temperature window for ammonia injection is about 700 °C^1100 °C. CO can improve the NH3 ability at lower temperature. During advanced reburning, 72.9% NO reduction was measured. To achieve more than 70% NO reduction, Selective Non-catalytic NOx Reduction (SNCR) should need NH3/NO stoichiometric ratio larger than 5, while advanced reburning only uses common dose of ammonia as in conventional SNCR technology. Mechanism study shows the oxidization of CO can improve the decomposition of H2O, which will rich the radical pools igniting the whole reactions at lower temperatures.
基金Supported by the National Natural Science Foundation of China(21507119)the Key Technology Research and Development Program of Qinghai Province(2012-J-144)the National High Technology Research and Development Program of China(2012AA06A11303)
文摘In this study,to prepare a series of activated carbon-supported metals for the catalytic reduction of NO_x to N_2 in excess O_2,activated carbons derived from lignocellulosic and herbaceous biomasses were selected as the reducing agents,and alkali and transition metals were used as the catalytic active phases.The effects of the type of biomass,carbonization temperature and catalyst composition on NO_x reduction efficiency were analyzed in a fixed-bed flow reactor.The results showed that two temperature regimes are present for the NO_x-carbon reaction:at temperatures below 250°C,the NO_x adsorption process on the carbon surface was predominant,whereas true NO_x reduction by carbon occurred at temperatures above 250°C,producing N_2,CO_2 and CO.The influence of the carbonization temperature on carbon reactivity depended on the effect of the carbonization temperature on the carbon surface area and the reduction of the metal species on carbon.All studied metals catalyzed both NO_xand O_2reduction by carbon,and potassium could strongly enhance the C-NO_x reaction without substantial carbon consumption by O_2.Moreover,the potassium supported by sawdust-derived activated carbon exhibited higher selectivity and capacity towards NO_x reduction than did its previously reported coal-derived counterparts.These properties were ascribed to the high dispersion of the active potassium species on the carbon surface,as observed through the comparison of X-ray photoelectron spectroscopy and powder X-ray diffraction results for the carbons made from biomass and coal-based precursors.
基金the National Natural Science Foundation of China(Nos.22125604,22106100,21976117)Shanghai Rising-Star Program(No.22QA1403700)+1 种基金Chenguang Program supported by Shanghai Education Development FoundationShanghai Municipal Education Commission(No.22Z00354).
文摘Commercial V_(2)O_(5)-based catalysts have been successfully applied in NH_(3) selective catalytic reduction(NH_(3)-SCR)of NO_(x) from power stations,but their poor alkali-resistance restrains the wider application in nonelectrical industries.In this study,NO_(x) reduction against alkali poisoning over V_(2)O_(5)/TiO_(2) is greatly improved via Ce(SO_(4))_(2) modification.It has been originally demonstrated that Ce^(4+)-SO_(4)^(2−)pair sites play crucial roles in improving NO_(x) reduction against alkali poisoning over V_(2)O_(5)/TiO_(2) catalysts.The strong interaction between V species and Ce sites of Ce^(4+)-SO_(4)^(2−)pairs triggers the reaction between NH_(4)^(+) species and gaseous NO via Eley-Rideal(E-R)reaction pathway.After K-poisoning,the SO_(4)^(2−)sites of Ce^(4+)-SO_(4)^(2−)pairs as protective sites strongly bond with K and thus maintain the high reaction efficiency via the E-R reaction pathway.This work demonstrates an effective strategy to enhance NO_(x) reduction against alkali poisoning over catalysts via constructing Ce^(4+)-SO_(4)^(2−)pair sites,contributing to developing alkali-resistant SCR catalysts for practical application in nonelectrical industries.
基金supported by the National Natural Science Foundation of China(Nos.22293015,22121002)the Beijing Natural Science Foundation,China(No.J210020)+1 种基金the Strategic Priority Research Program(A)of the Chinese Academy of Sciences(No.XDA0390400)the Project of the Photon Science Center for Carbon Neutrality of CAS.
