Excessive emissions of nitrogen oxides from flue gas have imposed various detrimental impacts on environment,and the development of deNO_(x) catalysts with low-cost and high performance is an urgent requirement.Iron o...Excessive emissions of nitrogen oxides from flue gas have imposed various detrimental impacts on environment,and the development of deNO_(x) catalysts with low-cost and high performance is an urgent requirement.Iron oxide-based material has been explored for promising deNO_(x) catalysts.However,the unsatisfactory low-temperature activity limits their practical applications.In this study,a series of excellent low-temperature denitrification catalysts(Ha-FeO_(x)/yZS)were prepared by acid treatment of zinc slag,and the mass ratios of Fe to impure ions was regulated by adjusting the acid concentrations.Ha-FeO_(x)/yZS showed high denitrification performance(>90%)in the range of 180–300℃,and the optimal NO conversion and N2 selectivity were higher than 95%at 250℃.Among them,the Ha-FeO_(x)/2ZS synthesized with 2 mol/L HNO3 exhibited the widest temperature window(175–350℃).The excellent denitrification performance of Ha-FeO_(x)/yZS was mainly attributed to the strong interaction between Fe and impurity ions to inhibit the growth of crystals,making Ha-FeO_(x)/yZS with amorphous structure,nice fine particles,large specific surface area,more surface acid sites and high chemisorbed oxygen.The in-situ DRIFT experiments confirmed that the SCR reaction on the Ha-FeO_(x)/yZS followed both Langmuir-Hinshelwood(L-H)mechanism and Eley-Rideal(E-R)mechanism.The present work proposed a high value-added method for the preparation of cost-effective catalysts from zinc slag,which showed a promising application prospect in NO_(x) removal by selective catalytic reduction with ammonia.展开更多
TiO_(2)-supported V_(2)O_(5)catalysts are commonly used in NO_(x)reduction with ammonia due to their robust catalytic performance.Over these catalysts,it is generally considered that the active species are mainly deri...TiO_(2)-supported V_(2)O_(5)catalysts are commonly used in NO_(x)reduction with ammonia due to their robust catalytic performance.Over these catalysts,it is generally considered that the active species are mainly derived from the vanadia species rather than the intrinsic structure of V-O-Ti entities,namely the interface sites.To reveal the role of V-O-Ti entities in NH_(3)-SCR,herein,we prepared TiO_(2)/V_(2)O_(5)catalysts and demonstrated that V-O-Ti entities were more active for NO_(x)reduction under wet conditions than the V sites(V=O)working alone.On the V-O-Ti entities,kinetic measurements and first principles calculations revealed that NH_(3)activation exhibited a much lower energy barrier than that on V=O sites.Under wet conditions,the V-O-Ti interface significantly inhibited the transformation of V=O to V-OH sites thus benefiting NH_(3)activation.Under wet conditions,meanwhile,the migration of NH_(4)^(+)from Ti site neighboring the V-O-Ti interface to Ti site of the V-O-Ti interface was exothermic;thus,V-O-Ti entities together with neighboring Ti sites could serve as channels linking NH_(3)pool and active centers for activation of NH_(4)^(+).This finding reveals that the V-O-Ti interface sites on V-based catalysts play a crucial role in NO_(x)removal under realistic conditions,providing a new perspective on NH_(3)-SCR mechanism.展开更多
The synergetic abatement of multi-pollutants is one of the development trends of flue gas pollution control technology,which is still in the initial stage and facing many challenges.We developed a V_(2)O_(5)/TiO_(2)gr...The synergetic abatement of multi-pollutants is one of the development trends of flue gas pollution control technology,which is still in the initial stage and facing many challenges.We developed a V_(2)O_(5)/TiO_(2)granular catalyst and established the kinetic model for the simultaneous removal of NO and chlorobenzene(i.e.,an important precursor of dioxins).The granular catalyst synthesized using vanadyl acetylacetonate precursor showed good synergistic catalytic performance and stability.Although the SCR reaction of NO and the oxidation reaction of chlorobenzene mutually inhibited,the reaction order of each reaction was not considerably affected,and the pseudo-first-order reaction kinetics was still followed.The performance prediction of this work is of much value to the understanding and reasonable design of a catalytic system for multi-pollutants(i.e.,NO and dioxins)emission control.展开更多
