针对当前钠离子电池钠储存反应动力学慢、倍率性能较低等关键问题开展结构设计,利用同轴静电纺将氧化锡(SnO_(x))纳米颗粒嵌入碳纳米纤维中得到碳包覆非晶相氧化锡SnO_(x)纳米纤维(SnO_(x)@C)。随后通过等离子体氟化处理SnO_(x)@C得到具...针对当前钠离子电池钠储存反应动力学慢、倍率性能较低等关键问题开展结构设计,利用同轴静电纺将氧化锡(SnO_(x))纳米颗粒嵌入碳纳米纤维中得到碳包覆非晶相氧化锡SnO_(x)纳米纤维(SnO_(x)@C)。随后通过等离子体氟化处理SnO_(x)@C得到具有C-F半离子键的SnO_(x)@C的纳米纤维(PF-SnO_(x)@C)。研究讨论纳米纤维PF-SnO_(x)@C的结构形貌演化规律及其电化学性能,PF-SnO_(x)@C电极在大电流密度5 A g^(-1)下循环5000可逆容量仍保持在100 mAh g^(-1),显示出超稳定的长循环性能和良好的倍率性能。展开更多
Formaldehyde is a common atmospheric pollutant produced in industrial production and daily life.However,the traditional semiconductor formaldehyde gas sensor cannot work at room temperature,which limits its practical ...Formaldehyde is a common atmospheric pollutant produced in industrial production and daily life.However,the traditional semiconductor formaldehyde gas sensor cannot work at room temperature,which limits its practical application.Therefore,developing high-performance gas sensors for rapidly and accurately detecting formaldehyde at room temperature is an important topic.In this study,Ti_(3)C_(2)Tx/SnO_(2)heterostructures were constructed,which could selectively detect formaldehyde at room temperature with a response value of 29.16%(10×10^(-6)).In addition,the sensor shows a remarkable theoretical detection limit of 5.09×10^(-9)and good longterm stability.Density functional theory(DFT)simulations reveal that SnO_(2)nano spheres provide the majority of adsorption sites that strongly interact with formaldehyde.Meanwhile,Ti_(3)C_(2)T_(x)acting as a conductive layer facilitates the transfer of charge carriers so that they show a sensing response to formaldehyde at room temperature.Moreover,the formation of p-n heterostructures between SnO_(2)and Ti_(3)C_(2)T_(x)boosts the Schottky barrier at the interface,which is the critical factor in enhancing the sensing properties by turning the Schottky barrier upon introducing formaldehyde gas.This perspective is expected to provide instructive guidance for utilizing MXene/metal oxide nanocomposites to improve the gas sensing performance at room temperature.展开更多
The selective catalytic reduction(SCR) of NO_(x) with NH_(3)(NH_(3)-SCR) technology has been widely applied for reducing NO_(x) emissions from stationary and mobile sources.In this work,the extruded monolith MnO_(x)-C...The selective catalytic reduction(SCR) of NO_(x) with NH_(3)(NH_(3)-SCR) technology has been widely applied for reducing NO_(x) emissions from stationary and mobile sources.In this work,the extruded monolith MnO_(x)-CeO_(2)-TiO_(2) catalyst was installed in a cement kiln for NH_(3)-SCR of NO_(x),where the flue gas temperature was 110-140℃.It is found that the monolith catalyst is severely deactivated after operating for about 200 h with almost no NO_(x) conversion at 160℃ under GHSV of 50000 h^(-1),while the fresh monolith catalyst remains 60% NO_(x) conversion.Scanning electron microscopy-energy dispersive spectroscopy(SEM-EDS),X-ray photoelectron spectroscopy(XPS),temperature-programmed desorption of SO_(2)(SO_(2)-TPD) and thermogravimetric-differential thermal analysis(TG-DTG) experiments reveal that both MnO_(x) and CeO_(2) oxides in monolith are severely sulfated to manganese sulfate and cerium sulfate,and the external monolith walls are covered by massive ceria sulfate and little ammonium nitrate.In situ diffuse reflectance infrared Fourier trans form spectroscopy(DRIFTS) analysis demonstrates that the formation of nitrates at low temperatures is inhibited due to the occupation of active sites in MnO_(x)-CeO_(2)-TiO_(2) by sulfates,resulting in the decrease of low temperature activity.After washing with water,the activity of deactivated monolith catalyst can be partially recovered,together with significant loss of manganese and cerium from monolith.展开更多