文摘With the excessive use of fossil fuels leading to significant CO_(2)emissions,and the continuous increase of NOx in water bodies and soils,the use of electrochemical methods for the conversion of CO_(2)and NOx has garnered widespread attention as a green chemical approach due to its advantages of being environmentally friendly,low-carbon,and straightforward.C—N bonds are widely present in many value-added chemicals,such as urea,amides,and oximes.However,traditional methods for constructing C—N bonds typically involve thermochemical processes.Therefore,using electrochemical methods to catalyze the reduction of CO_(2)and NOx for C—N bond formation has emerged as a green and sustainable alternative.This paper summarizes the research progress of electrochemical C—N bond construction involving CO_(2)and NOx from the perspectives of reaction mechanisms and catalytic system construction,reviews the electrochemical synthesis of urea,amines,amides,and oximes through electrochemical C—N bond construction,and finally analyzes the current problems and challenges in the field,providing prospects for its future development.
基金supported by the U.S.Department of Energy(DOE)under award No.DE-EE0000205
文摘Fully formulated lean NOx trap(LNT)catalysts of the type Pt/Rh/BaO/Al2O3 were prepared with and without incorporation of CeO2-ZrO2 in the washcoat,and their NOx reduction behavior was evaluated in steady-state,continuous flow experiments.In the fresh state, the CeO2-ZrO2 addition was found to exert little effect on NOx reduction activity using H2,CO,and NH3 as the reductants.However,after simulated road aging,NOx reduction activity was significantly impaired for the CeO2-ZrO2-free catalyst,whereas the performance of the CeO2-ZrO2-containing analog was affected to only a minor degree.These differences are explained on the basis of high-resolution transmission electron microscopy measurements showing that Pt supported on CeO2-ZrO2 remained highly dispersed after aging,whereas Pt supported on BaO/Al2O3 underwent significant sintering.In addition,the Pt/CeO2-ZrO2 component did not accumulate sulfur during aging, unlike Pt/BaO/Al2O3 for which significant sulfation of the Ba phase occurred.For both catalysts,selectivity to NH3 in NO and NO2 reduction by H2 increased after the catalyst aging,indicative of a change in the relative surface coverages of N and H ad-atoms on the precious metal sites.
文摘Oxy fuel combustion and conventional cycle(currently working cycle) in Kazeroon plant are modeled using commercial thermodynamic modeling software. Economic evaluation of the two models regarding the resources of transport and injection of carbon dioxide into oil fields at Gachsaran for enhanced oil recovery in the various oil price indices is conducted and indices net present value(NPV) and internal rate of return on investment(IRR) are calculated. The results of the two models reveal that gross efficiency of the oxy fuel cycle is more than reference cycle(62% compared to 49.03%), but the net efficiency is less(41.85% compared to 47.92%) because of the high-energy consumption of the components, particularly air separation unit(ASU) in the oxy fuel cycle. In this model, pure carbon dioxide with pressure of 20×105 Pa and purity of 96.84% was captured. NOX emissions also decrease by 4289.7 tons per year due to separation of nitrogen in ASU. In this model, none of the components of oxy fuel cycle is a major engineering challenge. With increasing oil price, economic justification of oxy fuel combustion model increases. With the price of oil at $ 80 per barrel in mind and $ 31 per ton fines for emissions of carbon dioxide in the atmosphere, IRR is the same for both models.
文摘In the present study reduction of nitrogen oxides using reburning technology, during combustion of sewage sludge (fuel I) and the mixture of sewage sludge, wasted bleaching earth and CaO (fuel II), was carried out. The experimental works were conducted in a laboratory-scale fluidized bed reactor (power up to 10 kW) with application of two types of beds: chemically inert bed (sand) and chemically active bed (CaO). The second combustion (reburning) zone in the reactor was formed by dosing into an area above the bed, additional gaseous fuel (propane). Obtained reduction in emissions of nitrogen oxides in both types of beds was at a level 70% - 79%. Additionally bed of CaO has the desulfurizing effect and also reduces the CO concentration in the exhaust fumes. A significant drawback of active bed is the adverse effect on increase of the primary NO which enters the second combustion zone. The result of this fact is higher NOx emission during combustion of the same fuel in bed of CaO in comparison to the combustion of this fuel in the sand bed, when the same maximum degree of reduction of NOx will be obtained for both types of beds.
基金This work was supported by the general institute of building materials research of china(No.2017YFC0210801)the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD).