The simultaneous removal of SO_(2),NO_(x)and Hg^(0)from industrial exhaust flue gas has drawn worldwide attention in recent years.A particularly attractive technique is selective catalytic reduction,which effectively ...The simultaneous removal of SO_(2),NO_(x)and Hg^(0)from industrial exhaust flue gas has drawn worldwide attention in recent years.A particularly attractive technique is selective catalytic reduction,which effectively removes SO_(2),NO_(x)and Hg^(0)at low temperatures.This paper first reviews the simultaneous removal of SO_(2),NO_(x)and Hg^(0)by unsupported and supported catalysts.It then describes and compares the research progress of various carriers,eg.,carbon-based materials,metal oxides,silica,molecular sieves,metal-organic frameworks,and pillared interlayered clays,in the simultaneous removal of SO_(2),NO_(x)and Hg^(0).The effects of flue-gas components(such as O_(2),NH3,HCl,H2 O,SO_(2),NO and Hg^(0))on the removal of SO_(2),NOx,and Hg^(0)are discussed comprehensively and systematically.After summarizing the pollutantremoval mechanism,the review discusses future developments in the simultaneous removal of SO_(2),NOx and Hg^(0)by catalysts.展开更多
Simultaneously removal of NO_(x)and VOCs over NH3-SCR catalysts have attracted lots of attention recently.However,the presence of VOCs would have negative effect on deNOx efficiency especially at low temperature.In th...Simultaneously removal of NO_(x)and VOCs over NH3-SCR catalysts have attracted lots of attention recently.However,the presence of VOCs would have negative effect on deNOx efficiency especially at low temperature.In this study,copper modification onto Sb_(0.5)CeZr_(2)O_(x)(SCZ)catalyst were performed to enhance the catalytic performance for simultaneous control of NNO_(x)and methanol.It was obtained that copper addition could improve the low-temperature activity of both NOx conversion and methanol oxidation,where the optimal catalyst(Cu_(0.05)SCZ)exhibited a deNOx activity of 96%and a mineralization rate of 97%at 250℃,which are around 10%higher than that of Cu free sample.The characterization results showed that copper addition could obviously enhance the redox capacity of the catalysts.As such,the inhibition effect of methanol incomplete oxidation on NO adsorption and NH3 activation were then lessened and the conversion of surface formamide species were also accelerated,resulting in the rising of NOx conversion at low temperature.However,excessive copper addition would damage the Sb-Ce-Zr oxides solid solution structure owing to Cu-Ce strong interactions,decreasing the surface area and acidity.Meanwhile,due to easier over-oxidation of NH3 with more Cu addition,the temperature window for NOx conversion would become quite narrow.These findings could provide useful guidelines for the synergistic removal of VOCs over SCR catalyst in real application.展开更多
The significant increase of NO_(x)concentration causes severe damages to environment and human health.Light-driven photocatalytic technique affords an ideal solution for the removal of NO_(x)at ambient conditions.To e...The significant increase of NO_(x)concentration causes severe damages to environment and human health.Light-driven photocatalytic technique affords an ideal solution for the removal of NO_(x)at ambient conditions.To enhance the performance of NO_(x)removal,1D,2D and 3D photocatalysts have been constructed as the light absorption and the separation of charge carriers can be manipulated through controlling the morphology of the photocatalyst.Related works mainly focused on the construction and modification of special morphologic photocatalyst,including element doping,heterostructure constructing,crystal facet exposing,defect sites introducing and so on.Moreover,the excellent performance of the photocatalytic NO_(x)removal creates great awareness of the application,which has promising practical applications in NO_(x)removal by paint(removing NO_(x)indoor and outdoor)and pavement(degrading vehicle exhausts).For these considerations,recent advances in special morphologic photocatalysts for NO_(x)removal was summarized and commented in this review.The purpose is to provide insights into understanding the relationship between morphology and photocatalytic performance,meanwhile,to promote the application of photocatalytic technology in NO_(x)degradation.展开更多