In this work,SnO_(x)/activated carbon(AC)was synthesized by hydrothermal method,which was applied to acetylene hydrochlorination.Characterizations showed the SnO_(x)nanoparticles were uniformly dispersed on the carbon...In this work,SnO_(x)/activated carbon(AC)was synthesized by hydrothermal method,which was applied to acetylene hydrochlorination.Characterizations showed the SnO_(x)nanoparticles were uniformly dispersed on the carbon,with the coexistence of SnO and SnO_(2).The acetylene conversion of SnO_(x)/AC was 75%,much higher than that of SnCl_(4)/AC.It was shown that the adsorption of reactants on SnO_(x)was stronger than on SnCl_(4).Theoretical calculations showed the adsorption energies of reactants on SnO_(x)were thermodynamically favorable and suggested that Sn^(4+)and Sn^(2+)in SnO_(x)have different adsorption capacities for reactants.Through adjusting the valence ratio of SnO_(x),SnO_(x)/AC O 4 h(O for oxidation)exhibited the best catalytic performance and had the strongest adsorption capacity for the reactants.However,the SnO_(x)/AC catalyst was easily deactivated during acetylene hydrochlorination due to the loss of Sn.The doping of N effectively reduced the loss of Sn and improved the stability of the catalyst due to the anchoring effect of N on the SnO_(x)particles.展开更多
Fascinating with high specific capacity and moderate lithiation potential,SnO_(x)-based materials have been intensively investigated as one of the most promising anodes for lithium-ion batteries.However,due to poor cy...Fascinating with high specific capacity and moderate lithiation potential,SnO_(x)-based materials have been intensively investigated as one of the most promising anodes for lithium-ion batteries.However,due to poor cycling stability,sluggish reaction kinetics,and limited electrochemical reaction reversibility,the development of SnO_(x)-based anodes has been hindered.And the current preparation and modification routes for SnO_(x)-based anodes lack direct and specific illustration.Herein,modification routes for SnO_(x)-based anodes have been emphasized.Firstly,to provide more direct instructions,the tuning routes of morphological structure for SnO_(x)-based electrodes(including slurry-based and self-supported)have been thoroughly discussed from the preparation perspective.Secondly,according to the properties of SnO_(x)-based anodes,the phase structure design ideas have also been properly classified and organized for addressing chemical reaction kinetics or thermodynamic issues.Finally,for future-oriented studies,new insights into the development and commercialization prospects of SnO_(x)-based anodes are also provided.This review,with comprehensive information on SnO_(x)-based anodes,aims to bring more specific guidance and valuable inspiration for peer researchers who are promoting the application of SnO_(x)-based materials for energy conversion and storage devices.展开更多
High-performance and low-cost gas sensors are highly desirable and involved in industrial production and environmental detection.The combination of highly conductive MXene and metal oxide materials is a promising stra...High-performance and low-cost gas sensors are highly desirable and involved in industrial production and environmental detection.The combination of highly conductive MXene and metal oxide materials is a promising strategy to further improve the sensing performances.In this study,the hollow SnO_(2)nanospheres and few-layer MXene are assembled rationally via facile electrostatic synthesis processes,then the SnO_(2)/Ti_(3)C_(2)T_(x)nanocomposites were obtained.Compared with that based on either pure SnO_(2)nanoparticles or hollow nanospheres of SnO_(2),the SnO_(2)/Ti_(3)C_(2)T_(x)composite-based sensor exhibits much better sensing performances such as higher response(36.979),faster response time(5 s),and much improved selectivity as well as stability(15 days)to 100ppm C2H5OH at low working temperature(200°C).The improved sensing performances are mainly attributed to the large specific surface area and significantly increased oxygen vacancy concentration,which provides a large number of active sites for gas adsorption and surface catalytic reaction.In addition,the heterostructure interfaces between SnO_(2)hollow spheres and MXene layers are beneficial to gas sensing behaviors due to the synergistic effect.展开更多
