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
Cr_(2)O_(3)-bearing castables bonded with reactive MgO(RM)or calcium aluminate cement(CAC)were studied to evaluate the binder effect on their performance in corrosive environments.The properties of the as-prepared cas...Cr_(2)O_(3)-bearing castables bonded with reactive MgO(RM)or calcium aluminate cement(CAC)were studied to evaluate the binder effect on their performance in corrosive environments.The properties of the as-prepared castables were compared with respect to the differences in phase composition and microstructure.The corrosion behavior of the as-prepared castables by CaO-Al_(2)O_(3)-Fe_(2)O_(3)-SiO_(2)-based slag was systematically compared viarefractory cup testing at 1600℃with respect to the differences in phase composition and microstructure.The analysis indicates that RM bonded castables show higher apparent porosity,lower bulk density and strengths after drying at 110℃and firing at 1300℃,and higher permanent linear change after firing at 1300℃,but better slag corrosion and infiltration resistance compared with CAC bonded castables.展开更多
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the Joint Founds of R&D Program of Henan Province (222301420034)National Natural Science Foundation of China (51802287)Collaborative Innovation Major Special Project of Zhengzhou (No. 20XTZX12025) for the financial support
文摘Cr_(2)O_(3)-bearing castables bonded with reactive MgO(RM)or calcium aluminate cement(CAC)were studied to evaluate the binder effect on their performance in corrosive environments.The properties of the as-prepared castables were compared with respect to the differences in phase composition and microstructure.The corrosion behavior of the as-prepared castables by CaO-Al_(2)O_(3)-Fe_(2)O_(3)-SiO_(2)-based slag was systematically compared viarefractory cup testing at 1600℃with respect to the differences in phase composition and microstructure.The analysis indicates that RM bonded castables show higher apparent porosity,lower bulk density and strengths after drying at 110℃and firing at 1300℃,and higher permanent linear change after firing at 1300℃,but better slag corrosion and infiltration resistance compared with CAC bonded castables.
