Nitric oxide （NO） removal and sulfur dioxide （SO2） removal by sodium persulfate （Na2S2O8） were studied in a Bubble Column Reactor. The proposed reaction pathways of NO and SO2 removal are discussed. The effects ...Nitric oxide （NO） removal and sulfur dioxide （SO2） removal by sodium persulfate （Na2S2O8） were studied in a Bubble Column Reactor. The proposed reaction pathways of NO and SO2 removal are discussed. The effects of temperatures （35-90℃）, Na25208 （0.05-0.5 mol·L-1）, FeSO4 （0.5-5.0 m mol·L-1） and H2O2 （0.25 mol·L-1） on NO and SO2 removal were investigated. The results indicated that increased persulfate concentration led to increase in NO removal at various temperatures. SO2 was almost completely removed in the temperature range of 55-85 ℃. Fe2 ＋ accelerated persulfate activation and enhanced NO removal efficiency. At 0.2 mol· L- 1 Na2S2O8 and 0.5-1.0 mmol· L-1Fe2 ＋, NO removal of 93.5%-99% was obtained at 75-90 ℃, SO2 removal was higher than 99% at all temperatures. The addition of 0.25 mol. L i H202 into 0.2 mol·L-1· Na2S2O8 solution promoted NO removal efficiency apparently until utterly decomposition of H2O2, the SO2 removal was as high as 98.4% separately at 35 ℃ and 80 ℃.展开更多
Absorption and catalytic oxidation of nitric oxide can be achieved by using cobalt（Ⅲ） ethylenediamine （Co（en）3^3＋. When simultaneous absorbing SO2 and NO, the precipitation of Co2（SO3）3 will be yielded and th...Absorption and catalytic oxidation of nitric oxide can be achieved by using cobalt（Ⅲ） ethylenediamine （Co（en）3^3＋. When simultaneous absorbing SO2 and NO, the precipitation of Co2（SO3）3 will be yielded and the NO removal will be decreased. A new catalyst system using Co（en）3^3＋ coupled with urea has been developed to simultaneous remove NO and SO2 in the flue gas. NO is absorbed and catalytically oxidized to nitrite and nitrate by Co（en）3^3＋. The dissolved oxygen in scrubbing solution from the feed stream acts as oxidant. Urea restrains the precipitation of Co2（SO3）3 by oxidizing SO3^2-to SO4^2- as COSO4 is more soluble in water. The experimental results proved that nearly all SO3^2- can be oxidized to SO4^2- and the high NO and SO2 removal could be obtained with the new system. The NO removal is influenced by gas flow rate, the concentration of Co（en）3^3＋ and urea in the absorption solution, the temperature of the scrubbing solution and the content of oxygen in the flue gas. The low gas flow rate is favorable to increase the NO removal. The experiments proved that the NO removal could be maintained at more than 95% by the system of 0.02 mol/L Co（en）3^3＋ and 1% urea at 50℃ with 10% O2 in the flue gas.展开更多
V-Pd/γ-Al2O3-TiO2 catalysts with different vanadium contents were prepared by a combined sol-gel and impregnation method. X-ray diffraction （XRD）, N2 adsorption-desorption （BET）, X-ray photoelectron spectroscopy ...V-Pd/γ-Al2O3-TiO2 catalysts with different vanadium contents were prepared by a combined sol-gel and impregnation method. X-ray diffraction （XRD）, N2 adsorption-desorption （BET）, X-ray photoelectron spectroscopy （XPS） and catalytic removal of ethanol, acetaldehyde and nitrogen oxides at low temperature （〈300 ？C） were used to assess the properties of the catalysts. The results showed that the sample with 1wt% vanadium exhibited an excellent catalytic performance for simultaneous removal of ethanol, acetaldehyde and nitrogen oxides. The conversions of ethanol, acetaldehyde and nitrogen oxides at 250 ？C were 100%, 74.4% and 98.7%, respectively. V-Pd/γ-Al2O3-TiO2 catalyst with 1 wt% vanadium showed the largest surface area and higher dispersion of vanadium oxide on the catalyst surface, and possessed a larger mole fraction of V4＋ species and unique PdO species on the surface, which can be attributed to the strong synergistic effect among palladium, vanadium and the carriers. The higher activity of V-Pd/γ-Al2O3-TiO2 catalyst is related to the V4＋ and Pd2＋ species on the surface, which might be favorable for the formation of active sites.展开更多
