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
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
Based on the basic principle and mechanism of flue gas denitrification,the commonly used catalysts for flue gas denitrification were introduced firstly,and then the catalytic performance,stability and reaction mechani...Based on the basic principle and mechanism of flue gas denitrification,the commonly used catalysts for flue gas denitrification were introduced firstly,and then the catalytic performance,stability and reaction mechanism of catalysts in the market were analyzed.Different types of catalysts were studied to look for green catalysts with high activity,sulfur resistance,water vapor resistance and other advantages.The mechanism of denitration reaction of green catalysts was discussed,and the laws of formation,propagation and consumption of active species in the reaction process were revealed to provide theoretical basis for optimizing catalyst design and improving reaction conditions.Then the research status and problems of new catalysts for flue gas denitrification were described.Finally,the future development direction of green catalysts for flue gas denitration was discussed to improve the performance and stability of catalysts and meet the performance requirements of denitration catalysts in different industries.展开更多
With the vigorous development of China’s iron and steel industry and the introduction of ultra-low emission policies, the emission of pollutants such as SO2 and NOx has received unprecedented attention. At present, t...With the vigorous development of China’s iron and steel industry and the introduction of ultra-low emission policies, the emission of pollutants such as SO2 and NOx has received unprecedented attention. At present, the commonly used denitrification methods include selective catalytic reduction (SCR), active coke, etc. As a newly developed denitrification technology, oxidation denitrification is not widely used, and the technical level is mixed, and there might be problems such as yellow smoke, secondary pollution and ozone escape in the practical application. In this paper, problems existing in the denitrification process of sintering flue gas oxidation are analyzed, and a 320 m2 sintering machine is taken as an example. Comparing the denitrification technology of sintering industry, it could be seen that the denitrification technology route of oxidation method has low pollution, low cost and high comprehensive environmental benefits, and has greatly potential development.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
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
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 relationship is established, using the least squares method, between the standard enthalpy of formation and the standard enthalpy of formation divided by the exothermic denitration decomposition peak absolute temper...A relationship is established, using the least squares method, between the standard enthalpy of formation and the standard enthalpy of formation divided by the exothermic denitration decomposition peak absolute temperature corresponding to β →0.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
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.
基金Supported by the Interdisciplinary Team Project of Shenyang University of Technology in 2021:Green and Low-carbon(Technology and Evaluation)of Typical Industries of Carbon Peak(2021-70-06)"Double First-class"Construction Project of Liaoning Province in 2020(Scientific Research)(FWDFGD2020041).
文摘Based on the basic principle and mechanism of flue gas denitrification,the commonly used catalysts for flue gas denitrification were introduced firstly,and then the catalytic performance,stability and reaction mechanism of catalysts in the market were analyzed.Different types of catalysts were studied to look for green catalysts with high activity,sulfur resistance,water vapor resistance and other advantages.The mechanism of denitration reaction of green catalysts was discussed,and the laws of formation,propagation and consumption of active species in the reaction process were revealed to provide theoretical basis for optimizing catalyst design and improving reaction conditions.Then the research status and problems of new catalysts for flue gas denitrification were described.Finally,the future development direction of green catalysts for flue gas denitration was discussed to improve the performance and stability of catalysts and meet the performance requirements of denitration catalysts in different industries.
文摘With the vigorous development of China’s iron and steel industry and the introduction of ultra-low emission policies, the emission of pollutants such as SO2 and NOx has received unprecedented attention. At present, the commonly used denitrification methods include selective catalytic reduction (SCR), active coke, etc. As a newly developed denitrification technology, oxidation denitrification is not widely used, and the technical level is mixed, and there might be problems such as yellow smoke, secondary pollution and ozone escape in the practical application. In this paper, problems existing in the denitrification process of sintering flue gas oxidation are analyzed, and a 320 m2 sintering machine is taken as an example. Comparing the denitrification technology of sintering industry, it could be seen that the denitrification technology route of oxidation method has low pollution, low cost and high comprehensive environmental benefits, and has greatly potential development.
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.
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.
文摘A relationship is established, using the least squares method, between the standard enthalpy of formation and the standard enthalpy of formation divided by the exothermic denitration decomposition peak absolute temperature corresponding to β →0.
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.
