The presence of alkali metals in exhaust gas from stationary resources causes a grand challenge for the practical application of selective catalytic reduction(SCR)of NO_(x) with NH_(3).Here,alkali-resistant NO_(x) red...The presence of alkali metals in exhaust gas from stationary resources causes a grand challenge for the practical application of selective catalytic reduction(SCR)of NO_(x) with NH_(3).Here,alkali-resistant NO_(x) reduction has been successfully implemented via tailoring the electron transfer over Fe and V species on FeVO_(4)/TiO_(2)catalysts.The strong interaction between Fe and V induced electron transfer from V to Fe and strengthened the adsorption and activation of NH_(3)and NO over active VO_(x) sites.In the presence of K_(2)O,the strong electron withdrawing effect of Fe offset the electron donating effect of K on the VO_(x) species,thus protecting the active species VO_(x) to maintain the NO_(x) reduction ability.The enhanced adsorption and activation of NH_(3) allowed SCR reaction to proceed via E-R mechanism even after K_(2)O poisoning.This work elucidated the electronic effects on the alkali metals resistance of traditional ferric vanadate SCR catalysts and provided a promising strategy to design SCR catalysts with superior alkali resistance.展开更多
Molecular sieve catalysts,owing to their unique chemical properties,are widely used as catalysts among various catalytic reactions.Abundant Br?nsted acid sites in molecular sieve catalysts usually enable active compon...Molecular sieve catalysts,owing to their unique chemical properties,are widely used as catalysts among various catalytic reactions.Abundant Br?nsted acid sites in molecular sieve catalysts usually enable active components to disperse well on the catalyst surface,and help to adsorb a large number of gas molecules to achieve maximum catalytic performance.Therefore,a variety of molecular sieve catalysts have been developed and used in the selective catalytic reduction of NO_(x)by NH_(3)(NH_(3)-SCR).For example,Cu molecular sieve catalysts such as Cu-SSZ-13 and Cu-SAPO-34 with wide temperature windows and stable structure are considered and applied as commercial catalysts for NO_(x)removal in diesel vehicles for a long time.Although molecular sieve catalysts possess many advantages,they still cannot avoid the serious deactivation caused by various factors in practical applications.In this review,reasons leading to the deactivation of molecular sieve catalysts for NO_(x)reduction in actual working conditions were concluded.The deactivation mechanisms of molecular sieve catalysts for NO_(x)reduction were analyzed and the corresponding anti-deactivation strategies were summarized.Finally,challenges and prospects of molecular sieve catalysts for NO_(x)reduction were also proposed.展开更多
The study focused on the effects of the interaction between axial and radial secondary air and the reductive intensity in reduction region on combustion characteristics and NO_(x) emission in a 30 kW preheating combus...The study focused on the effects of the interaction between axial and radial secondary air and the reductive intensity in reduction region on combustion characteristics and NO_(x) emission in a 30 kW preheating combustion system.The results revealed that the interaction and reductive intensity influenced the combustion in the down-fired combustor(DFC) and NO_(x) emission greatly.For the temperature distribution,the interaction caused the position of the main combustion region to shift down as R_(2-12)(ratio of axial secondary air flow to radial secondary air flow) decreased or λ_(2)(total secondary air ratio) increased,and there was the interplay between both of their effects.As R_(3-12)(ratio of first-staged tertiary air flow to second-staged tertiary air flow)increased,the decrease in the reductive intensity also caused the above phenomenon,and the peak temperature increased in this region.For the NO_(x) emission,the interaction affected the NO_(x) reduction adversely when λ_(2) or R_(2-12) was higher,and the range of this effect was larger,so that the NO_x emission increased obviously as they increased.The decrease in the reductive intensity caused the NO_(x) emission increased under the homogeneous reduction mechanism,while was unchanged at a high level under the heterogeneous reduction mechanism.For the combustion efficiency,the interaction improved the combustion efficiency as λ_(2) increased when R_(2-12) was lower,while reduced it as λ_(2) increased excessively when R_(2-12) was higher.The proper decrease in the reductive intensity caused the combustion efficiency increased obviously,while was hardly improved further when the intensity decreased excessively.In this study,the lowest NO_(x) emission was only 41.75 mg/m^(3) without sacrificing the combustion efficiency by optimizing the interaction and reductive intensity.展开更多