MnO2-10aded D301 weak basic anion exchange resin has been used as adsorbent to simultaneously remove lead and cadmium ions from aqueous solution. The effects of adsorbent dosage, solution pH and the coexistent ions on...MnO2-10aded D301 weak basic anion exchange resin has been used as adsorbent to simultaneously remove lead and cadmium ions from aqueous solution. The effects of adsorbent dosage, solution pH and the coexistent ions on the adsorption were investigated. Experimental results showed that with the adsorbent dosage more than 0.6 g/L, both Pb^2＋ and Cd^2＋ were simultaneously removed at pH range 5-6. Except for HPO4^2-, the high concentration coexistent ions such as Na^＋, K^＋, Cl^-, NO3^-, SO4^2- and HCO3^-, showed no significant effect on the removal efficiency of both Pb^2＋ and Cd^2＋ under the experimental conditions. The coexistence of Mg^2＋, Ca^2＋ caused the reduction of Cd^2＋ removal, but not for Pb^2＋. The adsorption equilibrium for Pb^2＋ and Cd^2＋ could be excellently described by the Langmuir isotherm model with R^2 〉 0.99. The maximum adsorption capacity was calculated as 80.64 mg/g for Pb^2＋ and 21.45 mg/g for Cd^2＋. The adsorption processes followed the pseudo first-order kinetics model. MnO2-loaded D301 resin has been shown to have a potential to be used as an effective adsorbent for simultaneous removal of lead and cadmium ions from aqueous solution.展开更多
Reconstituted wood panels have several advantages in terms of ease of manufacturing,but their shorter life span results in a huge amount of reconstituted wood panels being discarded in sorting centers yearly.Currently...Reconstituted wood panels have several advantages in terms of ease of manufacturing,but their shorter life span results in a huge amount of reconstituted wood panels being discarded in sorting centers yearly.Currently,the most common approach for dealing with this waste is incineration.In this study,reconstituted wood panels were converted into activated biochar through a two-step thermochemical process:(i)biochar production using pilot scale fast pyrolysis at 250 kg/h and 450℃;and(ii)a physical activation at three temperatures(750℃,850℃ and 950℃)using an in-house activation furnace(1 kg/h).Results showed that the first stage removed about 66% of the nitrogen from the wood panels in the form of NO,NH3,and trimethylamine,which were detected in small amounts compared to emitted CO_(2).Compared to other types of thermochemical conversion methods(e.g.,slow pyrolysis),isocyanic acid and hydrogen cyanide were not detected in this study.The second stage produced activated biochar with a specific surface area of up to 865 m^(2)/g at 950℃.The volatile gases generated during activation were predominantly composed of toluene and benzene.This two-step process resulted in nitrogen-rich carbon in the form of pyrrolic and pyridinic nitrogen.Activated biochars were then evaluated for their SO_(2) retention performance and showed an excellent adsorption capacity of up to 2140 mg/g compared to 65 mg/g for a commercial activated carbon(889 m^(2)/g).End-of-life reconstituted wood panels and SO_(2) gas are problematic issues in Canada where the economy largely revolves around forestry and mining industries.展开更多