文摘In order to study the combustion characteristics,NOx emission and NH3 slip in a new trinal-sprayed precalciner,the simulations of combustion and aqueous urea solution based selective non-catalytic reduction(SNCR)process were conducted by computational fluid dynamics in this precalciner,the effects of different injection heights,different injection flow rates and stratified injection under different flow rates on SNCR process were studied.The results showed that the flow field was symmetrically distributed in the precalciner,and the flue gas from the rotary kiln formed the recirculation region on both sides of the cone body,which increased the residence time of the solid particles.The temperature was mainly between 1100 K and 1250 K in the middle and upper column of the precalciner,which met the demand of the pulverized coal combustion and raw material decomposition.The concentration of NO at the outlet of the precalciner was 559 ppm,moreover,different injection heights and different injection flow rates had a strong influence on NOX removal efficiency and NH3 slip.The aqueous urea solution should be injected at SNCR-1 to prolong the residence time of NH3,and injection flow rate had an optimal flow rate but not the higher the better.When the injection flow rate under stratified injection was 0.019 kg/s,which could play a better optimization role on NO removal efficiency on the basic of the injection flow rate.In consideration of cost effective,a stratified injection with an injection flow rate of 0.019 kg/s and an injection height of 20 m,25 m and 30 m was suggested as a compromise of a satisfactory NOx reduction rates and reasonable NH3 slip.Under this condition,numerical simulation result showed that NOx concentration at the outlet of precalciner was 297.27 mg/Nm3 and NH3 slip was 4.67 mg/Nm3,meeting emission standard.
基金the National Natural Science Foundation of China(21878213)。
文摘Herein,we report the high De-NOx performance of the A-site defective perovskite-based Pd/La_(0.5)Sr_(0.3)MnO_(3) catalyst.The formation of the defective perovskite structure can be proved by both the increased Mn^(4+)/Mn^(3+) ratio and serious lattice contraction due to cationic nonstoichiometry.It promotes the Sr doping into perovskite lattice and reduces the formation of the SrCO_(3) phase.Our results demonstrate that below 300℃ the A-site defective perovskite can be more efficiently regenerated than the SrCO_(3) phase as NOx storage sites due to the latter’s stronger basicity,and also exhibits the higher NO oxidation ability than the A-site stoichiometric and excessive catalysts.Both factors promote the lowtemperature De-NOx activity of the Pd/La_(0.5)Sr_(0.3)MnO_(3) catalyst through improving its NOx trapping efficiency.Nevertheless,above 300℃,the NOx reduction becomes the determinant of the De-NOx activity of the perovskite-based catalysts.A-site defects can weaken the interactions between perovskite and Pd,inducing activation of Pd sites by in-situ transformation from PdO to metallic Pd in the alternative leanburn/fuel-rich atmospheric alternations,which boosts the De-NOx activity of the Pd/La_(0.5)Sr_(0.3)MnO_(3) catalyst.The Pd/L_(0.5)Sr_(0.3)MnO_(3) catalyst exhibits the high sulfur tolerance as well.These findings provide insight into optimizing the structural properties and catalytic activities of the perovskite-based catalysts via tuning formulation,and have potential to be applied for various related catalyst systems.
基金supported by the National Natural Science Foundation of China(21473064)~~
文摘Contaminants(K,Na,Ca,and Mg)were introduced into Cu-SAPO-18 via incipient wetness impregnation to investigate their effect on the selective catalytic reduction of NOx with NH3(NH3-SCR)over Cu-SAPO-18.After the introduction of contaminants into Cu-SAPO-18,the quantity of acidic sites and Cu^2+ species in catalyst decreases owing to the replacement of H^+ and Cu^2+ by K^+,Na^+,Ca^2+,and Mg^2+.Furthermore,the loss of isolated Cu^2+ induces the generation of CuO and CuAl2O4-like phases,which causes further loss in the Brunauer-Emmett-Teller surface area of the catalyst.Consequently,the deNOx performance of the contaminated Cu-SAPO-18 catalysts drops.Such decline in NH3-SCR performance becomes more pronounced by increasing the contaminant contents from 0.5 to 1.0 mmol/gcatal.In addition,the deactivation influence of the contaminants on Cu-SAPO-18 is presented in the order of K>Na>Ca>Mg,which is consistent with the order of reduction of acidic sites.To a certain degree,the effect of the acidic sites on the deactivation of Cu-SAPO-18 might be more significant than that of isolated Cu2+ and the catalyst framework.Moreover,kinetic analysis of NH3-SCR was conducted,and the results indicate that there is no influence of contaminants on the NH3-SCR mechanism.
