MnCeO_(x)/P84 catalytic filters with spherical,flower-like,cubic and rod-like catalytic interfaces were synthesized respectively,and their catalytic activities in the NH_(3)-SCR reaction were investigated.The MnCeO_(x...MnCeO_(x)/P84 catalytic filters with spherical,flower-like,cubic and rod-like catalytic interfaces were synthesized respectively,and their catalytic activities in the NH_(3)-SCR reaction were investigated.The MnCeO_(x)/P84 catalytic filter with spherical catalytic interfaces(recorded as S-MnCeO_(x)/P84)exhibits the best catalytic denitration performance.The NO_(x)removal efficiency of S-MnCeO_(x)/P84 reaches the highest value of 98.6%at 160℃when the catalyst loading is 100 g/m^(2).At the same time,S-MnCeO_(x)/P84 exhibits good SO_(2)resistance and stability,achieving a NO_(x)removal rate of 83%at 190℃with 30 ppm SO_(2).The characterization results illustrate that the MnCeO_x active component in S-MnCeO_(x)/P84 is present in weak crystalline states,tightly wrapped around the surface of the filter fiber,and uniformly dispersed,and the mesopore is the main pore structure of the S-MnCeO_(x)/P84,which can provide a channel for the catalytic reaction to proceed.At the same time,transmission electron microscopy(TEM)characterization shows that y-MnO_(2)is the main form of MnO_(2)in the S-MnCeO_(x)/P84.Further analysis of H_(2)temperature programmed reduction(H_(2)-TPR).NH_(3)temperature programmed desorption(NH_(3)-TPD)and in-situ diffuse reflectance infrared spectra(DRIFTS)show that S-MnCeO_(x)/P84 has good redox ability at 100-200℃and has abundant Lewis acid sites and Bronsteds acid sites,which provides an important guarantee for its superior low-temperature NH_(3)-SCR denitration performance.展开更多
The implementation of embedded selective catalytic reduction(SCR)denitration in chain grate during iron ore pelletizing process obviates additional flue gas heating.However,the influence of gas components and alkali m...The implementation of embedded selective catalytic reduction(SCR)denitration in chain grate during iron ore pelletizing process obviates additional flue gas heating.However,the influence of gas components and alkali metal on SCR denitration requires attention.The SCR denitration behavior in the preheating section of chain grate was investigated,and the combined influence mechanisms of H_(2)O(g),SO_(2),and potassium were revealed.The results show that the presence of H_(2)O(g)and SO_(2) in the flue gas decreases the NO conversion rate of the catalyst from 96.3%to 79.5%,while potassium adsorbed on the catalyst surface further reduces the NO conversion rate to 74.1%.H_(2)O(g),SO_(2),and potassium in the flue gas form sulfate and potassium salt on the catalyst surface,blocking the pore structure,thereby decreasing the gas adsorption capacity of the catalyst.Moreover,SO_(2) and potassium engage in competitive adsorption and reaction with NH_(3) and NO at the active sites on the catalyst surface,reducing the content and activity of the catalyst effective component.Increasing the flue gas temperature can promote the decomposition of ammonium sulfate and ammonium bisulfate on the catalyst surface,but it has little effect on potassium.Additionally,potassium will exacerbate sulfur poisoning of the catalyst.Hence,the embedded SCR denitration process requires electrostatic precipitation to eliminate the adverse impacts of potassium and thermal regime optimization to raise flue gas temperature to 350℃,thereby increasing NO conversion rate exceeding 85%.展开更多
Zirconium-based metal-organic framework UiO-66 was successfully prepared by solvothermal method,and UiO-66 was modified by adding regulators such as formic acid,acetic acid,and hydrochloric acid.The NH_(3)-SCR reactiv...Zirconium-based metal-organic framework UiO-66 was successfully prepared by solvothermal method,and UiO-66 was modified by adding regulators such as formic acid,acetic acid,and hydrochloric acid.The NH_(3)-SCR reactivity of the samples was evaluated by the denitration activity evaluation system,and the UiO-66 and the regulator-modified UiO-66 were characterized by XRD,SEM,BET,FTIR,TG,NH_(3)-TPD,etc.,the effects of regulator types on the structure and properties of UiO-66 were investigated.The experimental results show that,after adding the modifier,the morphology of UiO-66 changes from irregular quadrilateral with serious agglomeration to particles with regular crystal shape and good dispersibility,and the crystal morphology of the catalyst is improved.In addition,after adding the modifier,UiO-66 has a larger specific surface area and stronger surface acidity,which optimizes the catalytic performance of UiO-66.The catalytic performance test results of NH_(3)-SCR show that the low-temperature activity of UiO-66 is poor,and it only shows a certain catalytic activity at higher temperatures.The catalytic activity of UiO-66 was significantly improved after adding the regulator.Among them,the UiO-66-HCl modified with hydrochloric acid had the best catalytic activity,and the denitration rate reached 70%when the denitration temperature was 380℃.展开更多
In this paper, an integrated desulfurization and denitrification technology is proposed for ultra-low emissions of SO2 and NOx in the steel, power and cement industries. A cost-effective and operationally efficient co...In this paper, an integrated desulfurization and denitrification technology is proposed for ultra-low emissions of SO2 and NOx in the steel, power and cement industries. A cost-effective and operationally efficient control strategy is realized through a forced oxidation-absorption-reduction process, which reduces equipment investment and operating costs. The technology was adapted to continuous and intermittent denitrification in different temperature zones, promoting the recycling of desulfurization and denitrification products. The study also explored the use of a highly active absorbent obtained by the hydration reaction of coal ash and lime from a power company for the desulfurization and denitrification of sintered flue gases in iron and steel mills, which produces by-products that can be used as retarding agents in the cement industry, resulting in a circular economy. The article emphasizes the importance of improving the lime digestion process and developing new denitrification agents for environmentally safe and cost-effective flue gas treatment.展开更多
