Platinum/cerium-zirconium-sulfate（Pt/Ce-Zr-SO_4^（2-）） catalysts were prepared by wetness impregnation.Catalytic activities were evaluated from the combustion of propene and CO.Sulfate（SO_4^（2-））addition improv...Platinum/cerium-zirconium-sulfate（Pt/Ce-Zr-SO_4^（2-）） catalysts were prepared by wetness impregnation.Catalytic activities were evaluated from the combustion of propene and CO.Sulfate（SO_4^（2-））addition improved the catalytic activity significantly.When using Pt/Ce-Zr-SO_4^（2-） with 10 wt%SO_4^（2-）,the temperature for 90%conversion of propene and CO decreased by 75℃ compared with Pt/Ce-Zr.The conversion exceeded 95%at 240℃ even after 0.02%sulfur dioxide poisoning for 20 h.Temperature-programmed desorption of CO and X-ray photoelectron spectroscopy analyses revealed an improvement in Pt dispersion onto the Ce-Zr-SO_4^（2-） support,and the increased number of Pt particles built up more Pt^（-）-（SO_4^（2-））^（-） couples,which resulted in excellent activity.The increased total acidity and new Bronsted acid sites on the surface provided the Pt/Ce-Zr-SO_4^（2-） with good sulfur resistance.展开更多
It is urgent to develop catalysts with application potential for oxidative coupling of methane(OCM)at relatively lower temperature.Herein,three-dimensional ordered macro porous(3 DOM)La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)(...It is urgent to develop catalysts with application potential for oxidative coupling of methane(OCM)at relatively lower temperature.Herein,three-dimensional ordered macro porous(3 DOM)La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)(A_(2)B_(2)O_(7)-type)catalysts with disordered defective cubic fluorite phased structure were successfully prepared by a colloidal crystal template method.3DOM structure promotes the accessibility of the gaseous reactants(O2and CH4)to the active sites.The co-doping of Ca and Sr ions in La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)catalysts improved the formation of oxygen vacancies,thereby leading to increased density of surface-active oxygen species(O_(2)^(-))for the activation of CH4and the formation of C2products(C2H6and C2H4).3DOM La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)catalysts exhibit high catalytic activity for OCM at low temperature.3DOM La1.7Sr0.3Ce1.7Ca0.3O7-δcatalyst with the highest density of O_(2)^(-)species exhibited the highest catalytic activity for low-temperature OCM,i.e.,its CH4conversion,selectivity and yield of C2products at 650℃are 32.2%,66.1%and 21.3%,respectively.The mechanism was proposed that the increase in surface oxygen vacancies induced by the co-doping of Ca and Sr ions boosts the key step of C-H bond breaking and C-C bond coupling in catalyzing low-temperature OCM.It is meaningful for the development of the low-temperature and high-efficient catalysts for OCM reaction in practical application.展开更多
The aim of this paper is to investigate the effect of nitrite intercalated Mg-Al layered double hydroxides(Mg-Al LDH-NO_(2))on mortar durability under the coexisting environment of Cl−and SO_(4)^(2-).Cl−and SO_(4)^(2-...The aim of this paper is to investigate the effect of nitrite intercalated Mg-Al layered double hydroxides(Mg-Al LDH-NO_(2))on mortar durability under the coexisting environment of Cl−and SO_(4)^(2-).Cl−and SO_(4)^(2-) binding properties of Mg-Al LDH-NO_(2) in simulated concrete pore solutions,Cl−and SO_(4)^(2-) diffusion properties of mortars with Mg-Al LDHNO 2 were examined.The steel corrosion and resistance of mortar against SO_(4)^(2-) attack were also evaluated.The results indicate that Mg-Al LDH-NO_(2) can effectively adsorb the Cl−and SO_(4)^(2-) in simulated concrete pore solution,and inhibit the diffusion of Cl−and SO_(4)^(2-) into cement mortars.The presence of SO_(4)^(2-) can greatly affect the uptake amount of Cl−,and there is a coupled effect of Cl−and SO_(4)^(2-) on their penetration into mortar specimens.In addition,Mg-Al LDH-NO_(2) can greatly upgrade the resistance of mortars against SO_(4)^(2-) attack and well prevent the steel from corrosion.However,Cl−will aggravate the SO_(4)^(2-) attack and SO_(4)^(2-) can initially decrease and then increase the steel corrosion.展开更多
基金supported by the National Natural Science Foundation of China(21506194,21676255)the Provincial Natural Science Foundation of Zhejiang Province(LY16B070011)the Commission of Science and Technology of Zhejiang Province(2017C33106,2017C03007)~~
文摘Platinum/cerium-zirconium-sulfate（Pt/Ce-Zr-SO_4^（2-）） catalysts were prepared by wetness impregnation.Catalytic activities were evaluated from the combustion of propene and CO.Sulfate（SO_4^（2-））addition improved the catalytic activity significantly.When using Pt/Ce-Zr-SO_4^（2-） with 10 wt%SO_4^（2-）,the temperature for 90%conversion of propene and CO decreased by 75℃ compared with Pt/Ce-Zr.The conversion exceeded 95%at 240℃ even after 0.02%sulfur dioxide poisoning for 20 h.Temperature-programmed desorption of CO and X-ray photoelectron spectroscopy analyses revealed an improvement in Pt dispersion onto the Ce-Zr-SO_4^（2-） support,and the increased number of Pt particles built up more Pt^（-）-（SO_4^（2-））^（-） couples,which resulted in excellent activity.The increased total acidity and new Bronsted acid sites on the surface provided the Pt/Ce-Zr-SO_4^（2-） with good sulfur resistance.