Experiments of simultaneous removal of SO2 and NO from simulated flue gas,using NaClO2 solution as the absorbent,were carried out in a self-designed bubble reactor,and high simultaneous removal effi-ciencies of SO2 an...Experiments of simultaneous removal of SO2 and NO from simulated flue gas,using NaClO2 solution as the absorbent,were carried out in a self-designed bubble reactor,and high simultaneous removal effi-ciencies of SO2 and NO were obtained under the optimal experimental conditions.The mechanism of simultaneous removal based on NaClO2 acid solutions was proposed by analyzing the removal prod-ucts.Possibility and limitation of the desulfurization and denitrification using NaClO2 acid solutions were calculated by thermodynamic methods.Experimental results of reaction kinetics for simultaneous desulfurization and denitrification indicated that the oxidation-absorption processes of SO2 and NO were divided into two zones,namely the fast and slow reaction zones.In the slow reaction zones both were zero order reactions,and in the fast reaction zones,the reaction order,rate constant and activa-tion energy of SO2 reaction with absorbent were 1.4,1.22(mol.L-1)-0.4.s-1 and 66.25kJ.mol-1,respec-tively,and 2,3.15×103(mol.L-1)-1.s-1,and 42.50 kJ.mol-1 for NO reaction,respectively.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
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
Herein,a series of niobium oxide supported cerium nanotubes(Ce NTs)catalysts with different loading amount of Nb_(2)O_(5)(0–10 wt.%)were prepared and used for selective catalytic reduction of NOxwith NH_(3)(NH_(3)-SC...Herein,a series of niobium oxide supported cerium nanotubes(Ce NTs)catalysts with different loading amount of Nb_(2)O_(5)(0–10 wt.%)were prepared and used for selective catalytic reduction of NOxwith NH_(3)(NH_(3)-SCR)in the presence of CH_(2)Cl_(2).Commercial V_(2)O_(5)-WO_(3)-TiO_(2) catalyst was also prepared for comparison.The physcial properties and chemical properties of the Nb_(2)O_(5) loaded cerium nanotubes catalysts were investigated by X-ray diffractometer,Transmission electron microscope,Brunauer-Emmett-Teller specific surface area,H_(2)-temperature programmed reduction,NH_(3)-temperature programmed desorption and Xray photoelectron spectroscopy.The experiment results showed that the loading amount of Nb_(2)O_(5) had a significant effect on the catalytic performance of the catalysts.10 wt.%Nb-Ce NTs catalyst presented the best NH_(3)-SCR performance and degradation efficiency of CH_(2)Cl_(2) among the prepared catalysts,due to its superior redox capability,abundant surface oxygen species and acid sites,the interaction between Nb and Ce,higher ratio of Nb^(4+)/(Nb^(5+)+Nb^(4+))and Ce^(3+)/(Ce^(3+)+Ce^(4+)),as well as the special tubular structure of cerium nanotube.This study may provide a practical approach for the design and synthesis of SCR catalysts for the simultaneously removal NOxand chlorinated volatile organic compounds(CVOCs)emitted from the stationary industrial sources.展开更多
Simultaneous catalytic removal of polychlorinated dibenzo-p-dioxins and dibenzofurans(PCDD/Fs)and nitrogen oxides(NO_(x))emission at low temperature is of great significance to solve the multiple air pollution problem...Simultaneous catalytic removal of polychlorinated dibenzo-p-dioxins and dibenzofurans(PCDD/Fs)and nitrogen oxides(NO_(x))emission at low temperature is of great significance to solve the multiple air pollution problem caused during waste incineration.A novel catalyst with excellent low-temperature activity towards PCDD/Fs catalytic decomposition,as well as selective catalytic reduction(SCR)of NO with NH_(3)is urgently needed to simultaneously control PCDD/Fs and NO emis-sions.Manganese-cerium composite oxides supported on titanium dioxide(MnO_(x)-CeO_(2)/TiO_(2))or TiO_(2)and carbon nano-tubes(CNTs)composite carrier(MnO_(x)-CeO_(2)/TiO_(2)-CNTs)were prepared using sol-gel method,and their catalytic activity towards simultaneous abatement of ortho-dichlorobenzene(o-DCBz,model molecular to simulate PCDD/Fs)and NO was investigated.In comparison with their removal,the simultaneous removal efficiencies of o-DCBz and NO over MnO_(x)-CeO_(2)/TiO_(2)catalyst are lowered to 27.9%and 51.3%at 150℃under the gas hourly space velocity(GHSV)of 15,000 h−1,due to the competition between the reactants for the limited surface acid sites and surface reactive oxygen species.CNTs addition improves the catalytic activity for their simultaneous removal.The optimum condition occurs on MnO_(x)-CeO_(2)/TiO_(2)combined with 20 wt.