Hydrothermal stability is crucial for the practical application of deNO_(x)catalyst on diesel vehicles,for the selective catalytic reduction of NO_(x)with NH_(3)(NH_(3)-SCR).SnO_(2)-based materials possess superior hy...Hydrothermal stability is crucial for the practical application of deNO_(x)catalyst on diesel vehicles,for the selective catalytic reduction of NO_(x)with NH_(3)(NH_(3)-SCR).SnO_(2)-based materials possess superior hydrothermal stability,which is attractive for the development of NH_(3)-SCR catalyst.In this work,a series of Ce-Nb/SnO_(2)catalysts,with Ce and Nb loading on SnO_(2)support,were prepared by impregnation method.It was found that,the NH_(3)-SCR activities and hydrothermal stabilities of the Ce-Nb/SnO_(2)catalysts significantly varied with the impregnation sequences,and the Ce-Nb(f)/SnO_(2) catalyst that firstly impregnated Nb and then impregnated Ce exhibited the best performance.The characterization results revealed that CeNb(f)/SnO_(2)possessed appropriate acidity and redox capability.Furthermore,the strong synergistic effect between Nb and Sn species stabilized the structure and maintained the dispersion of acid sites.This study may provide a new understanding for the effect of impregnation sequence on activity and hydrothermal stability and a new environmental-friendly NH_(3)-SCR catalyst with potential applications for NO_(x)removal from diesel and hydrogenfueled engines.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
MnO_(x)-CeO_(2) catalysts are developed by hydrolysis driving redox method using acetate precursor(3 Mn1 Ce-Ac) and nitrate precursor(3 Mn1 Ce-N) for the selective catalytic reduction(SCR) of NO_(x) by NH_(3).A counte...MnO_(x)-CeO_(2) catalysts are developed by hydrolysis driving redox method using acetate precursor(3 Mn1 Ce-Ac) and nitrate precursor(3 Mn1 Ce-N) for the selective catalytic reduction(SCR) of NO_(x) by NH_(3).A counterpart sample(Cop-3 Mn1 Ce) was prepared by the NH_(3)·H_(2) O co-precipitation method for comparison purpose.Combining the results of physicochemical properties characterization and performance test,we find that the 3 Mn1 Ce-Ac catalyst with some nanorod structures is highly active for the deNOx process.The SCR activity of the 3 Mn1 Ce-Ac catalyst is more admirable than the 3 Mn1 Ce-N and the Cop-3 Mn1 Ce catalysts due to plentiful Lewis acid sites,excellent low-temperature reducibility,and superior surface area resulted from O_(2) generation during the pre paration procedure.The 3 Mn1 Ce-Ac still exhibits the greatest performance for the deNO_(x )process when gaseous acetone is in the SCR feed gas.The NOx conversion and N2 selectivity over the 3 Mn1 Ce-Ac are both improved by gaseous acetone above150℃ due to the inhibition of SCR undesired side reactions(NSCR & C-O reactions) and "slow-SCR" process.展开更多
MnO_(x)-CeO_(x)/ACFN were prepared by the impregnation method and used as catalyst for selective catalytic reduction of NO with NH_(3) at 80℃-150℃.The catalyst was characterized by N_(2)-BET,scanning electron micros...MnO_(x)-CeO_(x)/ACFN were prepared by the impregnation method and used as catalyst for selective catalytic reduction of NO with NH_(3) at 80℃-150℃.The catalyst was characterized by N_(2)-BET,scanning electron microscopy(SEM)and Fourier transform infrared spectroscopy(FT-IR).The fraction of the mesopore and the oxygen functional groups on the surface of activated carbon fiber(ACF)increased after the treatment with nitric acid,which was favorable to improve the catalytic activities of MnO_(x)-CeO_(x)/ACFN.The experimental results show that the conversion of NO is nearly 100%in the range 100℃-150℃under the optimal preparation conditions of MnO_(x)-CeO_(x)/ACFN.In addition,the effects of a series of performance parameters,including initial NH3 concentration,NO concentration and O_(2) concentration,on the conversion of NO were studied.展开更多
