Stability of protonic zeolites in the catalytic oxidation of chlorinated VOCs (1,2-dichloroethane)

Stability of protonic zeolites in the catalytic oxidation of chlorinated VOCs (1,2-dichloroethane)
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DOI:
10.1016/j.apcatb.2008.10.007
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发表时间:
2009-05-20
影响因子:
22.1
通讯作者:
Magnoux, P.
Magnoux, P.
中科院分区:
化学1区
文献类型:
--
作者:
Aranzabal, A.;Gonzalez-Marcos, J. A.;Magnoux, P.

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研究了质子分子筛在1,2-二氯乙烷(DCA)催化氧化反应中的失活现象. DCA氧化反应在常规固定床反应器中在大气压力下在空气中贫DCA浓度(1000 ppm)的条件下进行。通过气相色谱仪、基于IR光谱的分析仪和另一个UV分析仪分析出口组成。为了跟踪H-ZSM-5、H-MOR和H-ZSM-5在典型反应环境和条件(1000 ppm DCA,300 ℃,13,500 h(-1))下的催化稳定性,检查了沸石晶体结构的影响。为了更好地理解质子沸石的失活途径,分析了空速和温度对质子沸石耐久性的影响。由于反应过程中形成的一些产物也会导致失活,因此将H2O和HCl与DCA本身一起沿着引入进料流中,以评估它们的效果。结果表明,积炭是沸石催化剂失活的主要原因。焦炭由中间体氯乙烯(VC)形成,其由DCA的第一脱氯化氢步骤产生。(C)2008 Elsevier B. V.保留所有权利。
The deactivation of protonic zeolites in the catalytic oxidation of 1,2-dichloroethane (DCA) was evaluated. DCA oxidation reactions were carried out in a conventional fixed-bed reactor at atmospheric pressure under conditions of lean DCA concentration in air (1000 ppm). The outlet composition was analysed by a gas chromatograph, an IR spectroscopy-based analyser and another UV analyser. The effect of the zeolite crystalline structure was examined in order to track the catalytic stability of H-ZSM-5, H-MOR and H-BEA under typical reaction environment and conditions (1000 ppm DCA, 300 degrees C, 13,500 h(-1)). With the aim of a better understanding of the deactivation pathway, the influence of the space velocity and temperature on the durability of protonic zeolites was analysed. Since some products formed during reaction could also cause deactivation, H2O and HCl were introduced in the feed stream along with the DCA itself, so as to evaluate their effect. In general terms, coke formation was concluded to be the main reason for zeolite catalyst deactivation. Coke was formed from the intermediate vinyl chloride (VC), which resulted from a first dehydrochlorination step of DCA. (C) 2008 Elsevier B.V. All rights reserved.