%CNTs that above 70%of o-DCBz and NO are removed simultaneously.Characterization results reveal that MnO_(x)-CeO_(2)/TiO_(2)-CNTs catalyst with proper CNTs content has larger Brunauer-Emmet-Teller surface area and greatly improved surface acidity property,which are beneficial to both o-DCBz and NO adsorption.Moreover,the relatively higher surface atomic concentration of Mn^(4+)as well as the existence of abundant surface Ce^(3+)atom accelerates the redox cycle of the catalyst and enriches the surface reactive oxygen species.All the above factors alleviate the competition effect between o-DCBz catalytic oxidation and NH_(3)-SCR reaction and are conducive to the simultaneous abatement of o-DCBz and NO.However,excess CNTs make less contribution on enhancing the interaction between Mn atom and Ce atom,thereby result-ing in less improvement in the catalytic activity.展开更多
Poisonous gases,such as H_(2)S and PH3,produced by industrial production harm humans and damage the environment.In this study,H_(2)S and PH3 were simultaneously removed at low temperature by modified activated carbon ...Poisonous gases,such as H_(2)S and PH3,produced by industrial production harm humans and damage the environment.In this study,H_(2)S and PH3 were simultaneously removed at low temperature by modified activated carbon fiber(ACF)catalysts.We have considered the active metal type,content,precursor,calcination,and reaction temperature.Experimental results exhibited that ACF could best perform by loading 15%Cu from nitrate.The optimized calcination temperature and reaction temperature separately were 550℃ and 90℃.Under these conditions,the most removal capacity could reach 69.7 mg/g and 132.1 mg/g,respectively.Characterization results showed that moderate calcination temperature(550℃)is suitable for the formation of the copper element on the surface of ACF,lower or higher temperature will generate more cuprous oxide.Although both can exhibit catalytic activity,the role of the copper element is significantly greater.Due to the exceptional dispersibility of copper(oxide),the ACF can still maintain the advantages of larger specific surface area and pore volume after loading copper,which is the main reason for better performance of related catalysts.Finally,increasing the copper loading amount can significantly increase the crystallinity and particle size of copper(oxide)on the ACF,thereby improving its catalytic performance.In situ IR found that the reason for the deactivation of the catalyst should be the accumulation of generated H_(2)PO_(4)^(-) and S0_(4)^(2-)(H_(2)0)^(6) which could poison the catalyst.展开更多
基金Supported by the National Natural Science Foundation of China(21536009)Science and Technology Plan Projects of Shaanxi Province(2017ZDCXL-GY-10-03)
文摘Nitric oxide （NO） removal and sulfur dioxide （SO2） removal by sodium persulfate （Na2S2O8） were studied in a Bubble Column Reactor. The proposed reaction pathways of NO and SO2 removal are discussed. The effects of temperatures （35-90℃）, Na25208 （0.05-0.5 mol·L-1）, FeSO4 （0.5-5.0 m mol·L-1） and H2O2 （0.25 mol·L-1） on NO and SO2 removal were investigated. The results indicated that increased persulfate concentration led to increase in NO removal at various temperatures. SO2 was almost completely removed in the temperature range of 55-85 ℃. Fe2 ＋ accelerated persulfate activation and enhanced NO removal efficiency. At 0.2 mol· L- 1 Na2S2O8 and 0.5-1.0 mmol· L-1Fe2 ＋, NO removal of 93.5%-99% was obtained at 75-90 ℃, SO2 removal was higher than 99% at all temperatures. The addition of 0.25 mol. L i H202 into 0.2 mol·L-1· Na2S2O8 solution promoted NO removal efficiency apparently until utterly decomposition of H2O2, the SO2 removal was as high as 98.4% separately at 35 ℃ and 80 ℃.