Low-temperature selective catalytic reduction(SCR)is important for the elimination of NOfrom stationary sources.In the present study,the loading of Ce and W onα-Fe_(2)O_(3)was achieved through the integration of sing...Low-temperature selective catalytic reduction(SCR)is important for the elimination of NOfrom stationary sources.In the present study,the loading of Ce and W onα-Fe_(2)O_(3)was achieved through the integration of single-mode microwave and incipient wetness impregnation(IWI)methods.The scanning electron microscopy(SEM)and transmission electron microscopy(TEM)images reveal that the structure ofα-Fe_(2)O_(3)is spindle-like,and the structure remains unchanged after the introduction of Ce and/or W.The results of NH-SCR investigation demonstrate that NOconversion over Ce-W/α-Fe_(2)O_(3)is more than85%at 300℃,which is much higher than that over Ce/a-Fe_(2)O_(3)andα-Fe_(2)O_(3),Our studies illustrate that the addition of Ce can significantly increase the amount of surface oxygen vacancies as well as sites of moderate basicity.On the other hand,the addition of W can obviously decrease the amount of basic sites and increase the number of Br?nsted acid sites.The synergistic effect of Ce and W addition on balancing acidity/basicity properties accounts for the high activity of CeW/α-Fe_(2)O_(3)for NOremoval at low temperatures.The study provides insight into the relationship between acidity/basicity properties and catalytic performance of Ce-W/α-Fe_(2)O_(3)catalysts,which is beneficial to the design of high-performance NH-SCR catalyst for NOremoval at low temperatures.展开更多
Green and efficient NO_(x)removal at low temperature is still desired.NO_(x)removal via non-thermal plasma(NTP)reduction is one of such technique.This work presents the experimental and theoretical study on the NO_(x)...Green and efficient NO_(x)removal at low temperature is still desired.NO_(x)removal via non-thermal plasma(NTP)reduction is one of such technique.This work presents the experimental and theoretical study on the NO_(x)removal via NTP reduction(NTPRD)in dielectric barrier discharge reactor(DBD).The effect of O_(2)molar fraction on NO_(x)species in the outlet of DBD,and effects of NH_(3)/NO_(x)molar ratio and discharge power of DBD on NO_(x)removal efficiency are investigated.Results indicate that anaerobic condition and higher discharge power is beneficial to direct removal of NO_(x),and the NO_(x),removal efficiency can be up to 98.5%under the optimal operating conditions.It is also found that adding NH_(3)is favorable for the reduction of NO_(x),to N_(2)at lower discharge power.In addition,the NO_(x)removal mechanism and energy consumption analysis for the NTPRD process are also studied.It is found that the reduced active species(N^(+),N^(-),N^(+),N_(2)^(*),NH_(2)^(+),etc.)generated in the NTPRD process play important roles for the reduction of NO_(x),to N_(2).Our work paves a novel pathway for NO_(x)removal from anaerobic gas in industrial application.展开更多
基金National Natural Science Foundation of China(21676209)Natural Science Basic Research Program of Shaanxi(2022JQ-328)Postdoctoral Research Foundation of the Xi’an University of Architecture and Technology(19603210120).
文摘Excessive emissions of nitrogen oxides from flue gas have imposed various detrimental impacts on environment,and the development of deNO_(x) catalysts with low-cost and high performance is an urgent requirement.Iron oxide-based material has been explored for promising deNO_(x) catalysts.However,the unsatisfactory low-temperature activity limits their practical applications.In this study,a series of excellent low-temperature denitrification catalysts(Ha-FeO_(x)/yZS)were prepared by acid treatment of zinc slag,and the mass ratios of Fe to impure ions was regulated by adjusting the acid concentrations.Ha-FeO_(x)/yZS showed high denitrification performance(>90%)in the range of 180–300℃,and the optimal NO conversion and N2 selectivity were higher than 95%at 250℃.Among them,the Ha-FeO_(x)/2ZS synthesized with 2 mol/L HNO3 exhibited the widest temperature window(175–350℃).The excellent denitrification performance of Ha-FeO_(x)/yZS was mainly attributed to the strong interaction between Fe and impurity ions to inhibit the growth of crystals,making Ha-FeO_(x)/yZS with amorphous structure,nice fine particles,large specific surface area,more surface acid sites and high chemisorbed oxygen.The in-situ DRIFT experiments confirmed that the SCR reaction on the Ha-FeO_(x)/yZS followed both Langmuir-Hinshelwood(L-H)mechanism and Eley-Rideal(E-R)mechanism.The present work proposed a high value-added method for the preparation of cost-effective catalysts from zinc slag,which showed a promising application prospect in NO_(x) removal by selective catalytic reduction with ammonia.
