The catalytic synthesis of 1,3-butadiene(1,3-BD)from bio-based ethanol offers an alternative and sustainable process beyond petroleum.However,the intrinsic active sites and corresponding mechanism of 1,3-BD formation ...The catalytic synthesis of 1,3-butadiene(1,3-BD)from bio-based ethanol offers an alternative and sustainable process beyond petroleum.However,the intrinsic active sites and corresponding mechanism of 1,3-BD formation have not been fully elucidated yet.By correlating systematic characterization results with catalytic performance,the open Zr species,i.e.,Zr(OH)(OSi)_(3)moieties,were identified as the active site over the Zr/MFI-BM catalysts for the catalytic transformation of ethanol-acetaldehyde into 1,3-BD.In conjunction with controlled experiments and theory calculations,ethanol and acetaldehyde are proposed to synergistically co-adsorb on the Zr(OH)(OSi)_(3)species in a bi-molecular mode,which assists the acetaldehyde condensation and accelerates the critical Meerwein-Ponndorf-Verley-Oppenauer reduction,and accordingly promotes 1,3-BD formation.These findings will stimulate the search towards new metal-zeolite combinations for efficient production of value-added 1,3-BD via biomass-derived ethanol and beyond.展开更多
文摘The catalytic synthesis of 1,3-butadiene(1,3-BD)from bio-based ethanol offers an alternative and sustainable process beyond petroleum.However,the intrinsic active sites and corresponding mechanism of 1,3-BD formation have not been fully elucidated yet.By correlating systematic characterization results with catalytic performance,the open Zr species,i.e.,Zr(OH)(OSi)_(3)moieties,were identified as the active site over the Zr/MFI-BM catalysts for the catalytic transformation of ethanol-acetaldehyde into 1,3-BD.In conjunction with controlled experiments and theory calculations,ethanol and acetaldehyde are proposed to synergistically co-adsorb on the Zr(OH)(OSi)_(3)species in a bi-molecular mode,which assists the acetaldehyde condensation and accelerates the critical Meerwein-Ponndorf-Verley-Oppenauer reduction,and accordingly promotes 1,3-BD formation.These findings will stimulate the search towards new metal-zeolite combinations for efficient production of value-added 1,3-BD via biomass-derived ethanol and beyond.