基金supported by the National Key Research and Development Program of China(Nos.2022YFB3504100,2022YFB3506200)the National Natural Science Foundation of China(Nos.22208373,22376217)+1 种基金the Beijing Nova Program(No.20220484215)the Science Foundation of China University of Petroleum,Beijing(No.2462023YJRC030)。
文摘It is urgent to develop catalysts with application potential for oxidative coupling of methane(OCM)at relatively lower temperature.Herein,three-dimensional ordered macro porous(3 DOM)La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)(A_(2)B_(2)O_(7)-type)catalysts with disordered defective cubic fluorite phased structure were successfully prepared by a colloidal crystal template method.3DOM structure promotes the accessibility of the gaseous reactants(O2and CH4)to the active sites.The co-doping of Ca and Sr ions in La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)catalysts improved the formation of oxygen vacancies,thereby leading to increased density of surface-active oxygen species(O_(2)^(-))for the activation of CH4and the formation of C2products(C2H6and C2H4).3DOM La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)catalysts exhibit high catalytic activity for OCM at low temperature.3DOM La1.7Sr0.3Ce1.7Ca0.3O7-δcatalyst with the highest density of O_(2)^(-)species exhibited the highest catalytic activity for low-temperature OCM,i.e.,its CH4conversion,selectivity and yield of C2products at 650℃are 32.2%,66.1%and 21.3%,respectively.The mechanism was proposed that the increase in surface oxygen vacancies induced by the co-doping of Ca and Sr ions boosts the key step of C-H bond breaking and C-C bond coupling in catalyzing low-temperature OCM.It is meaningful for the development of the low-temperature and high-efficient catalysts for OCM reaction in practical application.
基金Project(51478164)supported by the National Natural Science Foundation of ChinaProject(BK20181306)supported by Natural Science Foundation of Jiangsu Province,China。
文摘The aim of this paper is to investigate the effect of nitrite intercalated Mg-Al layered double hydroxides(Mg-Al LDH-NO_(2))on mortar durability under the coexisting environment of Cl−and SO_(4)^(2-).Cl−and SO_(4)^(2-) binding properties of Mg-Al LDH-NO_(2) in simulated concrete pore solutions,Cl−and SO_(4)^(2-) diffusion properties of mortars with Mg-Al LDHNO 2 were examined.The steel corrosion and resistance of mortar against SO_(4)^(2-) attack were also evaluated.The results indicate that Mg-Al LDH-NO_(2) can effectively adsorb the Cl−and SO_(4)^(2-) in simulated concrete pore solution,and inhibit the diffusion of Cl−and SO_(4)^(2-) into cement mortars.The presence of SO_(4)^(2-) can greatly affect the uptake amount of Cl−,and there is a coupled effect of Cl−and SO_(4)^(2-) on their penetration into mortar specimens.In addition,Mg-Al LDH-NO_(2) can greatly upgrade the resistance of mortars against SO_(4)^(2-) attack and well prevent the steel from corrosion.However,Cl−will aggravate the SO_(4)^(2-) attack and SO_(4)^(2-) can initially decrease and then increase the steel corrosion.
