Citation: Christian Ahoba-Sam, Marius Westgård Erichsen, Unni Olsbye. Ethene and butene oligomerization over isostructural H-SAPO-5 and H-SSZ-24: Kinetics and mechanism[J]. Chinese Journal of Catalysis, ;2019, 40(11): 1766-1777. doi: S1872-2067(19)63426-1 shu

Ethene and butene oligomerization over isostructural H-SAPO-5 and H-SSZ-24: Kinetics and mechanism

SMN Centre for Materials Science and Nanotechnology, Department of Chemistry, University of Oslo, N-0315 Oslo, Norway. aCurrent address:Matriks AS, Gaustadallèen 21, 0349 Oslo, Norway

Received Date: 17 June 2019
Revised Date: 20 June 2019

Brønsted-acidic zeolite and zeotype materials are potential catalysts for the conversion of ethene to higher alkenes. In this study, two materials with AFI structure but different acid strength, H-SAPO-5 and H-SSZ-24, were subject to studies of ethene, cis-2-butene and ethene-butene mixture conversion under conditions where C₃-C₅ alkene formation is thermodynamically favoured over higher hydrocarbons (673-823 K, 1 atm). Ethene and cis-2-butene partial pressures were varied in the range 9-60 and 0.9-8.1 kPa, respectively, and contact times were varied in the range 3.78-756 and 0.573-76.4 s.µmol H+/cm³ over H-SAPO-5 and H-SSZ-24, respectively. Less than 1% conversion of ethene and less than 10% conversion of butene was obtained in the range of conditions used for elucidation of rate parameters.
The ethene conversion rates were more than an order of magnitude higher over the more acidic H-SSZ-24 than over H-SAPO-5 (6.5 vs. 0.3 mmol/mol H⁺.s at 748 K, P_ethene=33 kPa), with corre-sponding lower reaction order in ethene (1.5 vs. 2.0 at 673 K) and lower apparent activation energy (52 vs. 80 kJ/mol at 698-823 K). Propene selectivity was substantially higher over H-SSZ-24 than over H-SAPO-5 (68% vs. 36% at 0.5% ethene conversion). A similar difference in apparent reaction rates was observed for cis-2-butene conversion over the two catalysts, and for co-feeds of ethene and cis-2-butene. However, the cis-2-butene conversion to C₃-C₅ alkenes was found to be severely influenced by thermodynamic limitations, impeding a detailed kinetic analysis, and leading predominantly to isobutene formation at the highest temperatures.
- Ethene oligomerization,
- Butene oligomerization,
- Kinetics,
- Zeolite,
- Acid strength,
- H-SAPO-5,
- H-SSZ-24
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