Abstract The detailed kinetic model of selective non-catalytic reduction （SNCR） of nitric oxide, including so-dium species reactions, was deyeloped on the basis of recent studies on thermal DeNOx mechanism, NOxOUTme...Abstract The detailed kinetic model of selective non-catalytic reduction （SNCR） of nitric oxide, including so-dium species reactions, was deyeloped on the basis of recent studies on thermal DeNOx mechanism, NOxOUTmechanism and promotion mechanism of Na2CO3. The model was validated by comparison with several experi-mental findings, thus providing an effective tool for the primary and promoted SNCR process simulation. Experimental and simulated results show part-per-million level of sodium carbonate enhances NO removal efficiency andextend the effective SNCR temperature range in comparison with use of a nitrogen agent alone. The kinetic modeling, sensitivity and rate-of-production analysis suggest that the performance improvement can be explained as ho-mogeneous sodium species reactions producing more reactive OH radicals. The net result of sodium species reac-tions is conversion of H2O and inactive HO2 radicals into reactive OH radicals, i.e. H2O＋HO2=3OH, which enhances the SNCR performance of nitrogen agents by mainly increasing the production rate of NH2 radicals. More-over, N2O and CO are eliminated diversely via the reactions Na＋N20=NaO＋N2, NaO＋CO=Na＋CO2 andNaO2＋CO =NaO＋CO2, in.the pro.moted SNCR process, especially in the NOxOUT process.展开更多
An experimental study of thermal de-NOx using NH3 as reductant in 02/C02 atmosphere with the effect of S02 and different additives was performed in a drop tube furnace. Results show that the optimum temperature win- d...An experimental study of thermal de-NOx using NH3 as reductant in 02/C02 atmosphere with the effect of S02 and different additives was performed in a drop tube furnace. Results show that the optimum temperature win- dow is 841-1184 ℃, and the optimum reaction temperature is about 900 ℃ with a de-NOx efficiency of 95.4%. A certain amount of S02 has an inhibiting effect on NO reduction. The effect of additives, including Na2C03, C2H5OH and FeCI3, on NO reduction by NH3 is also explored. The addition of Na2CO3 and FeCI3 is useful to widen the tem- perature window and shift the reaction to lower temperature for the efficiency is increased from 30.5% to 74.0% and 67.4% respectively at 800 ℃. Qualitatively, the modeling results using a detailed kinetic modeling mecha- nism represent well most of the process features. The effect of Na2CO3, C2H5OH and FeCI3 addition can be reproduced well by the Na2C03, C2H5OH and Fe（CO）5 sub-mechanism respectively. The reaction mechanism analysis shows that the effects of these additives on NO reduction are achieved mainly by promoting the produc- tion of OH radicals at lower temperature.展开更多
Nitrous oxide is not an environmentally regulated species in the U.S., but it does participate in the stratospheric ozone chemistry and contributes to the greenhouse effect. Nitrous oxide has been found to be a by-pro...Nitrous oxide is not an environmentally regulated species in the U.S., but it does participate in the stratospheric ozone chemistry and contributes to the greenhouse effect. Nitrous oxide has been found to be a by-product of the selective non-catalytic reduction process. Chemical kinetic calculations demonstrated that the formation of nitrous oxide in the urea-based selective non-catalytic reduction process is linked to the conversion of NO by cyano species released from the process parent compounds. This conversion occurs within in temperature window between 850 and 1050℃. With urea injection, nitrous oxide emissions represent up to 20 percent conversion of the NOx reduced. The amount of nitrous oxide formed depends primarily on the process temperature, the amount of chemical injected, the initial NOx level, and the carbon monoxide level in the gas stream. These observations, which were based on the chemical kinetics of the process, should be considered in designing selective non-catalytic reduction systems to minimize nitrous oxide by- product formation.展开更多
We rationally designed a high performance denitration(De-NOx) catalyst based on a micrometer-sized spherical Mn–Ce–Fe–Ti(CP-SD)catalyst for selective catalytic reduction(SCR). This was prepared by a co-precipitatio...We rationally designed a high performance denitration(De-NOx) catalyst based on a micrometer-sized spherical Mn–Ce–Fe–Ti(CP-SD)catalyst for selective catalytic reduction(SCR). This was prepared by a co-precipitation and spray drying(CP-SD) method. The catalyst was systematically characterized, and its morphological structure and surface properties were identified. Compare with conventional Mn–Ce–Fe–Ti(CP) catalysts, the Mn–Ce–Fe–Ti(CP-SD) catalyst had superior surface-adsorbed oxygen leading to enhanced 'fast NH3-SCR' reaction. The asobtained Mn–Ce–Fe–Ti(CP-SD) catalyst offered excellent NO conversion and N2 selectivity of 100.0% and 84.8% at 250℃, respectively, with a gas hourly space velocity(GHSV) of 40,000 h-1. The porous micro-spherical structure provides a larger surface area and more active sites to adsorb and activate the reaction gases. In addition, the uniform distribution and strong interaction of manganese, iron, cerium, and titanium oxide species improved H2O and SO2 resistance. The results showed that the Mn–Ce–Fe–Ti(CP-SD) catalyst could be used prospectively as a denitration(De-NOx) catalyst.展开更多