The presented work reports the selective catalytic reduction(SCR)of NO_(x) assisted by dielectric barrier discharge plasma via simulating marine diesel engine exhaust,and the experimental results demonstrate that the ...The presented work reports the selective catalytic reduction(SCR)of NO_(x) assisted by dielectric barrier discharge plasma via simulating marine diesel engine exhaust,and the experimental results demonstrate that the low-temperature activity of NH_(3)-SCR assisted by non-thermal plasma is enhanced significantly,particularly in the presence of a C_(3)H_(6) additive.Simultaneously,CeMnZrO_(x)@TiO_(2) exhibits strong tolerance to SO_(2) poisoning and superior catalytic stability.It is worthwhile to explore a new approach to remove NO_(x) from marine diesel engine exhaust,which is of vital significance for both academic research and practical applications.展开更多
Substantial NO_(x) emission mitigation is crucial for the synergistic reduction of particulate matter and ozone(O_(3))pollution in China.The traditional air quality model does not consider heterogeneous HONO chemistry...Substantial NO_(x) emission mitigation is crucial for the synergistic reduction of particulate matter and ozone(O_(3))pollution in China.The traditional air quality model does not consider heterogeneous HONO chemistry,leading to uncertainties in estimating the benefits of NO_(x) control.Previous studies have shown that the parameterization of heterogeneous HONO formation increases both the simulated value of sulfate–nitrate–ammonium(SNA)and that of O_(3),thus adding the heterogeneous reactions of HONO into air quality models inevitably leads to changes in the estimated benefits of NO_(x) abatement.Here we investigated the changes in SNA and O_(3)concentrations from NO_(x) emission reduction before and after adding heterogeneous HONO reactions in the Community Multi-Scale Air Quality(CMAQ)model.Including heterogeneous HONO reactions in the simulation improved the benefits of NO_(x) reduction in terms of SNA control in winter.With 80%NO_(x) reduction,the reduction in SNA increased from 36.9%without considering heterogeneous HONO reactions to 42.8%with heterogeneous HONO chemistry.The reduction in the maximum daily 8h average(MDA8)O_(3)in summer caused by NO_(x) reduction increased slightly from 4.7%to 5.2%after adding heterogeneous HONO reactions.The results in this study highlight the enhanced effectiveness of NO_(x) controls for the reduction of SNA and O_(3)after considering heterogeneous HONO formation in a complex chemical ambient,demonstrating the importance of NO_(x) controls in reducing PM2.5 and O_(3)pollution in China.展开更多
基金the National Natural Science Foundation of China(No.22125604)Shanghai Rising-Star Program(No.22QA1403700)Chenguang Program supported by Shanghai Education Development Foundation and Shanghai Municipal Education Commission(No.22Z00354).
文摘The presence of alkali metals in exhaust gas from stationary resources causes a grand challenge for the practical application of selective catalytic reduction(SCR)of NO_(x) with NH_(3).Here,alkali-resistant NO_(x) reduction has been successfully implemented via tailoring the electron transfer over Fe and V species on FeVO_(4)/TiO_(2)catalysts.The strong interaction between Fe and V induced electron transfer from V to Fe and strengthened the adsorption and activation of NH_(3)and NO over active VO_(x) sites.In the presence of K_(2)O,the strong electron withdrawing effect of Fe offset the electron donating effect of K on the VO_(x) species,thus protecting the active species VO_(x) to maintain the NO_(x) reduction ability.The enhanced adsorption and activation of NH_(3) allowed SCR reaction to proceed via E-R mechanism even after K_(2)O poisoning.This work elucidated the electronic effects on the alkali metals resistance of traditional ferric vanadate SCR catalysts and provided a promising strategy to design SCR catalysts with superior alkali resistance.
基金the support from the National Natural Science Foundation of China(No.22125604)the Chenguang Program supported by Shanghai Education Development Foundation and Shanghai Municipal Education Commission(No.22Z00354)。
文摘Molecular sieve catalysts,owing to their unique chemical properties,are widely used as catalysts among various catalytic reactions.Abundant Br?nsted acid sites in molecular sieve catalysts usually enable active components to disperse well on the catalyst surface,and help to adsorb a large number of gas molecules to achieve maximum catalytic performance.Therefore,a variety of molecular sieve catalysts have been developed and used in the selective catalytic reduction of NO_(x)by NH_(3)(NH_(3)-SCR).For example,Cu molecular sieve catalysts such as Cu-SSZ-13 and Cu-SAPO-34 with wide temperature windows and stable structure are considered and applied as commercial catalysts for NO_(x)removal in diesel vehicles for a long time.Although molecular sieve catalysts possess many advantages,they still cannot avoid the serious deactivation caused by various factors in practical applications.In this review,reasons leading to the deactivation of molecular sieve catalysts for NO_(x)reduction in actual working conditions were concluded.The deactivation mechanisms of molecular sieve catalysts for NO_(x)reduction were analyzed and the corresponding anti-deactivation strategies were summarized.Finally,challenges and prospects of molecular sieve catalysts for NO_(x)reduction were also proposed.
