A novel route involving self‐metathesis of1‐butene under mild conditions that gave high yields ofethene and hexene was proposed.The results of thermodynamic analysis revealed that the Gibbsenergy of the target Metat...A novel route involving self‐metathesis of1‐butene under mild conditions that gave high yields ofethene and hexene was proposed.The results of thermodynamic analysis revealed that the Gibbsenergy of the target Metathesis I reaction(1‐butene?ethene+3‐hexene)was much higher thanthat of the main side Metathesis II(1‐butene+2‐butene?propene+2‐pentene).Suppression of1‐butene double‐bond isomerization was the key step to increase the selectivity for the target olefinin the reaction network.The relationship between the catalytic performance and support nature was investigated in detail.On basis of H2‐TPR,UV‐Vis spectra and HRTEM results,an alumina(Al2O3)support with large surface area was beneficial for the dispersion of molybdenum(Mo)species.Both suitable acidity and sufficient Mo dispersion were important to selectively promote the self‐metathesis reaction of1‐butene.On the optimal6Mo/Al2O3catalyst,1‐butene conversion reached47%and ethene selectivity was as high as42%on the premise of good catalytic stability(80°C,1.0MPa,3h?1).?2018,Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by Elsevier B.V.All rights reserved.展开更多
The performance of ZRP zeolite catalysts for aromatization of C6 aliphatic hydrocarbons was investigated in a pulsed microreactor. The influence of metal modified ZRP zeolites on aromatization reaction was also studie...The performance of ZRP zeolite catalysts for aromatization of C6 aliphatic hydrocarbons was investigated in a pulsed microreactor. The influence of metal modified ZRP zeolites on aromatization reaction was also studied, coupled with comparison of aromatization tendencies of olefins, paraffins and paraffins with different degrees of chain branching. Test results had shown that the lower the silicon/aluminum ratio in the ZRP zeolite, the higher the aromatization reactivity of aliphatic hydrocarbons. Modification of ZRP zeolite by zinc and its zinc content had apparent impact on the yield and distribution of aromatics. The aromatization tendency of olefins was apparently better than paraffins, while the aromatization tendency of monomethyl paraffins was better than that of straight-chain paraffins with the exception of dimethyl paraffins, which had worse aromatization tendency because of their steric hindrance.展开更多
Pt@ZIF-8 composites with crystallite sizes of ca.150 nm were synthesized.The composite was used as a catalyst for the regioselective hydrogenation of trans-1,3-hexadiene to 3-hexene.1-Hexyne was hydrogenated to 1-hexe...Pt@ZIF-8 composites with crystallite sizes of ca.150 nm were synthesized.The composite was used as a catalyst for the regioselective hydrogenation of trans-1,3-hexadiene to 3-hexene.1-Hexyne was hydrogenated to 1-hexene and hexane while 3-hexyne did not react.In all cases,the Pt@ZIF-8 composite had higher selectivity than Pt/C.展开更多
文摘A novel route involving self‐metathesis of1‐butene under mild conditions that gave high yields ofethene and hexene was proposed.The results of thermodynamic analysis revealed that the Gibbsenergy of the target Metathesis I reaction(1‐butene?ethene+3‐hexene)was much higher thanthat of the main side Metathesis II(1‐butene+2‐butene?propene+2‐pentene).Suppression of1‐butene double‐bond isomerization was the key step to increase the selectivity for the target olefinin the reaction network.The relationship between the catalytic performance and support nature was investigated in detail.On basis of H2‐TPR,UV‐Vis spectra and HRTEM results,an alumina(Al2O3)support with large surface area was beneficial for the dispersion of molybdenum(Mo)species.Both suitable acidity and sufficient Mo dispersion were important to selectively promote the self‐metathesis reaction of1‐butene.On the optimal6Mo/Al2O3catalyst,1‐butene conversion reached47%and ethene selectivity was as high as42%on the premise of good catalytic stability(80°C,1.0MPa,3h?1).?2018,Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by Elsevier B.V.All rights reserved.
文摘The performance of ZRP zeolite catalysts for aromatization of C6 aliphatic hydrocarbons was investigated in a pulsed microreactor. The influence of metal modified ZRP zeolites on aromatization reaction was also studied, coupled with comparison of aromatization tendencies of olefins, paraffins and paraffins with different degrees of chain branching. Test results had shown that the lower the silicon/aluminum ratio in the ZRP zeolite, the higher the aromatization reactivity of aliphatic hydrocarbons. Modification of ZRP zeolite by zinc and its zinc content had apparent impact on the yield and distribution of aromatics. The aromatization tendency of olefins was apparently better than paraffins, while the aromatization tendency of monomethyl paraffins was better than that of straight-chain paraffins with the exception of dimethyl paraffins, which had worse aromatization tendency because of their steric hindrance.
基金the financial support from National Science Foundation(DMR-1334928)Acquisition of data on trace analysis and GC instruments used in the IMSERC facility of Northwestern University was made possible by support from Northwestern University and grant CHE-0923236 from the National Science Foundation,respectively.C.J.S would like to acknowledge Dr Benjamin Klahr and Cassandra Whitford for recording SEM and TEM data,respectively.C.J.S.would also like to acknowledge Dr Neil Schweitzer for helpful discussion relating to catalytic results.This work made use of the EPIC facility(NUANCE Center-Northwestern University)+3 种基金which has received support from the MRSEC program(NSF DMR-1121262)the Materials Research Centerthe Nanoscale Science and Engineering Center(NSF EEC-0647560)at the International Institute for Nanotechnologythe State of Illinois,through the International Institute for Nanotechnology.
文摘Pt@ZIF-8 composites with crystallite sizes of ca.150 nm were synthesized.The composite was used as a catalyst for the regioselective hydrogenation of trans-1,3-hexadiene to 3-hexene.1-Hexyne was hydrogenated to 1-hexene and hexane while 3-hexyne did not react.In all cases,the Pt@ZIF-8 composite had higher selectivity than Pt/C.