SnO 2 nanospheres with diameters of 30∼50 nm and Pt x Cu 1-x bimetallic nanoparticles with sizes of approxi-mately 10 nm were synthesized via hydrothermal and solvothermal methods,respectively.The Pt x Cu 1-x bimetal...SnO 2 nanospheres with diameters of 30∼50 nm and Pt x Cu 1-x bimetallic nanoparticles with sizes of approxi-mately 10 nm were synthesized via hydrothermal and solvothermal methods,respectively.The Pt x Cu 1-x bimetal-lic nanoparticles were impregnated on the surface of the SnO 2 spheres to form Pt x Cu 1-x-SnO 2 nanocomposites.By varying the atomic ratios between platinum(Pt)and copper(Cu),we found that Pt 0.75 Cu 0.25-SnO 2,with a large specific surface area of 89.21 m 2/g,enabled the selective and accurate detection of low-concentration formalde-hyde compared to other metal-deposited samples and pure SnO 2.The response value of Pt 0.75 Cu 0.25-SnO 2 to 500×10−9 formaldehyde was approximately 20 at an operating temperature of 160◦C with an extremely high-speed response(15 s).The porous structures with large specific surface areas,as well as the improved catalytic effects of Pt 0.75 Cu 0.25,comprehensively contributed to the enhanced sensing performance towards formaldehyde.展开更多
文摘针对当前钠离子电池钠储存反应动力学慢、倍率性能较低等关键问题开展结构设计,利用同轴静电纺将氧化锡(SnO_(x))纳米颗粒嵌入碳纳米纤维中得到碳包覆非晶相氧化锡SnO_(x)纳米纤维(SnO_(x)@C)。随后通过等离子体氟化处理SnO_(x)@C得到具有C-F半离子键的SnO_(x)@C的纳米纤维(PF-SnO_(x)@C)。研究讨论纳米纤维PF-SnO_(x)@C的结构形貌演化规律及其电化学性能,PF-SnO_(x)@C电极在大电流密度5 A g^(-1)下循环5000可逆容量仍保持在100 mAh g^(-1),显示出超稳定的长循环性能和良好的倍率性能。
基金financially supported by the National Natural Science Foundation of China(No.61973223)the Innovative Talents in Colleges and Universities in Liaoning Province(No.2020389)+3 种基金Liao Ning Revitalization Talents Program(No.XLYC2007051)Liaoning Educational Department Foundation(No.LJKMZ20220762)the Natural Science Foundation of Liaoning Province(No.2021-MS-257)the Young and Middle-aged Scientific and Technological Innovation Talents of Shenyang Science and Technology Bureau(No.RC200352)。
文摘Formaldehyde is a common atmospheric pollutant produced in industrial production and daily life.However,the traditional semiconductor formaldehyde gas sensor cannot work at room temperature,which limits its practical application.Therefore,developing high-performance gas sensors for rapidly and accurately detecting formaldehyde at room temperature is an important topic.In this study,Ti_(3)C_(2)Tx/SnO_(2)heterostructures were constructed,which could selectively detect formaldehyde at room temperature with a response value of 29.16%(10×10^(-6)).In addition,the sensor shows a remarkable theoretical detection limit of 5.09×10^(-9)and good longterm stability.Density functional theory(DFT)simulations reveal that SnO_(2)nano spheres provide the majority of adsorption sites that strongly interact with formaldehyde.Meanwhile,Ti_(3)C_(2)T_(x)acting as a conductive layer facilitates the transfer of charge carriers so that they show a sensing response to formaldehyde at room temperature.Moreover,the formation of p-n heterostructures between SnO_(2)and Ti_(3)C_(2)T_(x)boosts the Schottky barrier at the interface,which is the critical factor in enhancing the sensing properties by turning the Schottky barrier upon introducing formaldehyde gas.This perspective is expected to provide instructive guidance for utilizing MXene/metal oxide nanocomposites to improve the gas sensing performance at room temperature.
