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首页> 外文期刊>Catalysis science & technology >Mechanism of SAPO-34 catalyst deactivation in the course of MTO conversion in a slurry reactor
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Mechanism of SAPO-34 catalyst deactivation in the course of MTO conversion in a slurry reactor

机译：SAPO-34催化剂失活的机制在泥浆反应器的MTO转换

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摘要

The deactivation of a SAPO-34 catalyst in the course of the methanol-to-olefin conversion has been studied in a slurry reactor in polydimethylsiloxane medium and compared with that in a fixed-bed reactor. The carbonaceous deposits accumulated on the catalyst have been investigated by thermo-gravimetric analysis, UV/vis and fluorescence spectroscopy, the MALDI-TOF technique and GC/MS analysis after dissolution of used catalysts in hydrofluoric acid and extraction of coke with dichloromethane. The results show that under slurry conditions the catalyst deactivation is much faster than under fixed-bed conditions. The main reason for the fast deactivation is the accumulation of olefinic products on the catalyst/polydimethylsiloxane boundary due to their high solubility in polydimethylsiloxane. The proposed mechanism involves the interaction of olefins with aromatic compounds formed at the outer surface and in the pore mouths of the catalyst crystals leading to polyaromatic products, which block the entrances to the pores and prevent further reaction. It has been demonstrated that the stability of the catalytic activity with time on stream can be improved by decreasing the N-2/CH3OH molar ratio in the flow and by selective poisoning of BrOnsted acid sites at the outer surface of the crystals. The results obtained show the way for further improvement of catalytic performance in a slurry reactor.
机译：SAPO-34催化剂的失活methanol-to-olefin转换的过程研究浆反应堆聚二甲硅氧烷中并与这个床反应器。存款累积的催化剂研究了重分析,UV / vis和荧光光谱MALDI-TOF技术和GC / MS分析解散在氢氟酸的催化剂使用酸和二氯甲烷萃取的可乐。结果表明,在泥浆条件下催化剂失活要快得多固定床的条件。快速失活是烯的积累产品的催化剂/聚二甲硅氧烷边界由于他们的高溶解度聚二甲硅氧烷。涉及烯烃和芳烃之间的交互外表面和化合物形成的晶体导致毛孔口的催化剂聚芳产品,阻止入口毛孔,防止进一步的反应。被证明的稳定性催化活性随时间在流改善减少n / CH3OH摩尔比率流和选择性中毒的布仑斯惕酸网站的外表面晶体。催化性能的进一步改善泥浆反应堆。

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