基金Acknowledgements This work was financially supported by the National Key Research and Development Program (No. 2017YFC0211002) and the National Natural Science Foundation of China (Grant No. 21476170).
文摘N2O is a powerful greenhouse gas and plays an important role in destructing the ozone layer. This present work investigated the effects of Pd doping on N2O formation over Pt/BaO/Al2O3 catalyst. Three types of catalysts, Pt/BaO/Al2O3, Pt/Pd mechanical mixing catalyst (Pt/BaO/Al203 + Pd/Al2O3) and Pt-Pd co-impregnation catalyst (Pt-Pd/BaO/Al2O3) were prepared by incipient wetness imoreenation method. These catalysts were first evaluated in NSR activity tests using H2/CO as reductants and then carefully characterized by BET, CO chemisorption, CO-DRIFTs and H2-TPR techniques. In addition, temperature programmed reactions of NO with H2/CO were conducted to obtain further information about NzO formation mechanism. Compared with Pt/BaO/Al2O3 (Pt/BaO/Al2O3 + Pd/Al2O3) produced less N2O and more NH3 during NOx storage and reduction process, while an opposite trend was found over (Pt-Pd/BaO/Al2O3 + Al2O3). Temperature programmed reactions of NO with H2/CO results showed that Pd/Al2O3 component in (Pt/BaO/Al2O3 + Pd/Al2O3) played an important role in NO reduction to NH3, and the formed NH3 could reduce NOx to N2 leading to a decrease in N2O formation. Most of N2O formed over (Pt-Pd/BaO/Al2O3 + Al2O3) was originated from Pd/BaO/Al2O3 component. H2-TPR results indicated Pd-Ba interaction resulted in more difficult- to-reduce PdOx species over Pd/BaO/Al2O3, which inhibits the NO dissociation and thus drives the selectivity to N2O in NO reduction.
基金financially supported by the National Natural Science Foundation of China(No.52072306)the National Key R&D Program of China(No.2021YFB3701500)the Fundamental Research Funds for the Central Universities(Nos.3102019PJ008 and 3102018JCC002)。
文摘NH_(3)-SCR was one of the most promising de NO_x technologies and it has been widely applied in industrial NO_x reduction.However,with the further development of energy transformation in power generation sector,the development of NH_(3)-SCR catalysts is facing some new challenges.It is becoming an urgent problem to solve low catalytic activity and stability of NH_(3)-SCR catalysts at the working condition of ultra-low temperature(≤200℃)and high concentrations of H_(2)O+SO_(2) due to the gradual deployment of new energy power plants.Furthermore,the traditional coal-fired power plants would need flexible operation with the increasing share of renewable energy generation.The NH_(3)-SCR catalysts which were applied in coal-fired power industry would be requested to work in a wide temperature window from 200℃ to 500℃ in the near future.Therefore,in this review,we summarized the progress of NH_(3)-SCR catalysts in solving these different industrial problems in recent years.And the research directions which were deserved to be focused on the development of NH_(3)-SCR catalysts for the energy transition of power generation sector are proposed.
基金the Ministry of Science and Technology, PR China for financial support of Project 2010CB732304Science and Technology Department of Zhejiang Province Project 2011C31010
文摘A series of WO3/CeO2 (WOx/CeO2) catalysts were synthesized by wet impregnation of ammonium metatungstate on a CeO2 support. The resulting solid acid catalysts were characterized by X-ray diffraction (XRD), UV-Vis spectroscopy (UV-Vis), Raman spectroscopy (Raman), in-situ Fourier transform infrared spectroscopy (in-situ FT-IR) of ammonia adsorption, NH3-TPD, H2 temperature- programmed reduction (H2-TPR), NH3/NO oxidation and activity measurements for NOx reduction by NH3 (NH3-SCR). The results show that polytungstate (WOx) species are the main species of tungsten oxide on the surface of ceria. The addition of tungsten oxide enhances the BriSnsted acidity of ceria catalysts remarkably and decreases the amount of surface oxygen on celia, with strong interaction between CeO2 and WOx. As a result, the N2 selectivity of NH3 oxidation and NH3-SCR at high temperatures (〉 300℃) is enhanced. Therefore, a wide working temperature window in which NOx conversion exceeds 80% (NOx conversion 〉 80%) from 200 to 450℃, is achieved over 10 wt.% WOx/CeO2 catalyst. A tentative model of the NH3-SCR reaction route on WOx/CeO2 catalysts is presented.