基金supported by the National Natural Science Foundation of China (22188102,22072179)Cultivating Project of Strategic Priority Research Program of Chinese Academy of Sciences (XDPB190201)。
文摘The selective catalytic reduction(SCR) of NO_(x) with NH_(3)(NH_(3)-SCR) technology has been widely applied for reducing NO_(x) emissions from stationary and mobile sources.In this work,the extruded monolith MnO_(x)-CeO_(2)-TiO_(2) catalyst was installed in a cement kiln for NH_(3)-SCR of NO_(x),where the flue gas temperature was 110-140℃.It is found that the monolith catalyst is severely deactivated after operating for about 200 h with almost no NO_(x) conversion at 160℃ under GHSV of 50000 h^(-1),while the fresh monolith catalyst remains 60% NO_(x) conversion.Scanning electron microscopy-energy dispersive spectroscopy(SEM-EDS),X-ray photoelectron spectroscopy(XPS),temperature-programmed desorption of SO_(2)(SO_(2)-TPD) and thermogravimetric-differential thermal analysis(TG-DTG) experiments reveal that both MnO_(x) and CeO_(2) oxides in monolith are severely sulfated to manganese sulfate and cerium sulfate,and the external monolith walls are covered by massive ceria sulfate and little ammonium nitrate.In situ diffuse reflectance infrared Fourier trans form spectroscopy(DRIFTS) analysis demonstrates that the formation of nitrates at low temperatures is inhibited due to the occupation of active sites in MnO_(x)-CeO_(2)-TiO_(2) by sulfates,resulting in the decrease of low temperature activity.After washing with water,the activity of deactivated monolith catalyst can be partially recovered,together with significant loss of manganese and cerium from monolith.
基金the Taishan Scholars Program of Shandong Province(No.tsqn202103051)the Science and Technology Project of Xinjiang Bingtuan Supported by Central Government(No.2022BC001)the project of scientific research in Shihezi University(No.CXFZ202205).
文摘In this work,SnO_(x)/activated carbon(AC)was synthesized by hydrothermal method,which was applied to acetylene hydrochlorination.Characterizations showed the SnO_(x)nanoparticles were uniformly dispersed on the carbon,with the coexistence of SnO and SnO_(2).The acetylene conversion of SnO_(x)/AC was 75%,much higher than that of SnCl_(4)/AC.It was shown that the adsorption of reactants on SnO_(x)was stronger than on SnCl_(4).Theoretical calculations showed the adsorption energies of reactants on SnO_(x)were thermodynamically favorable and suggested that Sn^(4+)and Sn^(2+)in SnO_(x)have different adsorption capacities for reactants.Through adjusting the valence ratio of SnO_(x),SnO_(x)/AC O 4 h(O for oxidation)exhibited the best catalytic performance and had the strongest adsorption capacity for the reactants.However,the SnO_(x)/AC catalyst was easily deactivated during acetylene hydrochlorination due to the loss of Sn.The doping of N effectively reduced the loss of Sn and improved the stability of the catalyst due to the anchoring effect of N on the SnO_(x)particles.
基金financially supported by the National Natural Science Foundation of China(Nos.52071144,51831009 and 51621001)Guangzhou key research and development program(No.202103040001)。
文摘Fascinating with high specific capacity and moderate lithiation potential,SnO_(x)-based materials have been intensively investigated as one of the most promising anodes for lithium-ion batteries.However,due to poor cycling stability,sluggish reaction kinetics,and limited electrochemical reaction reversibility,the development of SnO_(x)-based anodes has been hindered.And the current preparation and modification routes for SnO_(x)-based anodes lack direct and specific illustration.Herein,modification routes for SnO_(x)-based anodes have been emphasized.Firstly,to provide more direct instructions,the tuning routes of morphological structure for SnO_(x)-based electrodes(including slurry-based and self-supported)have been thoroughly discussed from the preparation perspective.Secondly,according to the properties of SnO_(x)-based anodes,the phase structure design ideas have also been properly classified and organized for addressing chemical reaction kinetics or thermodynamic issues.Finally,for future-oriented studies,new insights into the development and commercialization prospects of SnO_(x)-based anodes are also provided.This review,with comprehensive information on SnO_(x)-based anodes,aims to bring more specific guidance and valuable inspiration for peer researchers who are promoting the application of SnO_(x)-based materials for energy conversion and storage devices.
