Oxidative coupling of methane to ethylene is of high importance to the future of light olefin industry.However,the carbon atom efficiency is normally below 50%in gas phase reaction which is limited to the overoxidatio...Oxidative coupling of methane to ethylene is of high importance to the future of light olefin industry.However,the carbon atom efficiency is normally below 50%in gas phase reaction which is limited to the overoxidation of methane to carbon dioxide with oxidants.Here we present an alternative approach of electrochemical oxidation of methane in an oxygen permeation membrane reactor and show the highest conversion of methane and C2 selectivity of 28%and 40.2%at 1150℃,respectively.We prepare the 100-μm-thick perovskite(La0.8 Sr0.2)1-x Cr0.5 Fe0.5 O3-δ(LSCrF)dense membrane(La0.8 Sr0.2)1-xCr0.5 Fe0.5O3-δ(LSCrF–Fe)(x=0,0.02,0.05 and 0.10)scaffolds while the excess of Fe would be exsolved on porous skeleton to create metal-oxide interfaces toward methane oxidation.The metal-oxide interfaces not only facilitate the activation of C–H bond in methane but also enhance the coking resistance.展开更多
Dehydrogenation coupling of methane(DCM),which can be effectively used to produce low carbon alkenes,has the advantages of rich raw materials,simple reaction device,low energy consumption,etc.Herein,we report a series...Dehydrogenation coupling of methane(DCM),which can be effectively used to produce low carbon alkenes,has the advantages of rich raw materials,simple reaction device,low energy consumption,etc.Herein,we report a series of Co doped perovskite porous-dense BaCe_(0.9)Y_(0.1)Co_(x)O_(3-δ)(BCYCx)membrane for DCM.After treatment in a reduced atmosphere,a large number of Co nanoparticles will exsolute on the surface of BCY.The metal-oxide interface is helpful to activate the C–H bonds,inhibit the carbon deposition,and so on.The XRD,SEM and XPS prove that Co nanoparticles homogeneously distributed on the BCYCx porous layers,which will create a large quantity of catalytic active sites.At 1100℃,the highest concentration of C_(2)product was 5.66%(5.25%ethane+0.41%ethylene)in output gas when methane conversion reaches a maximum value of 24.8%,and the C_(2)selectivity gets to 45.6%.We further demonstrate the catalytic performance of high-temperature DCM without obvious decrease after running for 30 hours.展开更多
基金Supported by the National Key Research and Development Program of China(2017YFA0700102)National Natural Science Foundation of China(91845202)+1 种基金Dalian National Laboratory for Clean Energy(DNL180404)Strategic Priority Research Program of Chinese Academy of Sciences(XDB2000000)。
文摘Oxidative coupling of methane to ethylene is of high importance to the future of light olefin industry.However,the carbon atom efficiency is normally below 50%in gas phase reaction which is limited to the overoxidation of methane to carbon dioxide with oxidants.Here we present an alternative approach of electrochemical oxidation of methane in an oxygen permeation membrane reactor and show the highest conversion of methane and C2 selectivity of 28%and 40.2%at 1150℃,respectively.We prepare the 100-μm-thick perovskite(La0.8 Sr0.2)1-x Cr0.5 Fe0.5 O3-δ(LSCrF)dense membrane(La0.8 Sr0.2)1-xCr0.5 Fe0.5O3-δ(LSCrF–Fe)(x=0,0.02,0.05 and 0.10)scaffolds while the excess of Fe would be exsolved on porous skeleton to create metal-oxide interfaces toward methane oxidation.The metal-oxide interfaces not only facilitate the activation of C–H bond in methane but also enhance the coking resistance.
基金the National Key Research and Development Program of China(2017YFA0700102)Natural Science Foundation of China(91845202)+1 种基金Dalian National Laboratory for Clean Energy(DNL180404)Strategic Priority Research Program of Chinese Academy of Sciences(XDB2000000)。
文摘Dehydrogenation coupling of methane(DCM),which can be effectively used to produce low carbon alkenes,has the advantages of rich raw materials,simple reaction device,low energy consumption,etc.Herein,we report a series of Co doped perovskite porous-dense BaCe_(0.9)Y_(0.1)Co_(x)O_(3-δ)(BCYCx)membrane for DCM.After treatment in a reduced atmosphere,a large number of Co nanoparticles will exsolute on the surface of BCY.The metal-oxide interface is helpful to activate the C–H bonds,inhibit the carbon deposition,and so on.The XRD,SEM and XPS prove that Co nanoparticles homogeneously distributed on the BCYCx porous layers,which will create a large quantity of catalytic active sites.At 1100℃,the highest concentration of C_(2)product was 5.66%(5.25%ethane+0.41%ethylene)in output gas when methane conversion reaches a maximum value of 24.8%,and the C_(2)selectivity gets to 45.6%.We further demonstrate the catalytic performance of high-temperature DCM without obvious decrease after running for 30 hours.
