High-performance ring-opening catalysts based on iridium-containing zeolite Beta in the hydroconversion of decalin

[Display omitted] ► Open-chain decanes were made from decalin with unprecedented yields up to 44%. ► The acid strength of the Ir/Beta catalyst was tuned by exchange with alkali cations. ► The term high-performance ring-opening catalysts (HIPEROCs) was introduced. ► The main mechanism of ring opening...

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Veröffentlicht in:Applied catalysis. A, General General, 2013-03, Vol.455, p.46-57
Hauptverfasser: Santi, Dominic, Holl, Tobias, Calemma, Vincenzo, Weitkamp, Jens
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Sprache:eng
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Zusammenfassung:[Display omitted] ► Open-chain decanes were made from decalin with unprecedented yields up to 44%. ► The acid strength of the Ir/Beta catalyst was tuned by exchange with alkali cations. ► The term high-performance ring-opening catalysts (HIPEROCs) was introduced. ► The main mechanism of ring opening on HIPEROCs is hydrogenolysis on the metal. ► A detailed reaction scheme was advanced for selective ring opening on HIPEROCs. Decalin was converted in a flow-type reactor under a hydrogen pressure of 5.2MPa on Ir/H,A-Beta zeolite catalysts, where A stands for an alkali metal cation. In one series of catalysts, the Ir content was 3wt.%, and the nature of A was varied from lithium to cesium. In a second series, the iridium content in Ir/H,Cs-Beta was varied from 1 to 5wt.%. On some of these catalysts, open-chain decanes (OCDs) were formed with unprecedented selectivities and yields of up to 47 and 44%, respectively. The term “High-Performance Ring-Opening Catalysts” (HIPEROCs) was defined. Evidence is presented for hydrogenolysis on the metal being the main ring-opening mechanism on HIPEROCs. The main function of the Brønsted-acid sites is a mild isomerization of six-membered into five-membered naphthenic rings which are much easier to open by hydrogenolysis. Valuable mechanistic information can be deduced from the carbon-number distributions and the naphthenes vs. alkanes content of the hydrocracked products (C9-).
ISSN:0926-860X
1873-3875
DOI:10.1016/j.apcata.2013.01.020