Conversion of 4-methylpentan-2-ol over alkali–metal ion-exchanged X and Y zeolites: a microcalorimetric and catalytic investigation

A Auroux , P Artizzu , I Ferino , R Monaci , E Rombi , V Solinas
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引用次数: 20

Abstract

The acid-base properties of alkali–metal ion-exchanged X and Y zeolites were investigated by ammonia and sulfur dioxide adsorption microcalorimetry, in parallel with a catalytic reaction, viz. 4-methylpentan-2-ol conversion. Li and Na zeolites present much higher heats of NH3 adsorption and greater coverage at the same pressure than the other zeolites. The acidic strength of X differs by only a few kilojoules per mole from the corresponding Y zeolites. The amounts of SO2 adsorbed are very similar for all the Y zeolites except for LiY, on which the amount is smaller. X zeolites adsorb higher amounts than Y zeolites. Most of the samples have centres possessing significant basicity (Q>150 kJ mol−1). The main product from 4-methylpentan-2-ol, for both X and Y catalysts, was 4-methylpent-2-ene; on Y zeolites, which exhibited the higher catalytic activity, a larger amount of other types of isomer was generally formed. In the case of Cs-exchanged X, excess cesium oxide was also added by impregnation with Cs acetate. Microcalorimetric measurements indicated that the extra framework cesium oxide provided even stronger basic adsorption sites; the catalytic runs showed that a significant amount of 4-methylpentan-2-one was produced only on CsX containing excess Cs oxide.

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碱金属离子交换的X和Y沸石上4-甲基戊烷-2-醇的转化:微热法和催化研究
用氨和二氧化硫吸附微量热法研究了碱金属离子交换的X和Y沸石的酸碱性质,并进行了催化反应,即4-甲基戊烷-2-醇转化。在相同压力下,Li和Na沸石比其他沸石表现出更高的NH3吸附热和更大的覆盖范围。X分子筛的酸性强度与对应的Y分子筛的酸性强度仅相差几千焦耳/摩尔。除LiY分子筛吸附量较小外,所有Y型分子筛的SO2吸附量都非常相似。X型沸石吸附量高于Y型沸石。大多数样品的中心具有显著的碱度(Q>150 kJ mol−1)。对于X和Y催化剂,4-甲基戊烯-2-醇的主要产物是4-甲基戊烯;在表现出较高催化活性的Y型分子筛上,通常会形成大量其他类型的异构体。在Cs交换X的情况下,过量的氧化铯也通过Cs醋酸浸渍加入。微量热测量表明,额外的框架氧化铯提供了更强的碱性吸附位点;催化运行表明,只有在含有过量氧化铯的CsX上才能产生大量的4-甲基戊烷-2- 1。
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Author index Subject index Contents Investigation of organosilanes as structure-directing agents in zeolite synthesis The influence of gel properties on the kinetics of crystallization and particulate properties of MFI-type zeolities. I. The influence of time and temperature of gel ageing on the particulate properties of silicalite-1 microcrystals
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