The selective catalytic reduction(SCR) of NO_x with NH_3 has been proven to be an efficient technology for NO_x conversion to N_2. However, the catalysts used for SCR usually suffer from the problem of sulfur poisonin...The selective catalytic reduction(SCR) of NO_x with NH_3 has been proven to be an efficient technology for NO_x conversion to N_2. 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 de NO_x catalysts and strategies to reduce deactivation caused by SO_2 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 SO_2-resistance of the catalysts.Several novel catalyst systems that exhibited good SO_2 resistance are also introduced. This paper could provide guidance for the development of highly efficient sulfur-tolerant de NO_x catalysts.展开更多
The reaction mechanisms of selective catalytic reduction(SCR)of nitric oxide(NO)by methane(CH4)over solid superacid-based catalysts were proposed and testified by DRIFTS studies on transient reaction as well as by kin...The reaction mechanisms of selective catalytic reduction(SCR)of nitric oxide(NO)by methane(CH4)over solid superacid-based catalysts were proposed and testified by DRIFTS studies on transient reaction as well as by kinetic models.Catalysts derived from different supports would lead to different reaction pathways,and the acidity of solid superacid played an important role in determining the reaction mechanisms and the catalytic activities.Higher ratios of BrØnsted acid sites to Lewis acid sites would lead to stronger oxidation of methane and then could facilitate the step of methane activation.Strong BrØnsted acid sites would not necessarily lead to better catalytic performance,however,since the active surface NO_(y) species and the corresponding reaction routes were determined by the overall acidity strength of the support.The reaction routes where NO_(2)moiety was engaged as an important intermediate involved moderate oxidation of methane,the rate of which could determine the overall activity.The reaction involving NO moiety was likely to be determined by the step of reduction of NO.Therefore,to enhance the SCR activity of solid superacid catalysts,reactions between appropriate couples of active NO_(y)species and activated hydrocarbon intermediates should be realized by modification of the support acidity.展开更多
By the end of 2010, China had approximately 650 GW of coal-fired electric generating capacity producing almost 75% of the country＇s total electricity generation. As a result of the heavy reliance on coal for electric...By the end of 2010, China had approximately 650 GW of coal-fired electric generating capacity producing almost 75% of the country＇s total electricity generation. As a result of the heavy reliance on coal for electricity generation, emissions of air pollutants, such as nitrogen oxides （NOx）, are increasing. To address these growing emissions, the Ministry of Environmental Protection （MEP） has introduced new NOx emission control policies to encourage the installation of selective catalytic reduction （SCR） technologies on a large number of coalfired electric power plants. There is, however, limited experience with SCR in China. It is therefore useful to explore the lessons from the use of SCR technologies in other countries. This paper provides an overview of SCR technology performance at coal-fired electric power plants demonstrating emission removal rates between 65% and 92%. It also reviews the design and operational challenges that, if not addressed, can reduce the reliability, performance, and cost-effectiveness of SCR technologies. These challenges include heterogeneous flue gas conditions, catalyst degradation, ammonia slip, sulfur trioxide （SO3） formation, and fouling and corrosion of plant equipment. As China and the rest of the world work to reduce greenhouse gas emissions, carbon dioxide （CO2） emissions from parasitic load and urea-to-ammonia conversion may also become more important. If these challenges are properly addressed, SCR can reliably and effectively remove up to 90% of NOx emissions at coal-fired power plants.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
NOx emission abatement catalysts V 2O 5 supported on various TiO 2 including anatase, rutile and mixture of both were investigated with various physico\|chemical measurements such as BET, NH\-3\|TPD, NARP, XRD and ...NOx emission abatement catalysts V 2O 5 supported on various TiO 2 including anatase, rutile and mixture of both were investigated with various physico\|chemical measurements such as BET, NH\-3\|TPD, NARP, XRD and so on, and the effect of TiO\-2 surface properties on the SCR(selective catalytic reduction) activity of V\-2O\-5/TiO\-2 catalysts was studied. It was found that the TiO\-2 surface properties had strong affect on the SCR activity of V\-2O\-5/TiO\-2 catalysts. The stronger acidic property resulted in the higher exposure of active sites as well as the higher SCR activity.展开更多
Selective Catalytic Reduction (SCR) catalysts respond slowly to transient inputs, which is troublesome when designing ammonia feed controllers. An experimental SCR test apparatus installed on a slipstream of a Coo-per...Selective Catalytic Reduction (SCR) catalysts respond slowly to transient inputs, which is troublesome when designing ammonia feed controllers. An experimental SCR test apparatus installed on a slipstream of a Coo-per-Bessemer GMV-4, 2-stroke cycle natural gas engine is utilized. Ammonia (NH3) feed rate control algo-rithm development is carried out. Two control algorithms are evaluated: a feed forward control algorithm, using a pre ammonia injection ceramic NOx sensor and a feed forward plus feedback control algorithm, us-ing a pre ammonia injection ceramic NOx sensor and post catalyst ceramic NOx sensor to generate feedback signals. The feed forward algorithm controls to constant user input NH3/NOx molar ratio. The data show the lack of pressure compensation on the ceramic NOx sensors cause errors in feed forward NOx readings, re-sulting in sub optimal ammonia feed. The feedback system minimizes the post catalyst ceramic NOx sensor signal by adjusting the NH3/NOx molar ratio. The NOx sensors respond to ammonia + NOx;therefore, the feed forward plus feedback algorithm minimizes the sum of NOx emissions and ammonia slip. Successful application of the feedback control minimization technique is demonstrated with feedback periods of 15 and 5 minutes with molar ratio step sizes of 5 and 2.5%, respectively.展开更多
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 NO_x with NH_3 has been proven to be an efficient technology for NO_x conversion to N_2. 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 de NO_x catalysts and strategies to reduce deactivation caused by SO_2 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 SO_2-resistance of the catalysts.Several novel catalyst systems that exhibited good SO_2 resistance are also introduced. This paper could provide guidance for the development of highly efficient sulfur-tolerant de NO_x catalysts.