In order to remove gas-phase mercury and NOx from flue gas, experimental studies on flue gas mercury oxidation removal and denitration of Guizhou anthracite combustion with NH4Br addition were carried out. The influen...In order to remove gas-phase mercury and NOx from flue gas, experimental studies on flue gas mercury oxidation removal and denitration of Guizhou anthracite combustion with NH4Br addition were carried out. The influence of NH4Br addition on the ignition temperature and combustion characteristics was studied using a thermogravimetric analyzer. The effects of the NHaBr addition amount on gas-phase mercury oxidation and removal were investigated in a bench scale of 6 kW fluidized bed combustor （FBC）. Mercury concentrations in flue gas were determined by the Ontario hydro method （OHM） and the mercury mass balance was obtained. Results show that the NH4Br addition has little influence on the ignition temperature of Guizhou anthracite. With the mercury mass balance of 95.47%, the proportion of particulate mercury Hg^p, gaseous mercury Hg^0 and Hg^2＋ are 75.28%, 11.60% and 13. 12%, respectively, as raw coal combustion. The high particulate mercury Hg^p in flue gas is caused by the high unburned carbon content in fly ash. When the NH4Br addition amount increases from 0 to 0. 3%, the concentration of gaseous Hg^0 and Hg^2＋ in flue gas decreases continuously, leading to the Hg^p increase accordingly. The oxidation rate of Hg^0 is positively correlated to the Br addition amount. It demonstrates that coal combustion with NH4Br addition can promote Hg^0 oxidation and removal. NOx concentration in flue gas exhibits a descending trend with the NHaBr addition and the removal rate reaches 17.31% with the addition amount of 0.3%. Adding NH4Br to coal also plays a synergistic role in denitration.展开更多
Gradiently denitrated gun propellant(GDGP)prepared by a“gradient denitration”strategy is obviously superior in progressive burning performance to the traditional deterred gun propellant.Currently,the preparation of ...Gradiently denitrated gun propellant(GDGP)prepared by a“gradient denitration”strategy is obviously superior in progressive burning performance to the traditional deterred gun propellant.Currently,the preparation of GDGP employed a tedious two-step method involving organic solvents,which hinders the large-scale preparation of GDGP.In this paper,GDGP was successfully prepared via a novelty and environmentally friendly one-step method.The obtained samples were characterized by FT-IR,Raman,SEM and XPS.The results showed that the content of nitrate groups gradiently increased from the surface to the core in the surface layer of GDGP and the surface layer of GDGP exhibited a higher compaction than that of raw gun propellant,with a well-preserved nitrocellulose structure.The denitration process enabled the propellant surface with regressive energy density and good progressive burning performance,as confirmed by oxygen bomb and closed bomb test.At the same time,the effects of different solvents on the component loss of propellant were compared.The result showed that water caused the least component loss.Finally,the stability of GDGP was confirmed by methyl-violet test.This work not only provided environmentally friendly,simple and economic preparation of GDGP,but also confirmed the stability of GDGP prepared by this method.展开更多
Sm and Ho were doped in Ce-Mn/TiO_(2)catalyst respectively to enhance its denitration performance at low temperature.X-ray diffraction(XRD),N2adsorption-desorption,X-ray photoelectron spectroscopy(XPS),NH3-temperature...Sm and Ho were doped in Ce-Mn/TiO_(2)catalyst respectively to enhance its denitration performance at low temperature.X-ray diffraction(XRD),N2adsorption-desorption,X-ray photoelectron spectroscopy(XPS),NH3-temperature programmed desorption(NH3-TPD),H2-temperature programmed reduction(H2-TPR)and in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)techniques were used to analyze the structure and performance of catalysts.The results demonstrate that Ho doping increases the amount of acid sites and improves low temperature redox property of Ce-Mn/TiO_(2),which lead to excellent DeNOxperformance of Ho-Ce-Mn/TiO_(2)in the whole reaction temperature range.Sm doping results in decline of redox property,but it is beneficial to increasing the acid sites of Ce-Mn/TiO_(2).The increased surface acid sites and moderate oxidative ability impart Sm-Ce-Mn/TiO_(2)higher denitration activity and N2selectivity at temperature above 150℃.Lewis acid sites and redox property are the main factors affecting the activity of catalysts.Doping of Ho and Sm both improves sulfur resistance performance of Ce-Mn/TiO_(2)by inhibiting the adsorption of SO_(2)and formation of sulfate.Ce-Mn/TiO_(2)modified by Ho shows better sulfur resistance than that doped with Sm because of its more surface acid sites.展开更多
Spent catalyst used for denitration by selective catalytic reduction(spent SCR denitration catalysts) is one of the important urban mines due to the high content of TiO_(2)(~85 wt%) and the massive accumulation amount...Spent catalyst used for denitration by selective catalytic reduction(spent SCR denitration catalysts) is one of the important urban mines due to the high content of TiO_(2)(~85 wt%) and the massive accumulation amount(over 100,000 tons),therefore,value-added reutilization of titanium in spent SCR catalysts is considerably meaningful.In this paper,a novel method is proposed for converting the titanium oxide in spent SCR denitration catalysts to metallic titanium.Specifically,titanium dioxide(TiO_(2)) was firstly obtained from spent SCR denitration catalysts after removing the impurities by hydrometallurgy process.Then,TiO_(2) is converted to Ti_(2)CO by carbothermic reduction method,and Ti_(2)CO was further purified by oleic acid capture.Finally,by utilizing the as-prepared Ti_(2)CO as the consumable anode in the NaCl-KCl molten salt,high-purity metallic titanium was deposited at cathode,all confirming the feasibility for the conversion of low-grade TiO_(2) in the spent catalysts,from 60 wt% to high-purity metallic Ti(99.5 wt%), furthermore,the energy consumption of this process is 3950 kWh tonne-1 Ti,which is lower than that of most traditional titanium metallurgy methods.The method herein can provide new insights for the value-added recycling of titanium resources in urban mines.展开更多
The purpose of this work is to explore the effects of the introduction methods of Ce^4+and Zr^4+on the physicochemical properties,activity,and K tolerance of V2 O5-WO3/TiO2 catalyst for the selective catalytic reducti...The purpose of this work is to explore the effects of the introduction methods of Ce^4+and Zr^4+on the physicochemical properties,activity,and K tolerance of V2 O5-WO3/TiO2 catalyst for the selective catalytic reduction of NOx by NH3.Four different methods,namely pre-impregnation,post-impregnation,coimpregnation,and co-precipitation,were used to synthesize a series of V2 O5-WO3-TiO2-CeO2-ZrO2 catalysts.The catalysts were characterized by XRD,BET,NH3-TPD,XPS,and H2-TPR techniques.Moreover,the activity and anti-K poisoning performance were tested by an NH3-SCR model reaction.The results show that the introduction of Ce^4+and Zr^4+can improve the catalytic performance of V2O5-WO3/TiO2 catalyst,but the impregnation method cannot enhance the anti-K poisoning performance.Ce^4+and Zr^4+introduced by co-precipitation method can effectively improve the tolerance of K,which is mainly due to the incorporation of Ce^4+and Zr^4+into TiO2 lattice to form a uniform TiO2-CeO2-ZrO2 solid solution,resulting in the optimal surface acidity and redox performance,and reducing the decreases caused by Kpoisoning.Furthermore,based on the best introduction method,we further optimized the molar ratio of Ce^4+/Zr^4+,It is found that the catalyst exhibits the best anti-K poisoning performance when the molar ratio of Ce^4+/Zr^4+is 2:1.展开更多