Reducing the NO_(x) emission from pelletizing process is of great importance to the green development of iron and steel industry.The flue gas temperature of preheating(PH)section during grate-kiln iron ore pelletizing...Reducing the NO_(x) emission from pelletizing process is of great importance to the green development of iron and steel industry.The flue gas temperature of preheating(PH)section during grate-kiln iron ore pelletizing process typically ranges within 850–1050℃,which meets the temperature requirements of selective non-catalytic reduction(SNCR)for NO_(x).The in-bed SNCR behavior of NO_(x) in the PH section was investigated,and the influence of relevant parameters was revealed.Results show that with the flue gas temperature rising,the denitration rate reached a peak value and then declined,where the appropriate temperature range was 950–1000℃.Increasing the NH_(3)/NO ratio(NSR)contributed to improving the denitration rate,and the appropriate NSR was 1.0.Oxygen content in the flue gas also showed an important influence on denitration rate,which reached a peak value and then dropped with the oxygen content rising.Under the condition of 18 vol.%oxygen content,the denitration reaction mainly occurred in the form of 4NO+4NH_(3)+O_(2)=4N_(2)+6H_(2)O.For restricting the competitive reaction of NH_(3) oxidation,the oxygen content in flue gas of PH section should be kept at an appropriate range.In general,the denitration rate reached about 25%in the PH section through spraying ammonia.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
Based on the basic principle and mechanism of flue gas denitrification,the commonly used catalysts for flue gas denitrification were introduced firstly,and then the catalytic performance,stability and reaction mechani...Based on the basic principle and mechanism of flue gas denitrification,the commonly used catalysts for flue gas denitrification were introduced firstly,and then the catalytic performance,stability and reaction mechanism of catalysts in the market were analyzed.Different types of catalysts were studied to look for green catalysts with high activity,sulfur resistance,water vapor resistance and other advantages.The mechanism of denitration reaction of green catalysts was discussed,and the laws of formation,propagation and consumption of active species in the reaction process were revealed to provide theoretical basis for optimizing catalyst design and improving reaction conditions.Then the research status and problems of new catalysts for flue gas denitrification were described.Finally,the future development direction of green catalysts for flue gas denitration was discussed to improve the performance and stability of catalysts and meet the performance requirements of denitration catalysts in different industries.展开更多
基金Supported by the Natural Science Foundation of Shandong Province （No.Z2006F04） and Science and Technology Program for Environment Protection of Shandong Province （No.2006046）.
文摘Abstract The detailed kinetic model of selective non-catalytic reduction （SNCR） of nitric oxide, including so-dium species reactions, was deyeloped on the basis of recent studies on thermal DeNOx mechanism, NOxOUTmechanism and promotion mechanism of Na2CO3. The model was validated by comparison with several experi-mental findings, thus providing an effective tool for the primary and promoted SNCR process simulation. Experimental and simulated results show part-per-million level of sodium carbonate enhances NO removal efficiency andextend the effective SNCR temperature range in comparison with use of a nitrogen agent alone. The kinetic modeling, sensitivity and rate-of-production analysis suggest that the performance improvement can be explained as ho-mogeneous sodium species reactions producing more reactive OH radicals. The net result of sodium species reac-tions is conversion of H2O and inactive HO2 radicals into reactive OH radicals, i.e. H2O＋HO2=3OH, which enhances the SNCR performance of nitrogen agents by mainly increasing the production rate of NH2 radicals. More-over, N2O and CO are eliminated diversely via the reactions Na＋N20=NaO＋N2, NaO＋CO=Na＋CO2 andNaO2＋CO =NaO＋CO2, in.the pro.moted SNCR process, especially in the NOxOUT process.
基金Supported by the National Natural Science Foundation of China(51206096)
文摘An experimental study of thermal de-NOx using NH3 as reductant in 02/C02 atmosphere with the effect of S02 and different additives was performed in a drop tube furnace. Results show that the optimum temperature win- dow is 841-1184 ℃, and the optimum reaction temperature is about 900 ℃ with a de-NOx efficiency of 95.4%. A certain amount of S02 has an inhibiting effect on NO reduction. The effect of additives, including Na2C03, C2H5OH and FeCI3, on NO reduction by NH3 is also explored. The addition of Na2CO3 and FeCI3 is useful to widen the tem- perature window and shift the reaction to lower temperature for the efficiency is increased from 30.5% to 74.0% and 67.4% respectively at 800 ℃. Qualitatively, the modeling results using a detailed kinetic modeling mecha- nism represent well most of the process features. The effect of Na2CO3, C2H5OH and FeCI3 addition can be reproduced well by the Na2C03, C2H5OH and Fe（CO）5 sub-mechanism respectively. The reaction mechanism analysis shows that the effects of these additives on NO reduction are achieved mainly by promoting the produc- tion of OH radicals at lower temperature.