基金This work is supported partially by the project of the State Key Laboratory of Alternate Electrical Power System with Renewable Energy Sources(Nos.LAPS21004,LAPS202114)National Natural Science Foundation of China(Nos.52272200,51972110,52102245 and 52072121)+6 种基金Beijing Science and Technology Project(No.Z211100004621010)Beijing Natural Science Foundation(Nos.2222076,2222077)Hebei Natural Science Foundation(No.E2022502022)Huaneng Group Headquarters Science and Technology Project(No.HNKJ20-H88)2022 Strategic Research Key Project of Science and Technology Commission of the Ministry of Education,China Postdoctoral Science Foundation(No.2022M721129)the Fundamental Research Funds for the Central Universities(Nos.2022MS030,2021MS028,2020MS023,2020MS028)the NCEPU“Double First-Class”Program.This research was also supported by Brain Pool program funded by the Ministry of Science and ICT through the National Research Foundation of Korea(No.2021H1D3A2A01100019).
文摘High-performance and low-cost gas sensors are highly desirable and involved in industrial production and environmental detection.The combination of highly conductive MXene and metal oxide materials is a promising strategy to further improve the sensing performances.In this study,the hollow SnO_(2)nanospheres and few-layer MXene are assembled rationally via facile electrostatic synthesis processes,then the SnO_(2)/Ti_(3)C_(2)T_(x)nanocomposites were obtained.Compared with that based on either pure SnO_(2)nanoparticles or hollow nanospheres of SnO_(2),the SnO_(2)/Ti_(3)C_(2)T_(x)composite-based sensor exhibits much better sensing performances such as higher response(36.979),faster response time(5 s),and much improved selectivity as well as stability(15 days)to 100ppm C2H5OH at low working temperature(200°C).The improved sensing performances are mainly attributed to the large specific surface area and significantly increased oxygen vacancy concentration,which provides a large number of active sites for gas adsorption and surface catalytic reaction.In addition,the heterostructure interfaces between SnO_(2)hollow spheres and MXene layers are beneficial to gas sensing behaviors due to the synergistic effect.
基金supported by the National Natural Science Foundation of China(Nos.52225004 and 22276182)the National Key R&D Program of China(Nos.2022YFC3701804 and 2022YFC3704400)the Science and Technology Innovation“2025”major program in Ningbo(No.2020Z103)。
文摘Hydrothermal stability is crucial for the practical application of deNO_(x)catalyst on diesel vehicles,for the selective catalytic reduction of NO_(x)with NH_(3)(NH_(3)-SCR).SnO_(2)-based materials possess superior hydrothermal stability,which is attractive for the development of NH_(3)-SCR catalyst.In this work,a series of Ce-Nb/SnO_(2)catalysts,with Ce and Nb loading on SnO_(2)support,were prepared by impregnation method.It was found that,the NH_(3)-SCR activities and hydrothermal stabilities of the Ce-Nb/SnO_(2)catalysts significantly varied with the impregnation sequences,and the Ce-Nb(f)/SnO_(2) catalyst that firstly impregnated Nb and then impregnated Ce exhibited the best performance.The characterization results revealed that CeNb(f)/SnO_(2)possessed appropriate acidity and redox capability.Furthermore,the strong synergistic effect between Nb and Sn species stabilized the structure and maintained the dispersion of acid sites.This study may provide a new understanding for the effect of impregnation sequence on activity and hydrothermal stability and a new environmental-friendly NH_(3)-SCR catalyst with potential applications for NO_(x)removal from diesel and hydrogenfueled engines.