文摘Three dimensional numerical simulation of bituminous coal reburning in a full-scale tangentially fired boiler was conducted with CFD method to study the effects of reburn zone length, the height of reburn nozzles, the stoichiometric ratio in reburn zone, the reburn fuel fraction and the reburn coal fineness on NOx reduction efficiency and unburned carbon in fly ash. The results indicate that the NOx reduction efficiency reaches the largest value when the relative height of reburn nozzles is about 0.21 and the stoichiometric ratio is between 0.8 and 0.9 in reburn zone; NOx reduction efficiency increases with reburn zone length, reburn fuel fraction and the decrease of reburn coal particle size; the smaller the coal particle size is, the better the burnout performance of coal is.
基金Project supported by the Guangxi Natural Science Foundation(2014GXNSFAA118057)Guangxi Science and Technology Planning Project(AB16380276)
文摘In this work, the effectiveness of V2O5-WO3/TiO2 catalysts modified with different CeO2 contents by impregnation and co-precipitation methods on the selective catalytic reduction of NOxby NH3 have been studied comparatively by various experimental techniques. The results showed that the NO conversion of V2O5-WO3/CeO2-TiO2 catalysts modified by co-precipitation method obviously increased with the Ce doping contents in the studied range below 20%(All Ce contents are in mass fractions), but the NO conversion of V2O5-WO3/CeO2/TiO2 catalysts modified by impregnation methods was lower than V2O5-WO3/CeO2-TiO2 catalysts especially beyond 2.5% Ce doping contents. The V2O5-WO3/CeO2-TiO2 catalysts showed better SCR activity, wider reaction window, and higher sulfur and water resistance. The characterization results elucidated that the modified catalysts by co-precipitation method exhibited higher specific surface area, much better dispersity of Ce component, more Ce^(3+)species and more Br?nsted acid sites than that by impregnation. The vacancies caused by more Ce^(3+)species were favorable for more NO oxidation to NO2, and the interaction between Ce species and WOxspecies generated more Br?nsted acid sites. It could be supposed that dispersed Ce Oxspecies and WOxspecies offered more second active centers respectively to adsorb oxygen and activate ammonia as co-catalysis to the primary active center of V ions, thus facilitated the better SCR activity of modified V2O5-WO3/CeO2-TiO2 catalysts by coprecipitation methods. The co-precipitation methods with Ce component were more suitable for production of modified commercial V2O5-WO3/TiO2 catalysts.
基金supported by the National Natural Science Foundation of China (Nos. 21376261, 21173270)the National Hi-Tech Research and Development Program (863) of China (No. 2015AA034603)+1 种基金the Beijing Natural Science Foundation(No. 2142027)the China University of Petroleum Fund (Nos. 20130007110007, 2462015QZDX04)
文摘A series of meso-microporous Cu-SAPO-34 catalysts were successfully synthesized by a one-pot hydrothermal crystallization method, and these catalysts exhibited excellent NH3-SCR performance at low temperature. Their structure and physic chemical properties were characterized by means of X-ray diffraction patterns (XRD), Scanning electron microscopy (SEM), Transmission electron microscopy (TEM), N2 sorption-desorption, nuclear magnetic resonance (NMR), Inductively Coupled Plasma-Atomic Emission spectrometer (ICP-AES), X-ray absorption spectroscopy (XPS), Temperature-programmed desorption of ammonia (NH3-TPD), Ultraviolet visible diffuse reflectance spectroscopy (UV-Vis DRS) and Temperature programmed reduction (TPR). The analysis results indicate that the high activities of Cu-SAPO-34 catalysts could be attributed to the enhancement of redox property, the formation of mesopores and the more acid sites. Furthermore, the kinetic results verify that the formation of mesopores remarkably reduces diffusion resistance and then improves the accessibility of reactants to catalytically active sites. The 1.0-Cu-SAPO-34 catalyst exhibited the high NO conversion (〉90%) among the wide activity temperature window in the range of 150- 425℃.