Selective catalytic reduction technology using NH3 as a reducing agent（NH3-SCR） is an effective control method to remove nitrogen oxides. TiO2-supported vanadium oxide catalysts with different levels of Ce and Sb mo...Selective catalytic reduction technology using NH3 as a reducing agent（NH3-SCR） is an effective control method to remove nitrogen oxides. TiO2-supported vanadium oxide catalysts with different levels of Ce and Sb modification were prepared by an impregnation method and were characterized by X-ray diffractometer（XRD）, Brunauer-Emmett-Teller（BET）, Transmission electron microscopy（TEM）, Fourier transform infrared spectroscopy（FT-IR）, UV-Vis diffuse reflectance spectroscopy（UV-Vis DRS）, Raman and Hydrogen temperature-programmed reduction（H2-TPR）. The catalytic activities of V5 CexS by/TiO2 catalysts for denitration were investigated in a fixed bed flow microreactor. The results showed that cerium, vanadium and antimony oxide as the active components were well dispersed on TiO2, and the catalysts exhibited a large number of d-d electronic transitions, which were helpful to strengthen SCR reactivity. The V5 CexS by/TiO2 catalysts exhibited a good low temperature NH3-SCR catalytic activity. In the temperature range of 210 to 400℃, the V5 CexS by/TiO2 catalysts gave NO conversion rates above 90%. For the best V5Ce35Sb2/TiO2 catalyst, at a reaction temperature of 210℃, the NO conversion rate had already reached 90%. The catalysts had different catalytic activity with different Ce loadings. With the increase of Ce loading, the NO conversion rate also increased.展开更多
With the advantages of high combustion efficiency, wide fuel flexibility and low concentrations of discharged pollutants, circulating fluid- ized bed （CFB） boiler has been widely used in recent years. However, in or...With the advantages of high combustion efficiency, wide fuel flexibility and low concentrations of discharged pollutants, circulating fluid- ized bed （CFB） boiler has been widely used in recent years. However, in order to meet the requirement of new emission standard, it＇s necessary to add flue gas desulfurization and denitration devices. In this paper, the choice of flue gas purification processes for CFB boiler has been discussed firstly, and then the economy and rationality of the SNCR ＋ CFB-FGD ＋ COA comprehensive solution to flue gas desulfurization and denitration have been analyzed.展开更多
A series of V2O5 with various morphologies was prepared by the hydrothermal method and loaded on the modified active coke（AC） which was prepared by the impregnation methods. The prepared samples were characterized b...A series of V2O5 with various morphologies was prepared by the hydrothermal method and loaded on the modified active coke（AC） which was prepared by the impregnation methods. The prepared samples were characterized by BET, Boehm titration test, XRD, SEM and EDS. The SEM exhibited that the morphologies of the samples prepared were signifi cantly different from each other. Then the samples prepared were studied on the selective catalytic reduction（SCR） of NO with ammonia in the presence of oxygen. The SCR activity measurements were undertaken in a fixed-bed unit with a sieve plate in the middle. From the contrastive experiments, the results showed that linear V2O5/AC had the best denitration performance and the denitration rate was up to 57.41%. It was speculated that the linear V2O5 with the crystal faces（110） may show the best performance in SCR. And the durability results also showed that linear V2O5/AC produced a denitration rate of 47.7% after three regenerations.展开更多
With the continuous increase of new energy installed capacity in recent years, thermal power units are facing deep peak regulation and frequent start-up and shut down for a long time. SCR denitration is widely used in...With the continuous increase of new energy installed capacity in recent years, thermal power units are facing deep peak regulation and frequent start-up and shut down for a long time. SCR denitration is widely used in power plants in our country. The recommended minimum temperature for continuous operation of the catalyst is 320℃, and the minimum temperature for short-term operation is 300 ~ 310℃. However, in low-load operation, especially in winter, the flue gas temperature can hardly reach the above minimum temperature for short-term operation. In order to protect the catalyst, the denitration system is generally withdrawn from operation. In order to meet the requirements of environmental protection emissions and avoid imposing penalties on environmental protection electricity prices, power plants urgently need to achieve full-load denitrification. Based on the research on the lowest continuous ammonia injection temperature MOT of denitration catalyst, Yangluo Power Plant realized full-load denitration under the condition of zero transformation through operation adjustment. In addition, the 300MW subcritical natural circulation furnace and 600MW supercritical once-through furnace in Yangluo Power Plant have been verified, which reflects the wide applicability of this technology.展开更多
To explore the denitration mechanism of iron-vanadium/activated carbon(Fe-V/AC)catalysts in ammonia-selective catalytic reduction(NH_(3)-SCR),the physicochemical properties of Fe-V/AC catalysts were characterized.The ...To explore the denitration mechanism of iron-vanadium/activated carbon(Fe-V/AC)catalysts in ammonia-selective catalytic reduction(NH_(3)-SCR),the physicochemical properties of Fe-V/AC catalysts were characterized.The denitration activities of the Fe-V/AC catalysts in the range of 150-300℃ were evaluated.The increase in denitration temperature leads to the highest and fastest recovery rate of NO conversion in the 10Fe-15V/AC catalyst.However,more metal oxides were attached to the catalyst surface as the V loading increased,and the accumulation occurred.The surface-active components are FeO,Fe_(2)O_(3),Fe_(3)O_(4),VO_(2),and V_(2)O_(5).In addition,the increase in the V loading induced a series of modification effects.A large amount of Fe^(3+)was reduced to Fe^(2+),and a large amount of V^(4+)was oxidized to V^(5+).The surface oxygen species(O_(α))were transformed into lattice oxygen(O_(β)).The presence of a large amount of V species deteriorated the pore-structure parameters and destroyed the oxygen-containing functional groups.Increasing the V loading can effectively increase the Lewis acid sites,thereby promoting NH_(3) adsorption and NO reduction and increasing the stretching vibration of weakly adsorbed ammonia species on the catalyst.The NH_(3) adsorption process produces a notable increase in the concentration of monodentate nitrite(NH_(4)^(+)).The NH_(3)-SCR denitration mechanism of the Fe-V/AC catalyst includes reaction gas adsorption,catalytic denitration of metal active components,and gas desorption.展开更多