基金Youth Innovation Promotion Association,CAS (2019148)CAS Project for Young Scientists in Basic Research (YSBR-028)the National Natural Science Foundation of China (No.52006233) are gratefully acknowledged。
文摘The study focused on the effects of the interaction between axial and radial secondary air and the reductive intensity in reduction region on combustion characteristics and NO_(x) emission in a 30 kW preheating combustion system.The results revealed that the interaction and reductive intensity influenced the combustion in the down-fired combustor(DFC) and NO_(x) emission greatly.For the temperature distribution,the interaction caused the position of the main combustion region to shift down as R_(2-12)(ratio of axial secondary air flow to radial secondary air flow) decreased or λ_(2)(total secondary air ratio) increased,and there was the interplay between both of their effects.As R_(3-12)(ratio of first-staged tertiary air flow to second-staged tertiary air flow)increased,the decrease in the reductive intensity also caused the above phenomenon,and the peak temperature increased in this region.For the NO_(x) emission,the interaction affected the NO_(x) reduction adversely when λ_(2) or R_(2-12) was higher,and the range of this effect was larger,so that the NO_x emission increased obviously as they increased.The decrease in the reductive intensity caused the NO_(x) emission increased under the homogeneous reduction mechanism,while was unchanged at a high level under the heterogeneous reduction mechanism.For the combustion efficiency,the interaction improved the combustion efficiency as λ_(2) increased when R_(2-12) was lower,while reduced it as λ_(2) increased excessively when R_(2-12) was higher.The proper decrease in the reductive intensity caused the combustion efficiency increased obviously,while was hardly improved further when the intensity decreased excessively.In this study,the lowest NO_(x) emission was only 41.75 mg/m^(3) without sacrificing the combustion efficiency by optimizing the interaction and reductive intensity.
基金supported by National Key Research and Development Project of China(No.2019YFC1805503)National Engineering Laboratory for Mobile Source Emission Control Technology(No.NELMS2019A13)+1 种基金the Open Project Program of the State Key Laboratory of Petroleum Pollution Control(No.PPC2019013)Major Science and Technology Projects of Shanxi Province(No.20181102017)。
文摘The presented work reports the selective catalytic reduction(SCR)of NO_(x) assisted by dielectric barrier discharge plasma via simulating marine diesel engine exhaust,and the experimental results demonstrate that the low-temperature activity of NH_(3)-SCR assisted by non-thermal plasma is enhanced significantly,particularly in the presence of a C_(3)H_(6) additive.Simultaneously,CeMnZrO_(x)@TiO_(2) exhibits strong tolerance to SO_(2) poisoning and superior catalytic stability.It is worthwhile to explore a new approach to remove NO_(x) from marine diesel engine exhaust,which is of vital significance for both academic research and practical applications.
基金supported by the Innovation Platform for Academicians of Hainan Province(No.YSPTZX202205)the National Key Research and Development Program of China(No.2022YFC3703404)+2 种基金the National Natural Science Foundation of China(No.22276205)the Excellent Young Talents Project of Yellow River Conservancy Commission(No.HQK-202313)the Research and Development Project of Yellow River Institute of Hydraulic Research(No.HKY-YF-2022-02)。
文摘Substantial NO_(x) emission mitigation is crucial for the synergistic reduction of particulate matter and ozone(O_(3))pollution in China.The traditional air quality model does not consider heterogeneous HONO chemistry,leading to uncertainties in estimating the benefits of NO_(x) control.Previous studies have shown that the parameterization of heterogeneous HONO formation increases both the simulated value of sulfate–nitrate–ammonium(SNA)and that of O_(3),thus adding the heterogeneous reactions of HONO into air quality models inevitably leads to changes in the estimated benefits of NO_(x) abatement.Here we investigated the changes in SNA and O_(3)concentrations from NO_(x) emission reduction before and after adding heterogeneous HONO reactions in the Community Multi-Scale Air Quality(CMAQ)model.Including heterogeneous HONO reactions in the simulation improved the benefits of NO_(x) reduction in terms of SNA control in winter.With 80%NO_(x) reduction,the reduction in SNA increased from 36.9%without considering heterogeneous HONO reactions to 42.8%with heterogeneous HONO chemistry.The reduction in the maximum daily 8h average(MDA8)O_(3)in summer caused by NO_(x) reduction increased slightly from 4.7%to 5.2%after adding heterogeneous HONO reactions.The results in this study highlight the enhanced effectiveness of NO_(x) controls for the reduction of SNA and O_(3)after considering heterogeneous HONO formation in a complex chemical ambient,demonstrating the importance of NO_(x) controls in reducing PM2.5 and O_(3)pollution in China.
