Dimethyl ether(DME),as a promising alternative to diesel fuel and liquefied petroleum gas,has attracted considerable attention in catalysis domain.The catalytic direct synthesis of DME from syngas is an upand-coming r...Dimethyl ether(DME),as a promising alternative to diesel fuel and liquefied petroleum gas,has attracted considerable attention in catalysis domain.The catalytic direct synthesis of DME from syngas is an upand-coming route but remains a challenge.In this work,we firstly prepared a Cu-embedded porous Al_(2)O_(3)bifunctional catalyst(Cu@Al_(2)O_(3)-dp)by filling Cu-1,3,5-benzenetricarboxylate metal–organic framework(Cu-BTC MOF)with Al(OH)_(3) followed by a two-step calcination process(400℃for 4 h and 600℃for1 h),exhibiting excellent catalytic performance for direct synthesis of DME from syngas.Cu@Al_(2)O_(3)-dp catalyst demonstrates much higher CO conversion(25.7%vs.15.4%)and extremely higher DME selectivity(90.4%vs.63.9%)with the increased catalytic stability compared to the supported Cu catalyst on MOF-derived porous Al_(2)O_(3)(Cu/Al_(2)O_(3))prepared by incipient wetness impregnation method,ascribed to the unique embedding-type structure,promoted Cu dispersion and stronger metal-support interaction.This work not only provides an efficient syngas-to-DME catalyst,but also paves a new way for designing highly-efficient core-shell bifunctional catalysts for diverse consecutive reactions.展开更多
基金the National Natural Science Foundation of China(No.U1610104)Liaoning Revitalization Talents Program(No.XLYC1907053,China)CAS Youth Innovation Promotion Association(No.2018220,China)。
文摘Dimethyl ether(DME),as a promising alternative to diesel fuel and liquefied petroleum gas,has attracted considerable attention in catalysis domain.The catalytic direct synthesis of DME from syngas is an upand-coming route but remains a challenge.In this work,we firstly prepared a Cu-embedded porous Al_(2)O_(3)bifunctional catalyst(Cu@Al_(2)O_(3)-dp)by filling Cu-1,3,5-benzenetricarboxylate metal–organic framework(Cu-BTC MOF)with Al(OH)_(3) followed by a two-step calcination process(400℃for 4 h and 600℃for1 h),exhibiting excellent catalytic performance for direct synthesis of DME from syngas.Cu@Al_(2)O_(3)-dp catalyst demonstrates much higher CO conversion(25.7%vs.15.4%)and extremely higher DME selectivity(90.4%vs.63.9%)with the increased catalytic stability compared to the supported Cu catalyst on MOF-derived porous Al_(2)O_(3)(Cu/Al_(2)O_(3))prepared by incipient wetness impregnation method,ascribed to the unique embedding-type structure,promoted Cu dispersion and stronger metal-support interaction.This work not only provides an efficient syngas-to-DME catalyst,but also paves a new way for designing highly-efficient core-shell bifunctional catalysts for diverse consecutive reactions.