The direct cleavage of C–NO_(2)bonds for reductive denitration of nitroarenes remains a challenging transformation in synthetic organic chemistry.Herein,we report a biocompatible palladium-deposited graphdiyne nanoca...The direct cleavage of C–NO_(2)bonds for reductive denitration of nitroarenes remains a challenging transformation in synthetic organic chemistry.Herein,we report a biocompatible palladium-deposited graphdiyne nanocatalyst(Pd@GDY/DSPE-PEG)that can catalyze reductive denitration of nitroarenes under ambient physiological conditions.Mechanistic studies support this transformation via the oxidative addition of nitroarenes with Pd(0)and subsequent ligand exchange to form arylpalladium hydride.This one-step reductive denitration via Pd@GDY/DSPE-PEG successfully facilitates the repair of the nitrated proteins arising from endogenic ONOO−and restores their physiological function,including blocking the apoptosis pathway in living cells.Moreover,Pd@GDY/DSPE-PEG was further successfully applied for catalytic denitration to reduce the level of 3-nitrotyrosine residues of proteins located in the mouse brain hippocampus in vivo.This study provides an ideal strategy for designing highly active enzymatic mimicking synthetic catalysts for the regulation of the nitrated protein level and the detoxification of nitrative damage of living cells and tissues.展开更多
Ultra-low emission of nitrogen oxide(NO_(x))is an irreversible trend for the development of waste-to-energy industry.But traditional approaches to remove NO_(x) face significant challenge s,such as low denitration eff...Ultra-low emission of nitrogen oxide(NO_(x))is an irreversible trend for the development of waste-to-energy industry.But traditional approaches to remove NO_(x) face significant challenge s,such as low denitration efficiency,complex denitration system,and high investment and operating cost.Here we put forward a novel polymer non-catalytic reduction(PNCR)technology that utilized a new type of polymer agent to remove NO_(x),and the proposed PNCR technology was applied to the existing waste-to-energy plant to test the denitration performance.The PNCR technology demonstrated excellent denitration performance with a NO_(x) emission concentration of<100 mg/Nm^(3) and high denitration efficiency of>75%at the temperature range of 800-900℃,which showed the application feasibility even on the complex and unstable industrial operating conditions.In addition,PNCR and hybrid polymer/selective non-catalytic reduction(PNCR/SNCR)technology possessed remarkable economic advantages including low investment fee and low operating cost of<10 CNY per ton of municipal solid waste(MSW)compared with selective catalytic reduction(SCR)technology.The excellent denitration performance of PNCR technology forebodes a broad industrial application prospect in the field of flue gas cleaning for waste-to-energy plants.展开更多
Nitrogen oxides(NO_(x))present in flue gas are economically renewable N1 resources.Unlike traditional selective catalytic reduction processes that convert NO into N_(2),redirecting NO towards the synthesis of value-ad...Nitrogen oxides(NO_(x))present in flue gas are economically renewable N1 resources.Unlike traditional selective catalytic reduction processes that convert NO into N_(2),redirecting NO towards the synthesis of value-added NH_(3)offers significant practical benefits.In this study,a Ti-based metal-organic framework(Ti-MOF),specifically MIL-125,was utilized as a support for Fe,which was subsequently calcined at 400℃to produce a Fe_(2)O_(3)/TiO_(2)-MOF catalyst.The resulting catalyst demonstrated exceptional performance,achieving 99%NO conversion and 95%NH_(3)selectivity under optimal conditions of 450℃,0.1 MPa,and a gas hourly space velocity of 38000 mL g^(–1)h^(−1).Additionally,the catalyst exhibited excellent stability and resistance to water and sulfur.The high efficiency of Fe_(2)O_(3)/TiO_(2)-MOF is attributed to the abundance of Fe^(2+)sites at the reaction temperature,which enhances NO adsorption and activation.Furthermore,density functional theory calculations suggest that NO undergoes hydrogenation at the N-terminus on the Fe_(2)O_(3)/TiO_(2)-MOF surface,leading directly to NH_(3)synthesis rather than dissociation followed by hydrogenation.This catalyst presents a novel approach for converting NO_(x)into high-value chemical products.展开更多
Ammonia selective catalytic reduction(NH_(3)-SCR)is the most widely used technology in thefield of industrialflue gas denitrification.However,the presence of heavy metals influe gas can seriously affect the performance of...Ammonia selective catalytic reduction(NH_(3)-SCR)is the most widely used technology in thefield of industrialflue gas denitrification.However,the presence of heavy metals influe gas can seriously affect the performance of SCR catalysts,leading to their deactivation or even failure.Therefore,it is of great significance to deeply study the poisoning mechanism of SCR catalysts under the action of heavy metals and how to enhance their resistance to poisoning.This article reviews the reaction mechanism of NH_(3)-SCR technology,compares the impact of heavy metals on the activity of different SCR catalysts,and then discusses in detail the poisoning mechanism of SCR catalysts by heavy metals,including pore blockage,reduction of specific surface area,and destruction of active centers caused by heavy metal deposition,all of which jointly lead to the physical or chemical poisoning of the catalyst.Meanwhile,the mechanism of action when multiple toxicants coexist was analyzed.To effectively address these challenges,the article further summarizes various methods to improve the catalyst's resistance to heavy metal poisoning,such as element doping,structural optimization,and carrier addition,which significantly enhance the heavy metal resistance of the catalyst.Finally,the article provides a prospective analysis of the challenges faced by NH_(3)-SCR catalysts in anti-heavy metal poisoning technology,emphasizing the necessity of in-depth research on the poisoning mechanism,exploration of the mechanism of synergistic action of multiple pollutants,development of comprehensive anti-poisoning strategies,and research on catalyst regeneration technology,in order to promote the development of efficient anti-heavy metal poisoning NH_(3)-SCR catalysts.展开更多
Performance of simultaneous desulfurization and denitration using the solution of NaClO2 and NaClO as new-style complex absorbent was investigated experimentally in self-designed bench scale bubbling reactor. The effe...Performance of simultaneous desulfurization and denitration using the solution of NaClO2 and NaClO as new-style complex absorbent was investigated experimentally in self-designed bench scale bubbling reactor. The effects of main parameters, such as the concentrations of NaClO2 and of NaClO, solution pH and reaction temperature and so on, on removal efficiencies of SO2 and NOx, were examined, then the optimal conditions were established, in which the molar ratio of NaClO to NaClO2 was 1：1, the reaction temperature was 50℃ and the solution pH was 5.5. The removal efficiencies of SO2 and NO under the optimal conditions were 100% and 89.2%, respectively. The mechanism of simultaneous removal based on complex absorbent was proposed by analyzing the removal products and the electrode potentials of related species, namely SO2 and NO are oxi- dized by chlorite anion, hypochlorite, chlorine dioxide and chlorine contained in complex absorbent. In thermodynamic aspect, simultaneous desulfurization and denitration reactions in liquid phase can happen spontaneously and completely, and are all exothermic reactions. It was confirmed by kinetics that for simultaneous desulfurization and denitration, the reaction order and average activation energy of SO2 were 1 and 21.6 kJ·mol^-1, respectively, and those of NO were 1 and 8.2 kJ·mol^-1, respectively.展开更多