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 Key Laboratory of Water and Air Pollution Control of Guangdong province,China (No.2017A030314001)the National Key Research and Development Plan (No.2019YFC0214303)+1 种基金Central Public-Interest Scientific Institution Basal Research Fund (No.PM-zx703-202002-015)the National Natural Science Foundation of China (No.22076224)。
文摘MnO_(x)-CeO_(2) catalysts are developed by hydrolysis driving redox method using acetate precursor(3 Mn1 Ce-Ac) and nitrate precursor(3 Mn1 Ce-N) for the selective catalytic reduction(SCR) of NO_(x) by NH_(3).A counterpart sample(Cop-3 Mn1 Ce) was prepared by the NH_(3)·H_(2) O co-precipitation method for comparison purpose.Combining the results of physicochemical properties characterization and performance test,we find that the 3 Mn1 Ce-Ac catalyst with some nanorod structures is highly active for the deNOx process.The SCR activity of the 3 Mn1 Ce-Ac catalyst is more admirable than the 3 Mn1 Ce-N and the Cop-3 Mn1 Ce catalysts due to plentiful Lewis acid sites,excellent low-temperature reducibility,and superior surface area resulted from O_(2) generation during the pre paration procedure.The 3 Mn1 Ce-Ac still exhibits the greatest performance for the deNO_(x )process when gaseous acetone is in the SCR feed gas.The NOx conversion and N2 selectivity over the 3 Mn1 Ce-Ac are both improved by gaseous acetone above150℃ due to the inhibition of SCR undesired side reactions(NSCR & C-O reactions) and "slow-SCR" process.
基金supported by the National Natural Science Foundation of China(Grant No.90610018)Tianjin Provincial Natural Science Foundation(Grant No.06YFJMJC-06200)“100 projects”of Creative Research for the Undergraduates of Nankai University.
文摘MnO_(x)-CeO_(x)/ACFN were prepared by the impregnation method and used as catalyst for selective catalytic reduction of NO with NH_(3) at 80℃-150℃.The catalyst was characterized by N_(2)-BET,scanning electron microscopy(SEM)and Fourier transform infrared spectroscopy(FT-IR).The fraction of the mesopore and the oxygen functional groups on the surface of activated carbon fiber(ACF)increased after the treatment with nitric acid,which was favorable to improve the catalytic activities of MnO_(x)-CeO_(x)/ACFN.The experimental results show that the conversion of NO is nearly 100%in the range 100℃-150℃under the optimal preparation conditions of MnO_(x)-CeO_(x)/ACFN.In addition,the effects of a series of performance parameters,including initial NH3 concentration,NO concentration and O_(2) concentration,on the conversion of NO were studied.
基金This study was supported by the Natural Science Foundation of Shan-dong Province(No.ZR2019QF012)the Natural Science and Develop-ment Foundation of Shenzhen(JCYJ20190807093205660)the Na-tional Natural Science Foundation of China(No.21902085).
文摘SnO 2 nanospheres with diameters of 30∼50 nm and Pt x Cu 1-x bimetallic nanoparticles with sizes of approxi-mately 10 nm were synthesized via hydrothermal and solvothermal methods,respectively.The Pt x Cu 1-x bimetal-lic nanoparticles were impregnated on the surface of the SnO 2 spheres to form Pt x Cu 1-x-SnO 2 nanocomposites.By varying the atomic ratios between platinum(Pt)and copper(Cu),we found that Pt 0.75 Cu 0.25-SnO 2,with a large specific surface area of 89.21 m 2/g,enabled the selective and accurate detection of low-concentration formalde-hyde compared to other metal-deposited samples and pure SnO 2.The response value of Pt 0.75 Cu 0.25-SnO 2 to 500×10−9 formaldehyde was approximately 20 at an operating temperature of 160◦C with an extremely high-speed response(15 s).The porous structures with large specific surface areas,as well as the improved catalytic effects of Pt 0.75 Cu 0.25,comprehensively contributed to the enhanced sensing performance towards formaldehyde.