文摘Absorption and catalytic oxidation of nitric oxide can be achieved by using cobalt（Ⅲ） ethylenediamine （Co（en）3^3＋. When simultaneous absorbing SO2 and NO, the precipitation of Co2（SO3）3 will be yielded and the NO removal will be decreased. A new catalyst system using Co（en）3^3＋ coupled with urea has been developed to simultaneous remove NO and SO2 in the flue gas. NO is absorbed and catalytically oxidized to nitrite and nitrate by Co（en）3^3＋. The dissolved oxygen in scrubbing solution from the feed stream acts as oxidant. Urea restrains the precipitation of Co2（SO3）3 by oxidizing SO3^2-to SO4^2- as COSO4 is more soluble in water. The experimental results proved that nearly all SO3^2- can be oxidized to SO4^2- and the high NO and SO2 removal could be obtained with the new system. The NO removal is influenced by gas flow rate, the concentration of Co（en）3^3＋ and urea in the absorption solution, the temperature of the scrubbing solution and the content of oxygen in the flue gas. The low gas flow rate is favorable to increase the NO removal. The experiments proved that the NO removal could be maintained at more than 95% by the system of 0.02 mol/L Co（en）3^3＋ and 1% urea at 50℃ with 10% O2 in the flue gas.
基金supported by the National Natural Science Foundation of China (No. 21073131)the Shanxi Natural Science Foundation(No. 2009011011-3)
文摘V-Pd/γ-Al2O3-TiO2 catalysts with different vanadium contents were prepared by a combined sol-gel and impregnation method. X-ray diffraction （XRD）, N2 adsorption-desorption （BET）, X-ray photoelectron spectroscopy （XPS） and catalytic removal of ethanol, acetaldehyde and nitrogen oxides at low temperature （〈300 ？C） were used to assess the properties of the catalysts. The results showed that the sample with 1wt% vanadium exhibited an excellent catalytic performance for simultaneous removal of ethanol, acetaldehyde and nitrogen oxides. The conversions of ethanol, acetaldehyde and nitrogen oxides at 250 ？C were 100%, 74.4% and 98.7%, respectively. V-Pd/γ-Al2O3-TiO2 catalyst with 1 wt% vanadium showed the largest surface area and higher dispersion of vanadium oxide on the catalyst surface, and possessed a larger mole fraction of V4＋ species and unique PdO species on the surface, which can be attributed to the strong synergistic effect among palladium, vanadium and the carriers. The higher activity of V-Pd/γ-Al2O3-TiO2 catalyst is related to the V4＋ and Pd2＋ species on the surface, which might be favorable for the formation of active sites.
基金supported by the National Mega-Project of Science and Technology of China (No.2008ZX07421-002)the International Cooperation Project of Chinese Ministry of Science and Technology(No.2007DFR90050)
文摘MnO2-10aded D301 weak basic anion exchange resin has been used as adsorbent to simultaneously remove lead and cadmium ions from aqueous solution. The effects of adsorbent dosage, solution pH and the coexistent ions on the adsorption were investigated. Experimental results showed that with the adsorbent dosage more than 0.6 g/L, both Pb^2＋ and Cd^2＋ were simultaneously removed at pH range 5-6. Except for HPO4^2-, the high concentration coexistent ions such as Na^＋, K^＋, Cl^-, NO3^-, SO4^2- and HCO3^-, showed no significant effect on the removal efficiency of both Pb^2＋ and Cd^2＋ under the experimental conditions. The coexistence of Mg^2＋, Ca^2＋ caused the reduction of Cd^2＋ removal, but not for Pb^2＋. The adsorption equilibrium for Pb^2＋ and Cd^2＋ could be excellently described by the Langmuir isotherm model with R^2 〉 0.99. The maximum adsorption capacity was calculated as 80.64 mg/g for Pb^2＋ and 21.45 mg/g for Cd^2＋. The adsorption processes followed the pseudo first-order kinetics model. MnO2-loaded D301 resin has been shown to have a potential to be used as an effective adsorbent for simultaneous removal of lead and cadmium ions from aqueous solution.
基金funded by the Ministere de l’Economie,de la Science et de l’Innovation du Quebec,the Natural Sciences and Engineering Research Council of Canada(NSERC)the Consortium de recherche et innovations en bioprocedes industriels au Quebec(Cribiq)+1 种基金the Canada Research Chair Program,the College of Abitibi-Temiscaminguethe Industrial Waste Technology Centre(Centre Technologique des Residus Industriels)through its partner on this project,Airex Energy.