We herein present an efficient denitrative iodination method of(hetero)nitroarenes mediated by commercially available and cost-effective hydroiodic acid(HI).During the reaction process,HI plays its dual roles as both ...We herein present an efficient denitrative iodination method of(hetero)nitroarenes mediated by commercially available and cost-effective hydroiodic acid(HI).During the reaction process,HI plays its dual roles as both the sustainable reductant of nitro group and iodine source in the iodination step,which successfully integrates three steps into a one-pot procedure and significantly simplifies the reaction system.This approach enables a smooth metal-free conversion of nitroarenes to corresponding aryl iodides via one-pot process,exhibits a broad substrate scope and good reaction efficiency,and was conveniently applied in the concise synthesis of pharmaceuticals.展开更多
基金Project supported by the National Natural Science Foundation of China(51902166)the Natural Science Foundation of Jiangsu Province(BK20190786)+1 种基金Jiangsu Collaborative Innovation Center of Atmospheric Environment and Equipment Technology(CICAEET)Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control。
文摘MnCeO_(x)/P84 catalytic filters with spherical,flower-like,cubic and rod-like catalytic interfaces were synthesized respectively,and their catalytic activities in the NH_(3)-SCR reaction were investigated.The MnCeO_(x)/P84 catalytic filter with spherical catalytic interfaces(recorded as S-MnCeO_(x)/P84)exhibits the best catalytic denitration performance.The NO_(x)removal efficiency of S-MnCeO_(x)/P84 reaches the highest value of 98.6%at 160℃when the catalyst loading is 100 g/m^(2).At the same time,S-MnCeO_(x)/P84 exhibits good SO_(2)resistance and stability,achieving a NO_(x)removal rate of 83%at 190℃with 30 ppm SO_(2).The characterization results illustrate that the MnCeO_x active component in S-MnCeO_(x)/P84 is present in weak crystalline states,tightly wrapped around the surface of the filter fiber,and uniformly dispersed,and the mesopore is the main pore structure of the S-MnCeO_(x)/P84,which can provide a channel for the catalytic reaction to proceed.At the same time,transmission electron microscopy(TEM)characterization shows that y-MnO_(2)is the main form of MnO_(2)in the S-MnCeO_(x)/P84.Further analysis of H_(2)temperature programmed reduction(H_(2)-TPR).NH_(3)temperature programmed desorption(NH_(3)-TPD)and in-situ diffuse reflectance infrared spectra(DRIFTS)show that S-MnCeO_(x)/P84 has good redox ability at 100-200℃and has abundant Lewis acid sites and Bronsteds acid sites,which provides an important guarantee for its superior low-temperature NH_(3)-SCR denitration performance.
基金financially supported by the National Key Research and Development Program of China(No.2023YFC3707002)Hunan Provincial Innovation Foundation for Postgraduate(No.QL20220069)Postgraduate Innovative Project of Central South University(No.1053320214756).
文摘The implementation of embedded selective catalytic reduction(SCR)denitration in chain grate during iron ore pelletizing process obviates additional flue gas heating.However,the influence of gas components and alkali metal on SCR denitration requires attention.The SCR denitration behavior in the preheating section of chain grate was investigated,and the combined influence mechanisms of H_(2)O(g),SO_(2),and potassium were revealed.The results show that the presence of H_(2)O(g)and SO_(2) in the flue gas decreases the NO conversion rate of the catalyst from 96.3%to 79.5%,while potassium adsorbed on the catalyst surface further reduces the NO conversion rate to 74.1%.H_(2)O(g),SO_(2),and potassium in the flue gas form sulfate and potassium salt on the catalyst surface,blocking the pore structure,thereby decreasing the gas adsorption capacity of the catalyst.Moreover,SO_(2) and potassium engage in competitive adsorption and reaction with NH_(3) and NO at the active sites on the catalyst surface,reducing the content and activity of the catalyst effective component.Increasing the flue gas temperature can promote the decomposition of ammonium sulfate and ammonium bisulfate on the catalyst surface,but it has little effect on potassium.Additionally,potassium will exacerbate sulfur poisoning of the catalyst.Hence,the embedded SCR denitration process requires electrostatic precipitation to eliminate the adverse impacts of potassium and thermal regime optimization to raise flue gas temperature to 350℃,thereby increasing NO conversion rate exceeding 85%.
基金Funded by the National Key Research and Development Program of China(No.2016YFC0209302)。
文摘Zirconium-based metal-organic framework UiO-66 was successfully prepared by solvothermal method,and UiO-66 was modified by adding regulators such as formic acid,acetic acid,and hydrochloric acid.The NH_(3)-SCR reactivity of the samples was evaluated by the denitration activity evaluation system,and the UiO-66 and the regulator-modified UiO-66 were characterized by XRD,SEM,BET,FTIR,TG,NH_(3)-TPD,etc.,the effects of regulator types on the structure and properties of UiO-66 were investigated.The experimental results show that,after adding the modifier,the morphology of UiO-66 changes from irregular quadrilateral with serious agglomeration to particles with regular crystal shape and good dispersibility,and the crystal morphology of the catalyst is improved.In addition,after adding the modifier,UiO-66 has a larger specific surface area and stronger surface acidity,which optimizes the catalytic performance of UiO-66.The catalytic performance test results of NH_(3)-SCR show that the low-temperature activity of UiO-66 is poor,and it only shows a certain catalytic activity at higher temperatures.The catalytic activity of UiO-66 was significantly improved after adding the regulator.Among them,the UiO-66-HCl modified with hydrochloric acid had the best catalytic activity,and the denitration rate reached 70%when the denitration temperature was 380℃.
文摘In this paper, an integrated desulfurization and denitrification technology is proposed for ultra-low emissions of SO2 and NOx in the steel, power and cement industries. A cost-effective and operationally efficient control strategy is realized through a forced oxidation-absorption-reduction process, which reduces equipment investment and operating costs. The technology was adapted to continuous and intermittent denitrification in different temperature zones, promoting the recycling of desulfurization and denitrification products. The study also explored the use of a highly active absorbent obtained by the hydration reaction of coal ash and lime from a power company for the desulfurization and denitrification of sintered flue gases in iron and steel mills, which produces by-products that can be used as retarding agents in the cement industry, resulting in a circular economy. The article emphasizes the importance of improving the lime digestion process and developing new denitrification agents for environmentally safe and cost-effective flue gas treatment.