基金supported by the National Natural Science Foundation of China (Nos.U20B6004,22072179,and 22276202)the Strategic Priority Research Program of the Chinese Academy of Sciences (No.XDA23010200)+1 种基金the Special project of eco-environmental technology for peak carbon dioxide emissions and carbon neutrality (No.RCEES-TDZ2021-2)the Youth Innovation Promotion Association of the Chinese Academy of Sciences (No.2019045)。
文摘TiO_(2)-supported V_(2)O_(5)catalysts are commonly used in NO_(x)reduction with ammonia due to their robust catalytic performance.Over these catalysts,it is generally considered that the active species are mainly derived from the vanadia species rather than the intrinsic structure of V-O-Ti entities,namely the interface sites.To reveal the role of V-O-Ti entities in NH_(3)-SCR,herein,we prepared TiO_(2)/V_(2)O_(5)catalysts and demonstrated that V-O-Ti entities were more active for NO_(x)reduction under wet conditions than the V sites(V=O)working alone.On the V-O-Ti entities,kinetic measurements and first principles calculations revealed that NH_(3)activation exhibited a much lower energy barrier than that on V=O sites.Under wet conditions,the V-O-Ti interface significantly inhibited the transformation of V=O to V-OH sites thus benefiting NH_(3)activation.Under wet conditions,meanwhile,the migration of NH_(4)^(+)from Ti site neighboring the V-O-Ti interface to Ti site of the V-O-Ti interface was exothermic;thus,V-O-Ti entities together with neighboring Ti sites could serve as channels linking NH_(3)pool and active centers for activation of NH_(4)^(+).This finding reveals that the V-O-Ti interface sites on V-based catalysts play a crucial role in NO_(x)removal under realistic conditions,providing a new perspective on NH_(3)-SCR mechanism.
基金We gratefully acknowledge the National Natural Science Foundation of China(Grant Nos.21876093 and 21777081).
文摘The synergetic abatement of multi-pollutants is one of the development trends of flue gas pollution control technology,which is still in the initial stage and facing many challenges.We developed a V_(2)O_(5)/TiO_(2)granular catalyst and established the kinetic model for the simultaneous removal of NO and chlorobenzene(i.e.,an important precursor of dioxins).The granular catalyst synthesized using vanadyl acetylacetonate precursor showed good synergistic catalytic performance and stability.Although the SCR reaction of NO and the oxidation reaction of chlorobenzene mutually inhibited,the reaction order of each reaction was not considerably affected,and the pseudo-first-order reaction kinetics was still followed.The performance prediction of this work is of much value to the understanding and reasonable design of a catalytic system for multi-pollutants(i.e.,NO and dioxins)emission control.
基金supported by the National Natural Science Foundation of China(Nos.52000093,51968034,41807373 and21667015)National Key R&D Program of China(No.2018YFC0213400)+1 种基金China Postdoctoral Science Foundation(Nos.2020T130271,2019M663911XB)Open Fund of National Engineering Laboratory for Mobile Source Emission Control Technology(No.NELMS2019B03)。
文摘The simultaneous removal of SO_(2),NO_(x)and Hg^(0)from industrial exhaust flue gas has drawn worldwide attention in recent years.A particularly attractive technique is selective catalytic reduction,which effectively removes SO_(2),NO_(x)and Hg^(0)at low temperatures.This paper first reviews the simultaneous removal of SO_(2),NO_(x)and Hg^(0)by unsupported and supported catalysts.It then describes and compares the research progress of various carriers,eg.,carbon-based materials,metal oxides,silica,molecular sieves,metal-organic frameworks,and pillared interlayered clays,in the simultaneous removal of SO_(2),NO_(x)and Hg^(0).The effects of flue-gas components(such as O_(2),NH3,HCl,H2 O,SO_(2),NO and Hg^(0))on the removal of SO_(2),NOx,and Hg^(0)are discussed comprehensively and systematically.After summarizing the pollutantremoval mechanism,the review discusses future developments in the simultaneous removal of SO_(2),NOx and Hg^(0)by catalysts.
基金the fnancial support of Fundamental Research Funds for the Central Universities(No.2021XZZX025)National Natural Science Foundation of China(No.22076164)Research Startup Program of Jaxing University(No.CD70520027).
文摘Simultaneously removal of NO_(x)and VOCs over NH3-SCR catalysts have attracted lots of attention recently.However,the presence of VOCs would have negative effect on deNOx efficiency especially at low temperature.In this study,copper modification onto Sb_(0.5)CeZr_(2)O_(x)(SCZ)catalyst were performed to enhance the catalytic performance for simultaneous control of NNO_(x)and methanol.It was obtained that copper addition could improve the low-temperature activity of both NOx conversion and methanol oxidation,where the optimal catalyst(Cu_(0.05)SCZ)exhibited a deNOx activity of 96%and a mineralization rate of 97%at 250℃,which are around 10%higher than that of Cu free sample.The characterization results showed that copper addition could obviously enhance the redox capacity of the catalysts.As such,the inhibition effect of methanol incomplete oxidation on NO adsorption and NH3 activation were then lessened and the conversion of surface formamide species were also accelerated,resulting in the rising of NOx conversion at low temperature.However,excessive copper addition would damage the Sb-Ce-Zr oxides solid solution structure owing to Cu-Ce strong interactions,decreasing the surface area and acidity.Meanwhile,due to easier over-oxidation of NH3 with more Cu addition,the temperature window for NOx conversion would become quite narrow.These findings could provide useful guidelines for the synergistic removal of VOCs over SCR catalyst in real application.
