工业级原料合成ZSM-35分子筛催化剂及其正丁烯骨架异构制异丁烯的应用
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摘要
本文以实验室小试ZSM-35分子筛合成配方为基础,采用工业级原料对ZSM-35分子筛进行了小规模放大合成,考察了工业级原料对ZSM-35分子筛理化特性及正丁烯骨架异构制异丁烯反应性能的影响。XRD、N2吸附-脱附表征结果表明,以工业级原料可以重复实验室小试合成结果,分子筛结晶度及酸性几乎保持不变,表面硅铝比略有升高。反应结果表明工业级原料合成的分子筛反应性能明显优于小试结果,异丁烯选择性升高且丙烯及重组分收率明显降低。
ZSM-35 catalysts for n-butene skeletal isomerization reaction were scaled up using industrial materials on the basis of lab tests. The catalysts were characterized by XRD,N_2 adsorption-desorption,XPS and NH3-TPD. The results showed that the ZSM-35 could be completely reproduced by using industrial materials. The crystallinity and the acidity remained the almost the same though the surface SiO_2/Al_2O_3 ratio slightly increased. The catalysts showed better catalytic results. The selectivity of iso-butene increased while the selectivity of propene and liquid products decreased.
ZSM-35 catalysts for n-butene skeletal isomerization reaction were scaled up using industrial materials on the basis of lab tests. The catalysts were characterized by XRD,N_2 adsorption-desorption,XPS and NH3-TPD. The results showed that the ZSM-35 could be completely reproduced by using industrial materials. The crystallinity and the acidity remained the almost the same though the surface SiO_2/Al_2O_3 ratio slightly increased. The catalysts showed better catalytic results. The selectivity of iso-butene increased while the selectivity of propene and liquid products decreased.
引文
[1]赵岚.丁烯异构化技术进展[J].石油化工,2010,17(4):39-42.
[2]Ménorval B D,Ayrault P,Gnep N S,et al.n-Butene skeletal isomerization over HFER zeolites:Influence of Si/Al ratio and of carbonaceous deposits[J].Applied Catalysis A:General,2006,304:1-13.
[3]Guisnet M,Andy P,Gnep N S,et al.Skeletal isomerization of n-butenes.I.mechanism of n-butene transformation on a nondeactivated H-ferrierite catalyst[J].Journal of Catealysis,1996,158:551-560.
[4]冯芳霞,窦涛,萧墉壮.纯硅ZSM-35的合成及模板剂的影响石油学报[J].石油加工,1998,14(3):77-80.
[5]Gy9rgy O.Comparison of butene skeletal isomerization selectivity over a pair of commercial H-ferrierites[J].Microporous and Mesoporous Materials,2007,104:192-198.
[2]Ménorval B D,Ayrault P,Gnep N S,et al.n-Butene skeletal isomerization over HFER zeolites:Influence of Si/Al ratio and of carbonaceous deposits[J].Applied Catalysis A:General,2006,304:1-13.
[3]Guisnet M,Andy P,Gnep N S,et al.Skeletal isomerization of n-butenes.I.mechanism of n-butene transformation on a nondeactivated H-ferrierite catalyst[J].Journal of Catealysis,1996,158:551-560.
[4]冯芳霞,窦涛,萧墉壮.纯硅ZSM-35的合成及模板剂的影响石油学报[J].石油加工,1998,14(3):77-80.
[5]Gy9rgy O.Comparison of butene skeletal isomerization selectivity over a pair of commercial H-ferrierites[J].Microporous and Mesoporous Materials,2007,104:192-198.