基金This work was supported by the National Natural Science Foundation of China(Grant No.20677034)the National High-Tech Research and Development(863)Program of China(Grant No.2006AA060301)the New Century Excellent Talents in University of China(No.NCET-2005).
文摘The reaction mechanisms of selective catalytic reduction(SCR)of nitric oxide(NO)by methane(CH4)over solid superacid-based catalysts were proposed and testified by DRIFTS studies on transient reaction as well as by kinetic models.Catalysts derived from different supports would lead to different reaction pathways,and the acidity of solid superacid played an important role in determining the reaction mechanisms and the catalytic activities.Higher ratios of BrØnsted acid sites to Lewis acid sites would lead to stronger oxidation of methane and then could facilitate the step of methane activation.Strong BrØnsted acid sites would not necessarily lead to better catalytic performance,however,since the active surface NO_(y) species and the corresponding reaction routes were determined by the overall acidity strength of the support.The reaction routes where NO_(2)moiety was engaged as an important intermediate involved moderate oxidation of methane,the rate of which could determine the overall activity.The reaction involving NO moiety was likely to be determined by the step of reduction of NO.Therefore,to enhance the SCR activity of solid superacid catalysts,reactions between appropriate couples of active NO_(y)species and activated hydrocarbon intermediates should be realized by modification of the support acidity.
文摘By the end of 2010, China had approximately 650 GW of coal-fired electric generating capacity producing almost 75% of the country＇s total electricity generation. As a result of the heavy reliance on coal for electricity generation, emissions of air pollutants, such as nitrogen oxides （NOx）, are increasing. To address these growing emissions, the Ministry of Environmental Protection （MEP） has introduced new NOx emission control policies to encourage the installation of selective catalytic reduction （SCR） technologies on a large number of coalfired electric power plants. There is, however, limited experience with SCR in China. It is therefore useful to explore the lessons from the use of SCR technologies in other countries. This paper provides an overview of SCR technology performance at coal-fired electric power plants demonstrating emission removal rates between 65% and 92%. It also reviews the design and operational challenges that, if not addressed, can reduce the reliability, performance, and cost-effectiveness of SCR technologies. These challenges include heterogeneous flue gas conditions, catalyst degradation, ammonia slip, sulfur trioxide （SO3） formation, and fouling and corrosion of plant equipment. As China and the rest of the world work to reduce greenhouse gas emissions, carbon dioxide （CO2） emissions from parasitic load and urea-to-ammonia conversion may also become more important. If these challenges are properly addressed, SCR can reliably and effectively remove up to 90% of NOx emissions at coal-fired power plants.
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.
文摘NOx emission abatement catalysts V 2O 5 supported on various TiO 2 including anatase, rutile and mixture of both were investigated with various physico\|chemical measurements such as BET, NH\-3\|TPD, NARP, XRD and so on, and the effect of TiO\-2 surface properties on the SCR(selective catalytic reduction) activity of V\-2O\-5/TiO\-2 catalysts was studied. It was found that the TiO\-2 surface properties had strong affect on the SCR activity of V\-2O\-5/TiO\-2 catalysts. The stronger acidic property resulted in the higher exposure of active sites as well as the higher SCR activity.
文摘Selective Catalytic Reduction (SCR) catalysts respond slowly to transient inputs, which is troublesome when designing ammonia feed controllers. An experimental SCR test apparatus installed on a slipstream of a Coo-per-Bessemer GMV-4, 2-stroke cycle natural gas engine is utilized. Ammonia (NH3) feed rate control algo-rithm development is carried out. Two control algorithms are evaluated: a feed forward control algorithm, using a pre ammonia injection ceramic NOx sensor and a feed forward plus feedback control algorithm, us-ing a pre ammonia injection ceramic NOx sensor and post catalyst ceramic NOx sensor to generate feedback signals. The feed forward algorithm controls to constant user input NH3/NOx molar ratio. The data show the lack of pressure compensation on the ceramic NOx sensors cause errors in feed forward NOx readings, re-sulting in sub optimal ammonia feed. The feedback system minimizes the post catalyst ceramic NOx sensor signal by adjusting the NH3/NOx molar ratio. The NOx sensors respond to ammonia + NOx;therefore, the feed forward plus feedback algorithm minimizes the sum of NOx emissions and ammonia slip. Successful application of the feedback control minimization technique is demonstrated with feedback periods of 15 and 5 minutes with molar ratio step sizes of 5 and 2.5%, respectively.