文摘Reconstituted wood panels have several advantages in terms of ease of manufacturing,but their shorter life span results in a huge amount of reconstituted wood panels being discarded in sorting centers yearly.Currently,the most common approach for dealing with this waste is incineration.In this study,reconstituted wood panels were converted into activated biochar through a two-step thermochemical process:(i)biochar production using pilot scale fast pyrolysis at 250 kg/h and 450℃;and(ii)a physical activation at three temperatures(750℃,850℃ and 950℃)using an in-house activation furnace(1 kg/h).Results showed that the first stage removed about 66% of the nitrogen from the wood panels in the form of NO,NH3,and trimethylamine,which were detected in small amounts compared to emitted CO_(2).Compared to other types of thermochemical conversion methods(e.g.,slow pyrolysis),isocyanic acid and hydrogen cyanide were not detected in this study.The second stage produced activated biochar with a specific surface area of up to 865 m^(2)/g at 950℃.The volatile gases generated during activation were predominantly composed of toluene and benzene.This two-step process resulted in nitrogen-rich carbon in the form of pyrrolic and pyridinic nitrogen.Activated biochars were then evaluated for their SO_(2) retention performance and showed an excellent adsorption capacity of up to 2140 mg/g compared to 65 mg/g for a commercial activated carbon(889 m^(2)/g).End-of-life reconstituted wood panels and SO_(2) gas are problematic issues in Canada where the economy largely revolves around forestry and mining industries.
基金Supported by the National High-Tech Research and Development Program of China("863" Project)(Grant No.2007AA061803)
文摘Experiments of simultaneous removal of SO2 and NO from simulated flue gas,using NaClO2 solution as the absorbent,were carried out in a self-designed bubble reactor,and high simultaneous removal effi-ciencies of SO2 and NO were obtained under the optimal experimental conditions.The mechanism of simultaneous removal based on NaClO2 acid solutions was proposed by analyzing the removal prod-ucts.Possibility and limitation of the desulfurization and denitrification using NaClO2 acid solutions were calculated by thermodynamic methods.Experimental results of reaction kinetics for simultaneous desulfurization and denitrification indicated that the oxidation-absorption processes of SO2 and NO were divided into two zones,namely the fast and slow reaction zones.In the slow reaction zones both were zero order reactions,and in the fast reaction zones,the reaction order,rate constant and activa-tion energy of SO2 reaction with absorbent were 1.4,1.22(mol.L-1)-0.4.s-1 and 66.25kJ.mol-1,respec-tively,and 2,3.15×103(mol.L-1)-1.s-1,and 42.50 kJ.mol-1 for NO reaction,respectively.
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financially supported by National Natural Science Foundation of China(Nos.52070168 and 51708492)National Key Research and Development Plan of China(No.2016YFC0204100)+1 种基金Zhejiang Provincial“151 Talents Programthe Program for Zhejiang Leading Team of S&T Innovation(No.2013TD07)。
文摘Herein,a series of niobium oxide supported cerium nanotubes(Ce NTs)catalysts with different loading amount of Nb_(2)O_(5)(0–10 wt.%)were prepared and used for selective catalytic reduction of NOxwith NH_(3)(NH_(3)-SCR)in the presence of CH_(2)Cl_(2).Commercial V_(2)O_(5)-WO_(3)-TiO_(2) catalyst was also prepared for comparison.The physcial properties and chemical properties of the Nb_(2)O_(5) loaded cerium nanotubes catalysts were investigated by X-ray diffractometer,Transmission electron microscope,Brunauer-Emmett-Teller specific surface area,H_(2)-temperature programmed reduction,NH_(3)-temperature programmed desorption and Xray photoelectron spectroscopy.The experiment results showed that the loading amount of Nb_(2)O_(5) had a significant effect on the catalytic performance of the catalysts.10 wt.%Nb-Ce NTs catalyst presented the best NH_(3)-SCR performance and degradation efficiency of CH_(2)Cl_(2) among the prepared catalysts,due to its superior redox capability,abundant surface oxygen species and acid sites,the interaction between Nb and Ce,higher ratio of Nb^(4+)/(Nb^(5+)+Nb^(4+))and Ce^(3+)/(Ce^(3+)+Ce^(4+)),as well as the special tubular structure of cerium nanotube.This study may provide a practical approach for the design and synthesis of SCR catalysts for the simultaneously removal NOxand chlorinated volatile organic compounds(CVOCs)emitted from the stationary industrial sources.
