A COMPARATIVE STUDY OF MICROWAVE AND BARRIER DISCHARGE PLASMA FOR THE REGENERATION OF SPENT ZEOLITE CATALYSTS

G. Bond, A. Halman, H. Eccles, R. Mao, S. Pollington, P. Hinde, V. Demidyuk, A. Gkelios
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Abstract

Due to their acid characteristics and pore structure, which can induce high product selectivity; zeolite catalysts are used extensively in industry to catalyse reactions involving hydrocarbons.  However, these catalysts can suffer from deactivation due to cracking reactions that result in the deposition of carbon leading to poisoning of the acid sites and blocking of the pores [1].  Depending upon the reaction and the particular catalyst involved this deactivation may take place over several months or even years but in some cases occurs in minutes.  Therefore, zeolite catalysts are frequently reactivated / regenerated.  This generally involves a thermal treatment involving air which results in oxidation of the carbon [2].  However, the oxidation of carbon is highly exothermic, and if not carefully controlled, results in the generation of exceedingly high localized temperatures which can destroy the zeolite structure and result in subsequent loss of catalyst activity.  More conservative thermal treatments can result in incomplete regeneration and again a catalyst displaying inferior activity. This paper explores the use of non-thermal plasma which had been either generated using microwaves or via a barrier discharge to regenerate spent zeolite catalysts.  The catalyst, H-mordenite, was tested for the disproportionation of toluene (Figure 1) using conventional heating.  The spent catalyst was then regenerated using a plasma or conventional thermal treatment before having its activity re-evaluated for the toluene disproportionation reaction as previous.           Fig. 1. Reaction Scheme for Toluene Disproportionation.   Interestingly, not only is plasma regeneration highly effective but also catalysts can be regenerated in greatly reduced times.  There is an additional advantage in that plasma regeneration can impart physical properties that result in a zeolite that is resistant to further deactivation.  However, the results are highly dependent upon the experimental conditions involved for plasma regeneration.   References Wu J, Leu L., Appl. Catal., 1983; 7:283-294. M. Guisnet and P. Magnoux, Deactivation of Zeolites by Coking. Prevention of Deactivation and Regeneration. In: Zeolite Microporous Solids: Synthesis, Structure, and Reactivity. E.G. Derouane, F Lemos, C. Naccache, F. Ramôa Ribeiro, Eds. Pages 437-456. Springer 1992.
微波与阻挡放电等离子体再生废沸石催化剂的比较研究
由于它们的酸性特性和孔隙结构,可以诱导高的产物选择性;沸石催化剂在工业上广泛用于催化烃类反应。然而,由于裂解反应,这些催化剂可能会失活,从而导致碳沉积,导致酸位点中毒和堵塞孔隙b[1]。根据反应和所涉及的特定催化剂的不同,这种失活可能在几个月甚至几年的时间内发生,但在某些情况下,几分钟就会发生。因此,沸石催化剂经常被再活化/再生。这通常涉及涉及空气的热处理,导致碳bb0氧化。然而,碳的氧化是高度放热的,如果不小心控制,会导致产生极高的局部温度,从而破坏沸石结构并导致催化剂活性的损失。更保守的热处理会导致再生不完全,并再次显示较差的催化剂活性。本文探讨了利用微波或屏障放电产生的非热等离子体再生废沸石催化剂的方法。催化剂,h -丝光沸石,测试了歧化甲苯(图1)使用常规加热。然后使用等离子体或传统热处理对废催化剂进行再生,然后像以前一样重新评估其甲苯歧化反应的活性。图1所示。甲苯歧化反应方案。有趣的是,等离子体再生不仅非常有效,而且催化剂的再生时间也大大缩短。还有一个额外的优点是等离子体再生可以赋予物理特性,从而使沸石具有抵抗进一步失活的能力。然而,结果高度依赖于等离子体再生的实验条件。参考文献吴杰,刘磊,李鹏。Catal。, 1983;7:283 - 294。M. Guisnet和P. Magnoux,焦化沸石的失活。防止失活和再生。见:沸石微孔固体:合成、结构和反应性。E.G. Derouane, F Lemos, C. Naccache, F. Ramôa Ribeiro, Eds。页437 - 456。施普林格1992年。
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