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甲醇制汽油过程中沸石催化剂H-ZSM-5的失活:原位时间分辨和空间分辨X射线衍射

Deactivation of Zeolite Catalyst H-ZSM-5 during Conversion of Methanol to Gasoline: Operando Time- and Space-Resolved X-ray Diffraction.

作者信息

Rojo-Gama Daniel, Mentel Lukasz, Kalantzopoulos Georgios N, Pappas Dimitrios K, Dovgaliuk Iurii, Olsbye Unni, Lillerud Karl Petter, Beato Pablo, Lundegaard Lars F, Wragg David S, Svelle Stian

机构信息

Center for Materials Science and Nanotechnology (SMN), Department of Chemistry , University of Oslo , P.O. Box 1033, Blindern , N-0315 Oslo , Norway.

Haldor Topsøe A/S , Haldor Topsøes Allé 1 , 2800 Kgs. Lyngby , Denmark.

出版信息

J Phys Chem Lett. 2018 Mar 15;9(6):1324-1328. doi: 10.1021/acs.jpclett.8b00094. Epub 2018 Mar 5.

Abstract

The deactivation of zeolite catalyst H-ZSM-5 by coking during the conversion of methanol to hydrocarbons was monitored by high-energy space- and time-resolved operando X-ray diffraction (XRD) . Space resolution was achieved by continuous scanning along the axial length of a capillary fixed bed reactor with a time resolution of 10 s per scan. Using real structural parameters obtained from XRD, we can track the development of coke at different points in the reactor and link this to a kinetic model to correlate catalyst deactivation with structural changes occurring in the material. The "burning cigar" model of catalyst bed deactivation is directly observed in real time.

摘要

通过高能空间和时间分辨的原位X射线衍射(XRD)监测了甲醇转化为烃类过程中因结焦导致的沸石催化剂H-ZSM-5失活情况。通过沿毛细管固定床反应器轴向长度进行连续扫描实现空间分辨率,每次扫描的时间分辨率为10秒。利用从XRD获得的真实结构参数,我们可以追踪反应器中不同位置焦炭的生成情况,并将其与动力学模型联系起来,以关联催化剂失活与材料中发生的结构变化。直接实时观察到了催化剂床层失活的“燃烧雪茄”模型。

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