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On the nature of active sites in alumina-supported zinc propane dehydrogenation catalysts
Molecular Catalysis ( IF 4.6 ) Pub Date : 2020-06-17 , DOI: 10.1016/j.mcat.2020.111055
Alexander I. Serykh , Yury A. Agafonov

Zinc-based materials are currently considered as an alternative for toxic chromium and costly platinum catalysts for propane dehydrogenation. So far however insufficient attention has been devoted to these materials in the literature. In this work we have revealed the nature of active sites in zinc-alumina (γ-alumina) catalysts. We have investigated zinc-alumina catalysts prepared by two different methods: traditional incipient wetness impregnation and zinc chemical vapor deposition (CVD) on alumina. The catalysts were characterized by infrared spectroscopy of adsorbed CO and H2 molecules, TPR measurements and tested in propane dehydrogenation. It has been shown that high-temperature interaction of zinc vapor with alumina results in the formation of surface Zn2+ cations which are active in hydrogen dissociation and propane conversion. The amount of zinc that can be introduced by this procedure depends on the alumina dehydroxylation degree. It has been found that molecular hydrogen heterolytically dissociates on Zn2+ surface cations resulting in the formation of surface zinc hydride species. The Zn2+ sites on the surface of alumina are heterogeneous and are characterized by different band positions in the IR spectra of adsorbed CO and H2 molecules. The Zn2+ sites are subjected to reduction under the reaction conditions.



中文翻译:

氧化铝负载的丙烷锌丙烷脱氢催化剂中活性位的性质

锌基材料目前被认为是有毒铬的替代品,也是丙烷脱氢的昂贵铂催化剂。到目前为止,文献中对这些材料的关注不足。在这项工作中,我们揭示了锌-氧化铝(γ-氧化铝)催化剂中活性位的性质。我们研究了通过两种不同方法制备的锌-氧化铝催化剂:传统的初湿浸渍法和在氧化铝上进行锌化学气相沉积(CVD)。通过吸附的CO和H 2分子的红外光谱,TPR测量并在丙烷脱氢中进行测试,对催化剂进行了表征。结果表明,锌蒸气与氧化铝的高温相互作用导致表面Zn 2+的形成。在氢离解和丙烷转化中具有活性的阳离子。可通过该程序引入的锌的量取决于氧化铝的脱羟基度。已经发现分子氢在Zn 2+表面阳离子上杂合解离,导致形成表面氢化锌物质。氧化铝表面上的Zn 2+位点是不均匀的,其特征在于吸附的CO和H 2分子的红外光谱中的能带位置不同。Zn 2+位点在反应条件下被还原。

更新日期:2020-06-17
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