基金The National Natural Science Foundation of China(No.51376046,51076030)the National Key Technology R&D Program of China during the 12th Five-Year Plan Period(No.2012BAA02B01)+2 种基金the United Creative Foundation of Jiangsu Province(No.BY2013073-10)the Fundamental Research Funds for the Central Universitiesthe Scientific Innovation Research of College Graduates in Jiangsu Province(CXZZ13_0093,KYLX_0115,KYLX_0184)
文摘In order to remove gas-phase mercury and NOx from flue gas, experimental studies on flue gas mercury oxidation removal and denitration of Guizhou anthracite combustion with NH4Br addition were carried out. The influence of NH4Br addition on the ignition temperature and combustion characteristics was studied using a thermogravimetric analyzer. The effects of the NHaBr addition amount on gas-phase mercury oxidation and removal were investigated in a bench scale of 6 kW fluidized bed combustor （FBC）. Mercury concentrations in flue gas were determined by the Ontario hydro method （OHM） and the mercury mass balance was obtained. Results show that the NH4Br addition has little influence on the ignition temperature of Guizhou anthracite. With the mercury mass balance of 95.47%, the proportion of particulate mercury Hg^p, gaseous mercury Hg^0 and Hg^2＋ are 75.28%, 11.60% and 13. 12%, respectively, as raw coal combustion. The high particulate mercury Hg^p in flue gas is caused by the high unburned carbon content in fly ash. When the NH4Br addition amount increases from 0 to 0. 3%, the concentration of gaseous Hg^0 and Hg^2＋ in flue gas decreases continuously, leading to the Hg^p increase accordingly. The oxidation rate of Hg^0 is positively correlated to the Br addition amount. It demonstrates that coal combustion with NH4Br addition can promote Hg^0 oxidation and removal. NOx concentration in flue gas exhibits a descending trend with the NHaBr addition and the removal rate reaches 17.31% with the addition amount of 0.3%. Adding NH4Br to coal also plays a synergistic role in denitration.
文摘Gradiently denitrated gun propellant(GDGP)prepared by a“gradient denitration”strategy is obviously superior in progressive burning performance to the traditional deterred gun propellant.Currently,the preparation of GDGP employed a tedious two-step method involving organic solvents,which hinders the large-scale preparation of GDGP.In this paper,GDGP was successfully prepared via a novelty and environmentally friendly one-step method.The obtained samples were characterized by FT-IR,Raman,SEM and XPS.The results showed that the content of nitrate groups gradiently increased from the surface to the core in the surface layer of GDGP and the surface layer of GDGP exhibited a higher compaction than that of raw gun propellant,with a well-preserved nitrocellulose structure.The denitration process enabled the propellant surface with regressive energy density and good progressive burning performance,as confirmed by oxygen bomb and closed bomb test.At the same time,the effects of different solvents on the component loss of propellant were compared.The result showed that water caused the least component loss.Finally,the stability of GDGP was confirmed by methyl-violet test.This work not only provided environmentally friendly,simple and economic preparation of GDGP,but also confirmed the stability of GDGP prepared by this method.
文摘Sm and Ho were doped in Ce-Mn/TiO_(2)catalyst respectively to enhance its denitration performance at low temperature.X-ray diffraction(XRD),N2adsorption-desorption,X-ray photoelectron spectroscopy(XPS),NH3-temperature programmed desorption(NH3-TPD),H2-temperature programmed reduction(H2-TPR)and in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)techniques were used to analyze the structure and performance of catalysts.The results demonstrate that Ho doping increases the amount of acid sites and improves low temperature redox property of Ce-Mn/TiO_(2),which lead to excellent DeNOxperformance of Ho-Ce-Mn/TiO_(2)in the whole reaction temperature range.Sm doping results in decline of redox property,but it is beneficial to increasing the acid sites of Ce-Mn/TiO_(2).The increased surface acid sites and moderate oxidative ability impart Sm-Ce-Mn/TiO_(2)higher denitration activity and N2selectivity at temperature above 150℃.Lewis acid sites and redox property are the main factors affecting the activity of catalysts.Doping of Ho and Sm both improves sulfur resistance performance of Ce-Mn/TiO_(2)by inhibiting the adsorption of SO_(2)and formation of sulfate.Ce-Mn/TiO_(2)modified by Ho shows better sulfur resistance than that doped with Sm because of its more surface acid sites.
基金the National Natural Science Foundation of China(Grant No.51804277)supported by the State Key Laboratory of Special Rare Metal Materials(No.SKL2020K004)+1 种基金Northwest Rare Metal Materials Research Institutesupported by the State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization(No.CNMRCUKF2008)。
文摘Spent catalyst used for denitration by selective catalytic reduction(spent SCR denitration catalysts) is one of the important urban mines due to the high content of TiO_(2)(~85 wt%) and the massive accumulation amount(over 100,000 tons),therefore,value-added reutilization of titanium in spent SCR catalysts is considerably meaningful.In this paper,a novel method is proposed for converting the titanium oxide in spent SCR denitration catalysts to metallic titanium.Specifically,titanium dioxide(TiO_(2)) was firstly obtained from spent SCR denitration catalysts after removing the impurities by hydrometallurgy process.Then,TiO_(2) is converted to Ti_(2)CO by carbothermic reduction method,and Ti_(2)CO was further purified by oleic acid capture.Finally,by utilizing the as-prepared Ti_(2)CO as the consumable anode in the NaCl-KCl molten salt,high-purity metallic titanium was deposited at cathode,all confirming the feasibility for the conversion of low-grade TiO_(2) in the spent catalysts,from 60 wt% to high-purity metallic Ti(99.5 wt%), furthermore,the energy consumption of this process is 3950 kWh tonne-1 Ti,which is lower than that of most traditional titanium metallurgy methods.The method herein can provide new insights for the value-added recycling of titanium resources in urban mines.
基金Project supported by the National Natural Science Foundation of China(21876168)the Key Projects for Common Key Technology Innovation in Key Industries in Chongqing(cstc2016zdcy-ztzx0020-01)+1 种基金Youth Innovation Promotion Association CAS(2019376)the Graduate Innovation Project of Chongqing Technology and Business University(yjscxx201803-028-22)。
文摘The purpose of this work is to explore the effects of the introduction methods of Ce^4+and Zr^4+on the physicochemical properties,activity,and K tolerance of V2 O5-WO3/TiO2 catalyst for the selective catalytic reduction of NOx by NH3.Four different methods,namely pre-impregnation,post-impregnation,coimpregnation,and co-precipitation,were used to synthesize a series of V2 O5-WO3-TiO2-CeO2-ZrO2 catalysts.The catalysts were characterized by XRD,BET,NH3-TPD,XPS,and H2-TPR techniques.Moreover,the activity and anti-K poisoning performance were tested by an NH3-SCR model reaction.The results show that the introduction of Ce^4+and Zr^4+can improve the catalytic performance of V2O5-WO3/TiO2 catalyst,but the impregnation method cannot enhance the anti-K poisoning performance.Ce^4+and Zr^4+introduced by co-precipitation method can effectively improve the tolerance of K,which is mainly due to the incorporation of Ce^4+and Zr^4+into TiO2 lattice to form a uniform TiO2-CeO2-ZrO2 solid solution,resulting in the optimal surface acidity and redox performance,and reducing the decreases caused by Kpoisoning.Furthermore,based on the best introduction method,we further optimized the molar ratio of Ce^4+/Zr^4+,It is found that the catalyst exhibits the best anti-K poisoning performance when the molar ratio of Ce^4+/Zr^4+is 2:1.
