Abstract

Ordered mesoporous Zn/Al2O3 materials with varying Zn content were simply prepared via an evaporation-induced self-assembly (EISA) method. Dehydrogenation of isobutane to isobutene was carried out on these materials; an isobutane conversion of 45.0% and isobutene yield of 39.0% were obtained over the 10%Zn/Al2O3 catalyst at 580 °C with 300 h−1 GHSV. The obtained materials with Zn content up to 10% possess large specific surface area and big pore volume and zinc species can be highly dispersed on the surface or incorporated into the framework. The acidity of these catalysts was changed by the introduction of Zn, the decrease of strong acid sites is conducive to the promotion of isobutene selectivity and the weak and medium acidic sites played an important role in isobutane conversion. In addition, these catalysts exhibited good catalytic stability, due to the effective inhibition of coke formation by the ordered mesoporous structure.

Highlights

  • Isobutene is one of the most important raw materials and intermediates to produce butyl rubber, ETBE, polyisobutene and other chemicals.[1,2] To better ful ll the ever-increasing market demand, a small portion of its production is by isobutane dehydrogenation.[3]

  • A series of xZn/Al2O3 materials with various Zn content were prepared via one pot evaporationinduced self-assembly (EISA) strategy and tested in isobutane dehydrogenation reaction

  • The obtained materials with Zn content up to 10% possessed well-ordered mesopore with large speci c surface areas, big pore volumes and uniform pore size

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Summary

Introduction

Isobutene is one of the most important raw materials and intermediates to produce butyl rubber, ETBE (ethyl tert-butyl ether), polyisobutene and other chemicals.[1,2] To better ful ll the ever-increasing market demand, a small portion of its production is by isobutane dehydrogenation.[3]. Ordered and adjustable mesoporous alumina materials have drawn research much attention Coupled with their moderate surface acidity and good thermostability, ordered mesoporous alumina as heterogeneous catalyst support has a wonderful applying prospect.[18] Morris et al successfully synthesized NiO–Al2O3 composites with ordered mesoporous structure and the metal oxide well dispersed on the alumina support.[19] Yuan et al reported a simple route to synthesize g-Al2O3 using P123 template agent, which have high quality mesoporous structure.[20] Schweitzer et al put forward the computed minority catalytic pathway consists of undesired C–C bond cleavage at Zn(II) site had a signi cantly higher activation energy barrier and the high ole n selectivity observed for singlesite Zn(II) on SiO2.21 In our previous work, well-ordered mesoporous Cr2O3/Al2O3 catalysts were synthesized and showed an advantage in catalytic stability.[22] So far, almost no research was reported on ordered mesoporous zinc alumina composites for alkane dehydrogenation. This study rstly prepared ordered mesoporous xZn/Al2O3 catalysts with different Zn content via evaporation-induced selfassembly (EISA) method and evaluated the catalytic performances in isobutane dehydrogenation. The Zn content in a series of xZn/Al2O3 catalysts were measured by inductively coupled plasma optical emission spectrometer (ICP-OES, 725-ES, Agilent)

Catalyst preparation
Catalytic dehydrogenation
XRD analysis
Characterization
Nitrogen adsorption–desorption analysis
TEM analysis
XPS analysis
IV IV IV III IV IV III
H2-TPR pro les
NH3-TPD analysis
Catalytic performance in the isobutane dehydrogenation
Conclusions
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