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Elucidating the nature of Mo species on ZSM-5 and its role in the methane aromatization reaction
Reaction Chemistry & Engineering ( IF 3.4 ) Pub Date : 2021-4-27 , DOI: 10.1039/d1re00044f
Ángeles López-Martín 1, 2, 3, 4, 5 , Francisco Platero 1, 2, 3, 4, 5 , Gerardo Colón 1, 2, 3, 4, 5 , Alfonso Caballero 1, 2, 3, 4, 5
Affiliation  

The valorization of methane is one of the most important goals during the transition period to the general use of renewable energies. Its transformation into a valuable chemical like benzene by direct aromatization of methane (DAM) reaction has been extensively studied in the past years, mainly using Mo/ZSM-5 catalytic systems. Although viable, this DAM reaction poses a number of issues mainly derived from poor conversion and deactivation processes. Therefore, a deeper knowledge of these systems is needed. Herein, by combining chemical (TPR), spectroscopic (XPS), HAADF and other techniques, we have identified the different Mo precursors stabilized in the calcined ZSM-5 support, their nature (monomers, dimers and bulk Mo oxides), location in the zeolite framework (external surface or micropores), and the partial segregation of aluminum during the preparation of catalysts. The role of each Mo phase promoting or hindering the transformation of methane in aromatics has been also clarified.

中文翻译:

阐明ZSM-5上Mo物种的性质及其在甲烷芳构化反应中的作用

在向可再生能源的一般使用过渡期间,甲烷的增值是最重要的目标之一。过去几年中,主要是使用Mo / ZSM-5催化系统,对通过甲烷直接芳香化(DAM)反应将其转化为有价值的化学物质(如苯)进行了广泛的研究。尽管可行,但这种DAM反应会带来许多问题,这些问题主要是由于转化和失活过程不佳而引起的。因此,需要对这些系统有更深入的了解。本文中,通过结合化学(TPR),光谱(XPS),HAADF和其他技术,我们确定了在煅烧过的ZSM-5载体中稳定的不同Mo前体,其性质(单体,二聚体和块状Mo氧化物),在金属中的位置沸石骨架(外表面或微孔),以及催化剂制备过程中铝的部分偏析。还已经阐明了每个Mo相促进或阻碍甲烷在芳族化合物中转化的作用。
更新日期:2021-05-13
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