基金supported by the Natural Science Foundation of China (Nos. 21376261, 21173270)the Beijing Natural Science Foundation (2142027)+1 种基金Doctor select Foundation (No. 20130007110007)the National Hi-Tech Research and Development Program (863) of China (No. 2013AA065302)
文摘Selective catalytic reduction technology using NH3 as a reducing agent（NH3-SCR） is an effective control method to remove nitrogen oxides. TiO2-supported vanadium oxide catalysts with different levels of Ce and Sb modification were prepared by an impregnation method and were characterized by X-ray diffractometer（XRD）, Brunauer-Emmett-Teller（BET）, Transmission electron microscopy（TEM）, Fourier transform infrared spectroscopy（FT-IR）, UV-Vis diffuse reflectance spectroscopy（UV-Vis DRS）, Raman and Hydrogen temperature-programmed reduction（H2-TPR）. The catalytic activities of V5 CexS by/TiO2 catalysts for denitration were investigated in a fixed bed flow microreactor. The results showed that cerium, vanadium and antimony oxide as the active components were well dispersed on TiO2, and the catalysts exhibited a large number of d-d electronic transitions, which were helpful to strengthen SCR reactivity. The V5 CexS by/TiO2 catalysts exhibited a good low temperature NH3-SCR catalytic activity. In the temperature range of 210 to 400℃, the V5 CexS by/TiO2 catalysts gave NO conversion rates above 90%. For the best V5Ce35Sb2/TiO2 catalyst, at a reaction temperature of 210℃, the NO conversion rate had already reached 90%. The catalysts had different catalytic activity with different Ce loadings. With the increase of Ce loading, the NO conversion rate also increased.
基金Supported by the National High Technology Research and Develop-ment Program of China(863 Program)(2013AA065403)Major Sci-ence and Technology Project of Fujian Province,China(2011HZ0005-1)+1 种基金International Science and Technology CooperationProgram(2010DFB93990)Natural Science Foundation of FujianProvince,China(2014J06020)
文摘With the advantages of high combustion efficiency, wide fuel flexibility and low concentrations of discharged pollutants, circulating fluid- ized bed （CFB） boiler has been widely used in recent years. However, in order to meet the requirement of new emission standard, it＇s necessary to add flue gas desulfurization and denitration devices. In this paper, the choice of flue gas purification processes for CFB boiler has been discussed firstly, and then the economy and rationality of the SNCR ＋ CFB-FGD ＋ COA comprehensive solution to flue gas desulfurization and denitration have been analyzed.
基金Funded by the Key Projects in the Technology Pillar Program during the Twelfth Five-Year Plan Period(No.2011BAB05B05)
文摘A series of V2O5 with various morphologies was prepared by the hydrothermal method and loaded on the modified active coke（AC） which was prepared by the impregnation methods. The prepared samples were characterized by BET, Boehm titration test, XRD, SEM and EDS. The SEM exhibited that the morphologies of the samples prepared were signifi cantly different from each other. Then the samples prepared were studied on the selective catalytic reduction（SCR） of NO with ammonia in the presence of oxygen. The SCR activity measurements were undertaken in a fixed-bed unit with a sieve plate in the middle. From the contrastive experiments, the results showed that linear V2O5/AC had the best denitration performance and the denitration rate was up to 57.41%. It was speculated that the linear V2O5 with the crystal faces（110） may show the best performance in SCR. And the durability results also showed that linear V2O5/AC produced a denitration rate of 47.7% after three regenerations.
文摘With the continuous increase of new energy installed capacity in recent years, thermal power units are facing deep peak regulation and frequent start-up and shut down for a long time. SCR denitration is widely used in power plants in our country. The recommended minimum temperature for continuous operation of the catalyst is 320℃, and the minimum temperature for short-term operation is 300 ~ 310℃. However, in low-load operation, especially in winter, the flue gas temperature can hardly reach the above minimum temperature for short-term operation. In order to protect the catalyst, the denitration system is generally withdrawn from operation. In order to meet the requirements of environmental protection emissions and avoid imposing penalties on environmental protection electricity prices, power plants urgently need to achieve full-load denitrification. Based on the research on the lowest continuous ammonia injection temperature MOT of denitration catalyst, Yangluo Power Plant realized full-load denitration under the condition of zero transformation through operation adjustment. In addition, the 300MW subcritical natural circulation furnace and 600MW supercritical once-through furnace in Yangluo Power Plant have been verified, which reflects the wide applicability of this technology.
基金financially supported by National Natural Science Foundation of China(No.52264043).
文摘To explore the denitration mechanism of iron-vanadium/activated carbon(Fe-V/AC)catalysts in ammonia-selective catalytic reduction(NH_(3)-SCR),the physicochemical properties of Fe-V/AC catalysts were characterized.The denitration activities of the Fe-V/AC catalysts in the range of 150-300℃ were evaluated.The increase in denitration temperature leads to the highest and fastest recovery rate of NO conversion in the 10Fe-15V/AC catalyst.However,more metal oxides were attached to the catalyst surface as the V loading increased,and the accumulation occurred.The surface-active components are FeO,Fe_(2)O_(3),Fe_(3)O_(4),VO_(2),and V_(2)O_(5).In addition,the increase in the V loading induced a series of modification effects.A large amount of Fe^(3+)was reduced to Fe^(2+),and a large amount of V^(4+)was oxidized to V^(5+).The surface oxygen species(O_(α))were transformed into lattice oxygen(O_(β)).The presence of a large amount of V species deteriorated the pore-structure parameters and destroyed the oxygen-containing functional groups.Increasing the V loading can effectively increase the Lewis acid sites,thereby promoting NH_(3) adsorption and NO reduction and increasing the stretching vibration of weakly adsorbed ammonia species on the catalyst.The NH_(3) adsorption process produces a notable increase in the concentration of monodentate nitrite(NH_(4)^(+)).The NH_(3)-SCR denitration mechanism of the Fe-V/AC catalyst includes reaction gas adsorption,catalytic denitration of metal active components,and gas desorption.
基金support from the National Natural Science Foundation of China(grant nos.22021002,22020102005,and 22022705)the CAS-Croucher Funding Scheme for Joint Laboratories.