基金This research is supported by National Natural Science Foundation of China(52006144)Natural Science Foundation of Shanghai(17ZR1419400).
文摘Simultaneous catalytic removal of polychlorinated dibenzo-p-dioxins and dibenzofurans(PCDD/Fs)and nitrogen oxides(NO_(x))emission at low temperature is of great significance to solve the multiple air pollution problem caused during waste incineration.A novel catalyst with excellent low-temperature activity towards PCDD/Fs catalytic decomposition,as well as selective catalytic reduction(SCR)of NO with NH_(3)is urgently needed to simultaneously control PCDD/Fs and NO emis-sions.Manganese-cerium composite oxides supported on titanium dioxide(MnO_(x)-CeO_(2)/TiO_(2))or TiO_(2)and carbon nano-tubes(CNTs)composite carrier(MnO_(x)-CeO_(2)/TiO_(2)-CNTs)were prepared using sol-gel method,and their catalytic activity towards simultaneous abatement of ortho-dichlorobenzene(o-DCBz,model molecular to simulate PCDD/Fs)and NO was investigated.In comparison with their removal,the simultaneous removal efficiencies of o-DCBz and NO over MnO_(x)-CeO_(2)/TiO_(2)catalyst are lowered to 27.9%and 51.3%at 150℃under the gas hourly space velocity(GHSV)of 15,000 h−1,due to the competition between the reactants for the limited surface acid sites and surface reactive oxygen species.CNTs addition improves the catalytic activity for their simultaneous removal.The optimum condition occurs on MnO_(x)-CeO_(2)/TiO_(2)combined with 20 wt.%CNTs that above 70%of o-DCBz and NO are removed simultaneously.Characterization results reveal that MnO_(x)-CeO_(2)/TiO_(2)-CNTs catalyst with proper CNTs content has larger Brunauer-Emmet-Teller surface area and greatly improved surface acidity property,which are beneficial to both o-DCBz and NO adsorption.Moreover,the relatively higher surface atomic concentration of Mn^(4+)as well as the existence of abundant surface Ce^(3+)atom accelerates the redox cycle of the catalyst and enriches the surface reactive oxygen species.All the above factors alleviate the competition effect between o-DCBz catalytic oxidation and NH_(3)-SCR reaction and are conducive to the simultaneous abatement of o-DCBz and NO.However,excess CNTs make less contribution on enhancing the interaction between Mn atom and Ce atom,thereby result-ing in less improvement in the catalytic activity.
基金supported by the National Natural Science Foundation of China(Nos.51968034,41807373 and 22006058)the National Key R&D Program of China(No.2018YFC0213400)the Science and Technology Program of Yunnan Province(No.2019FB069).
文摘Poisonous gases,such as H_(2)S and PH3,produced by industrial production harm humans and damage the environment.In this study,H_(2)S and PH3 were simultaneously removed at low temperature by modified activated carbon fiber(ACF)catalysts.We have considered the active metal type,content,precursor,calcination,and reaction temperature.Experimental results exhibited that ACF could best perform by loading 15%Cu from nitrate.The optimized calcination temperature and reaction temperature separately were 550℃ and 90℃.Under these conditions,the most removal capacity could reach 69.7 mg/g and 132.1 mg/g,respectively.Characterization results showed that moderate calcination temperature(550℃)is suitable for the formation of the copper element on the surface of ACF,lower or higher temperature will generate more cuprous oxide.Although both can exhibit catalytic activity,the role of the copper element is significantly greater.Due to the exceptional dispersibility of copper(oxide),the ACF can still maintain the advantages of larger specific surface area and pore volume after loading copper,which is the main reason for better performance of related catalysts.Finally,increasing the copper loading amount can significantly increase the crystallinity and particle size of copper(oxide)on the ACF,thereby improving its catalytic performance.In situ IR found that the reason for the deactivation of the catalyst should be the accumulation of generated H_(2)PO_(4)^(-) and S0_(4)^(2-)(H_(2)0)^(6) which could poison the catalyst.