文摘Nitrous oxide is not an environmentally regulated species in the U.S., but it does participate in the stratospheric ozone chemistry and contributes to the greenhouse effect. Nitrous oxide has been found to be a by-product of the selective non-catalytic reduction process. Chemical kinetic calculations demonstrated that the formation of nitrous oxide in the urea-based selective non-catalytic reduction process is linked to the conversion of NO by cyano species released from the process parent compounds. This conversion occurs within in temperature window between 850 and 1050℃. With urea injection, nitrous oxide emissions represent up to 20 percent conversion of the NOx reduced. The amount of nitrous oxide formed depends primarily on the process temperature, the amount of chemical injected, the initial NOx level, and the carbon monoxide level in the gas stream. These observations, which were based on the chemical kinetics of the process, should be considered in designing selective non-catalytic reduction systems to minimize nitrous oxide by- product formation.
基金supported by Major Scientific and Technological Project of Bingtuan (No.2018AA002)the Program for Changjiang Scholars and Innovative Research Team in University (No. IRT_15R46)
文摘We rationally designed a high performance denitration(De-NOx) catalyst based on a micrometer-sized spherical Mn–Ce–Fe–Ti(CP-SD)catalyst for selective catalytic reduction(SCR). This was prepared by a co-precipitation and spray drying(CP-SD) method. The catalyst was systematically characterized, and its morphological structure and surface properties were identified. Compare with conventional Mn–Ce–Fe–Ti(CP) catalysts, the Mn–Ce–Fe–Ti(CP-SD) catalyst had superior surface-adsorbed oxygen leading to enhanced 'fast NH3-SCR' reaction. The asobtained Mn–Ce–Fe–Ti(CP-SD) catalyst offered excellent NO conversion and N2 selectivity of 100.0% and 84.8% at 250℃, respectively, with a gas hourly space velocity(GHSV) of 40,000 h-1. The porous micro-spherical structure provides a larger surface area and more active sites to adsorb and activate the reaction gases. In addition, the uniform distribution and strong interaction of manganese, iron, cerium, and titanium oxide species improved H2O and SO2 resistance. The results showed that the Mn–Ce–Fe–Ti(CP-SD) catalyst could be used prospectively as a denitration(De-NOx) catalyst.
基金This work was supported by the National Natural Science Foundation of China(51974371)Key Research and Development Program of Hunan Province(2018SK2049).
文摘Reducing the NO_(x) emission from pelletizing process is of great importance to the green development of iron and steel industry.The flue gas temperature of preheating(PH)section during grate-kiln iron ore pelletizing process typically ranges within 850–1050℃,which meets the temperature requirements of selective non-catalytic reduction(SNCR)for NO_(x).The in-bed SNCR behavior of NO_(x) in the PH section was investigated,and the influence of relevant parameters was revealed.Results show that with the flue gas temperature rising,the denitration rate reached a peak value and then declined,where the appropriate temperature range was 950–1000℃.Increasing the NH_(3)/NO ratio(NSR)contributed to improving the denitration rate,and the appropriate NSR was 1.0.Oxygen content in the flue gas also showed an important influence on denitration rate,which reached a peak value and then dropped with the oxygen content rising.Under the condition of 18 vol.%oxygen content,the denitration reaction mainly occurred in the form of 4NO+4NH_(3)+O_(2)=4N_(2)+6H_(2)O.For restricting the competitive reaction of NH_(3) oxidation,the oxygen content in flue gas of PH section should be kept at an appropriate range.In general,the denitration rate reached about 25%in the PH section through spraying ammonia.
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 Interdisciplinary Team Project of Shenyang University of Technology in 2021:Green and Low-carbon(Technology and Evaluation)of Typical Industries of Carbon Peak(2021-70-06)"Double First-class"Construction Project of Liaoning Province in 2020(Scientific Research)(FWDFGD2020041).
文摘Based on the basic principle and mechanism of flue gas denitrification,the commonly used catalysts for flue gas denitrification were introduced firstly,and then the catalytic performance,stability and reaction mechanism of catalysts in the market were analyzed.Different types of catalysts were studied to look for green catalysts with high activity,sulfur resistance,water vapor resistance and other advantages.The mechanism of denitration reaction of green catalysts was discussed,and the laws of formation,propagation and consumption of active species in the reaction process were revealed to provide theoretical basis for optimizing catalyst design and improving reaction conditions.Then the research status and problems of new catalysts for flue gas denitrification were described.Finally,the future development direction of green catalysts for flue gas denitration was discussed to improve the performance and stability of catalysts and meet the performance requirements of denitration catalysts in different industries.
