Methanol-to-hydrocarbons reaction over SAPO-34. Molecules confined in the catalyst cavities at short time on stream

Methanol-to-hydrocarbons reaction over SAPO-34. Molecules confined in the catalyst cavities at short time on stream
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DOI:
10.1023/a:1009034600533
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发表时间:
2001-01-01
期刊:
影响因子:
2.8
通讯作者:
Kolboe, S
Kolboe, S
中科院分区:
化学4区
文献类型:
--
作者:
Arstad, B;Kolboe, S

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为了更深入地了解甲醇合成烃(MTH)反应,我们对SAPO-34催化剂中的有机分子进行了研究。反应进行不同时间,S 30min~30min。在预定的时间,反应停止,催化剂溶解在1M盐酸中。用气相色谱(MS检测器)分析了溶液上方的气相和CCl4萃取物。气相主要由异构烷烃C4-6组成。挥发性较低的有机分子集中在CCl4萃取物中。目前有200多种不同的物种,但具有1到6个甲基的多甲基苯总是占主导地位。它们占样本的30%-50%。五甲苯和六甲苯很容易从小碳氢化合物中分离出来,转化为二甲苯和三甲基苯。据推测,芳烃的甲基化可能是MTH反应中催化活性的重要部分,芳烃随后分裂出来,然后再重新甲基化。
In order to obtain more insight into the methanol-to-hydrocarbons (MTH) reaction the organic molecules confined in a working SAPO-34 catalyst have been studied. The reaction was run for varying times, 30 s to 30 min. At a predetermined time the reaction was stopped and the catalyst dissolved in 1 M HCl. The gas phase above the solution as well as a CCl4 extract were analyzed by gas chromatography (MS detector). The gas phase consists mainly of isoalkanes C4-6. The less volatile organic molecules were concentrated in the CCl4 extract. More than 200 different species are present, but polymethylbenzenes, with one to six methyl groups, are always dominating. They constitute 30-50% of the samples. Penta- and hexamethylbenzene easily split off small hydrocarbons and turn into di- and trimethylbenzenes. it is speculated that methylations of arenes which thereupon split off small alkenes and then are remethylated again may be an essential part of the catalytic activity in the MTH reaction.