基金supported by the National Natural Science Foundation of China(Nos.21607027,52002142,51772118,and 51972134)the Opening Project of Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention(LAP3,No.FDLAP19007)+2 种基金and some Foundation of Anhui Province in China:Natural Science Foundation(Nos.1808085J24 and 2108085MB43)the University Natural Science Research Project(No.KJ2020A0126)the Cultivating Outstanding Talents(No.gxbjZD2020066).
文摘The significant increase of NO_(x)concentration causes severe damages to environment and human health.Light-driven photocatalytic technique affords an ideal solution for the removal of NO_(x)at ambient conditions.To enhance the performance of NO_(x)removal,1D,2D and 3D photocatalysts have been constructed as the light absorption and the separation of charge carriers can be manipulated through controlling the morphology of the photocatalyst.Related works mainly focused on the construction and modification of special morphologic photocatalyst,including element doping,heterostructure constructing,crystal facet exposing,defect sites introducing and so on.Moreover,the excellent performance of the photocatalytic NO_(x)removal creates great awareness of the application,which has promising practical applications in NO_(x)removal by paint(removing NO_(x)indoor and outdoor)and pavement(degrading vehicle exhausts).For these considerations,recent advances in special morphologic photocatalysts for NO_(x)removal was summarized and commented in this review.The purpose is to provide insights into understanding the relationship between morphology and photocatalytic performance,meanwhile,to promote the application of photocatalytic technology in NO_(x)degradation.
基金Project supported by the National Natural Science Foundation of China(21703037,22108037)the Natural Science Foundation of Fujian(2018J10691)。
文摘Low-temperature selective catalytic reduction(SCR)is important for the elimination of NOfrom stationary sources.In the present study,the loading of Ce and W onα-Fe_(2)O_(3)was achieved through the integration of single-mode microwave and incipient wetness impregnation(IWI)methods.The scanning electron microscopy(SEM)and transmission electron microscopy(TEM)images reveal that the structure ofα-Fe_(2)O_(3)is spindle-like,and the structure remains unchanged after the introduction of Ce and/or W.The results of NH-SCR investigation demonstrate that NOconversion over Ce-W/α-Fe_(2)O_(3)is more than85%at 300℃,which is much higher than that over Ce/a-Fe_(2)O_(3)andα-Fe_(2)O_(3),Our studies illustrate that the addition of Ce can significantly increase the amount of surface oxygen vacancies as well as sites of moderate basicity.On the other hand,the addition of W can obviously decrease the amount of basic sites and increase the number of Br?nsted acid sites.The synergistic effect of Ce and W addition on balancing acidity/basicity properties accounts for the high activity of CeW/α-Fe_(2)O_(3)for NOremoval at low temperatures.The study provides insight into the relationship between acidity/basicity properties and catalytic performance of Ce-W/α-Fe_(2)O_(3)catalysts,which is beneficial to the design of high-performance NH-SCR catalyst for NOremoval at low temperatures.
基金supported by the National Natural Science Foundation of China(Grant Nos.21878009 and 21725601).
文摘Green and efficient NO_(x)removal at low temperature is still desired.NO_(x)removal via non-thermal plasma(NTP)reduction is one of such technique.This work presents the experimental and theoretical study on the NO_(x)removal via NTP reduction(NTPRD)in dielectric barrier discharge reactor(DBD).The effect of O_(2)molar fraction on NO_(x)species in the outlet of DBD,and effects of NH_(3)/NO_(x)molar ratio and discharge power of DBD on NO_(x)removal efficiency are investigated.Results indicate that anaerobic condition and higher discharge power is beneficial to direct removal of NO_(x),and the NO_(x),removal efficiency can be up to 98.5%under the optimal operating conditions.It is also found that adding NH_(3)is favorable for the reduction of NO_(x),to N_(2)at lower discharge power.In addition,the NO_(x)removal mechanism and energy consumption analysis for the NTPRD process are also studied.It is found that the reduced active species(N^(+),N^(-),N^(+),N_(2)^(*),NH_(2)^(+),etc.)generated in the NTPRD process play important roles for the reduction of NO_(x),to N_(2).Our work paves a novel pathway for NO_(x)removal from anaerobic gas in industrial application.