文摘The direct cleavage of C–NO_(2)bonds for reductive denitration of nitroarenes remains a challenging transformation in synthetic organic chemistry.Herein,we report a biocompatible palladium-deposited graphdiyne nanocatalyst(Pd@GDY/DSPE-PEG)that can catalyze reductive denitration of nitroarenes under ambient physiological conditions.Mechanistic studies support this transformation via the oxidative addition of nitroarenes with Pd(0)and subsequent ligand exchange to form arylpalladium hydride.This one-step reductive denitration via Pd@GDY/DSPE-PEG successfully facilitates the repair of the nitrated proteins arising from endogenic ONOO−and restores their physiological function,including blocking the apoptosis pathway in living cells.Moreover,Pd@GDY/DSPE-PEG was further successfully applied for catalytic denitration to reduce the level of 3-nitrotyrosine residues of proteins located in the mouse brain hippocampus in vivo.This study provides an ideal strategy for designing highly active enzymatic mimicking synthetic catalysts for the regulation of the nitrated protein level and the detoxification of nitrative damage of living cells and tissues.
基金supported by the National Natural Science Foundation of China(No.92367107)。
文摘Ultra-low emission of nitrogen oxide(NO_(x))is an irreversible trend for the development of waste-to-energy industry.But traditional approaches to remove NO_(x) face significant challenge s,such as low denitration efficiency,complex denitration system,and high investment and operating cost.Here we put forward a novel polymer non-catalytic reduction(PNCR)technology that utilized a new type of polymer agent to remove NO_(x),and the proposed PNCR technology was applied to the existing waste-to-energy plant to test the denitration performance.The PNCR technology demonstrated excellent denitration performance with a NO_(x) emission concentration of<100 mg/Nm^(3) and high denitration efficiency of>75%at the temperature range of 800-900℃,which showed the application feasibility even on the complex and unstable industrial operating conditions.In addition,PNCR and hybrid polymer/selective non-catalytic reduction(PNCR/SNCR)technology possessed remarkable economic advantages including low investment fee and low operating cost of<10 CNY per ton of municipal solid waste(MSW)compared with selective catalytic reduction(SCR)technology.The excellent denitration performance of PNCR technology forebodes a broad industrial application prospect in the field of flue gas cleaning for waste-to-energy plants.
文摘Nitrogen oxides(NO_(x))present in flue gas are economically renewable N1 resources.Unlike traditional selective catalytic reduction processes that convert NO into N_(2),redirecting NO towards the synthesis of value-added NH_(3)offers significant practical benefits.In this study,a Ti-based metal-organic framework(Ti-MOF),specifically MIL-125,was utilized as a support for Fe,which was subsequently calcined at 400℃to produce a Fe_(2)O_(3)/TiO_(2)-MOF catalyst.The resulting catalyst demonstrated exceptional performance,achieving 99%NO conversion and 95%NH_(3)selectivity under optimal conditions of 450℃,0.1 MPa,and a gas hourly space velocity of 38000 mL g^(–1)h^(−1).Additionally,the catalyst exhibited excellent stability and resistance to water and sulfur.The high efficiency of Fe_(2)O_(3)/TiO_(2)-MOF is attributed to the abundance of Fe^(2+)sites at the reaction temperature,which enhances NO adsorption and activation.Furthermore,density functional theory calculations suggest that NO undergoes hydrogenation at the N-terminus on the Fe_(2)O_(3)/TiO_(2)-MOF surface,leading directly to NH_(3)synthesis rather than dissociation followed by hydrogenation.This catalyst presents a novel approach for converting NO_(x)into high-value chemical products.
基金supported by National Natural Science Foundation of China(U20A20130)Fundamental Research Funds for the Central Universities(FRF-EYIT-23-07).
文摘Ammonia selective catalytic reduction(NH_(3)-SCR)is the most widely used technology in thefield of industrialflue gas denitrification.However,the presence of heavy metals influe gas can seriously affect the performance of SCR catalysts,leading to their deactivation or even failure.Therefore,it is of great significance to deeply study the poisoning mechanism of SCR catalysts under the action of heavy metals and how to enhance their resistance to poisoning.This article reviews the reaction mechanism of NH_(3)-SCR technology,compares the impact of heavy metals on the activity of different SCR catalysts,and then discusses in detail the poisoning mechanism of SCR catalysts by heavy metals,including pore blockage,reduction of specific surface area,and destruction of active centers caused by heavy metal deposition,all of which jointly lead to the physical or chemical poisoning of the catalyst.Meanwhile,the mechanism of action when multiple toxicants coexist was analyzed.To effectively address these challenges,the article further summarizes various methods to improve the catalyst's resistance to heavy metal poisoning,such as element doping,structural optimization,and carrier addition,which significantly enhance the heavy metal resistance of the catalyst.Finally,the article provides a prospective analysis of the challenges faced by NH_(3)-SCR catalysts in anti-heavy metal poisoning technology,emphasizing the necessity of in-depth research on the poisoning mechanism,exploration of the mechanism of synergistic action of multiple pollutants,development of comprehensive anti-poisoning strategies,and research on catalyst regeneration technology,in order to promote the development of efficient anti-heavy metal poisoning NH_(3)-SCR catalysts.
文摘Performance of simultaneous desulfurization and denitration using the solution of NaClO2 and NaClO as new-style complex absorbent was investigated experimentally in self-designed bench scale bubbling reactor. The effects of main parameters, such as the concentrations of NaClO2 and of NaClO, solution pH and reaction temperature and so on, on removal efficiencies of SO2 and NOx, were examined, then the optimal conditions were established, in which the molar ratio of NaClO to NaClO2 was 1：1, the reaction temperature was 50℃ and the solution pH was 5.5. The removal efficiencies of SO2 and NO under the optimal conditions were 100% and 89.2%, respectively. The mechanism of simultaneous removal based on complex absorbent was proposed by analyzing the removal products and the electrode potentials of related species, namely SO2 and NO are oxi- dized by chlorite anion, hypochlorite, chlorine dioxide and chlorine contained in complex absorbent. In thermodynamic aspect, simultaneous desulfurization and denitration reactions in liquid phase can happen spontaneously and completely, and are all exothermic reactions. It was confirmed by kinetics that for simultaneous desulfurization and denitration, the reaction order and average activation energy of SO2 were 1 and 21.6 kJ·mol^-1, respectively, and those of NO were 1 and 8.2 kJ·mol^-1, respectively.
基金the National Key Research and Development Project(No.2023YFF1205103)the National Natural Science Foundation of China(No.22371007)the Peking University Medicine plus X Pilot Program-Key Technologies R&D Project(No.2024YXXLHGG001)for financial support。
文摘We herein present an efficient denitrative iodination method of(hetero)nitroarenes mediated by commercially available and cost-effective hydroiodic acid(HI).During the reaction process,HI plays its dual roles as both the sustainable reductant of nitro group and iodine source in the iodination step,which successfully integrates three steps into a one-pot procedure and significantly simplifies the reaction system.This approach enables a smooth metal-free conversion of nitroarenes to corresponding aryl iodides via one-pot process,exhibits a broad substrate scope and good reaction efficiency,and was conveniently applied in the concise synthesis of pharmaceuticals.
