Selectivity control is a difficult scientific and industrial challenge in methanol-to-olefins(MTO)conversion.It has been experimentally established that the topology of zeolite catalysts influenced the distribution of...Selectivity control is a difficult scientific and industrial challenge in methanol-to-olefins(MTO)conversion.It has been experimentally established that the topology of zeolite catalysts influenced the distribution of products.Besides the topology effect on reaction kinetics,the topology influences the diffusion of reactants and products in catalysts as well.In this work,by using COMPASS force-field molecular dynamics method,we investigated the intracrystalline diffusion of ethene and propene in four different zeolites,CHA,MFI,BEA and FAU,at different temperatures.The self-diffusion coefficients and diffusion activation barriers were calculated.A strong restriction on the diffusion of propene in CHA was observed because the self-diffusion coefficient ratio of ethene to propene is larger than 18 and the diffusion activation barrier of propene is more than 20 kJ/mol in CHA.This ratio decreases with the increase of temperature in the four investigated zeolites.The shape selectivity on products from diffusion perspective can provide some implications on the understanding of the selectivity difference between HSAPO-34 and HZSM-5 catalysts for the MTO conversion.展开更多
Biobutanol is attracting increasingly interest as a source of renewable energy and biofuels because of its many advantages over bioethanol that include higher energy density, fuel efficiency, and reduced engine damage...Biobutanol is attracting increasingly interest as a source of renewable energy and biofuels because of its many advantages over bioethanol that include higher energy density, fuel efficiency, and reduced engine damages. Currently, there is a growing interest in producing biobutanol from bioethanol, in view of the tremendous potential benefits of this transformation for the bulk production of biobutanol in a target specific manner. This perspective paper describes recent progress for the ethanol to butanol process. The different catalysts, including homogeneous and heterogeneous catalytic systems, for ethanol to butanol are outlined and compared, and the key issues and requirements for future developments are highlighted. A major challenge for further development and application of ethanol to butanol process is to find an optimal balance between different catalytic functions and to suppress the formation of side products that has plagued most catalytic bioethanol upgrading systems. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B. V. and Science Press. All rights reserved.展开更多
基金supported by the National Basic Research Program of China (2009CB623504)the National Science Foundation of China (21103231)Shanghai Science Foundation (11ZR1449700)
文摘Selectivity control is a difficult scientific and industrial challenge in methanol-to-olefins(MTO)conversion.It has been experimentally established that the topology of zeolite catalysts influenced the distribution of products.Besides the topology effect on reaction kinetics,the topology influences the diffusion of reactants and products in catalysts as well.In this work,by using COMPASS force-field molecular dynamics method,we investigated the intracrystalline diffusion of ethene and propene in four different zeolites,CHA,MFI,BEA and FAU,at different temperatures.The self-diffusion coefficients and diffusion activation barriers were calculated.A strong restriction on the diffusion of propene in CHA was observed because the self-diffusion coefficient ratio of ethene to propene is larger than 18 and the diffusion activation barrier of propene is more than 20 kJ/mol in CHA.This ratio decreases with the increase of temperature in the four investigated zeolites.The shape selectivity on products from diffusion perspective can provide some implications on the understanding of the selectivity difference between HSAPO-34 and HZSM-5 catalysts for the MTO conversion.
基金supported by the National Natural Science Foundation of China(21273044,21473035,and 91545108)SINOPEC(X514005)the Open project of State Key Laboratory of Chemical Engineering(SKL-Ch E-15C02)
文摘Biobutanol is attracting increasingly interest as a source of renewable energy and biofuels because of its many advantages over bioethanol that include higher energy density, fuel efficiency, and reduced engine damages. Currently, there is a growing interest in producing biobutanol from bioethanol, in view of the tremendous potential benefits of this transformation for the bulk production of biobutanol in a target specific manner. This perspective paper describes recent progress for the ethanol to butanol process. The different catalysts, including homogeneous and heterogeneous catalytic systems, for ethanol to butanol are outlined and compared, and the key issues and requirements for future developments are highlighted. A major challenge for further development and application of ethanol to butanol process is to find an optimal balance between different catalytic functions and to suppress the formation of side products that has plagued most catalytic bioethanol upgrading systems. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B. V. and Science Press. All rights reserved.
