Effect of Support Species on Performance of Transition Metal-based Catalysts for Propane Dehydrogenation with Co-feeding of H2S
Effect of Support Species on Performance of Transition Metal-based Catalysts for Propane Dehydrogenation with Co-feeding of H2S
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DOI：
10.1627/jpi.63.228
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发表时间：
2020-01-01
影响因子：
1
通讯作者：
Fukuhara, Choji
中科院分区：
文献类型：
--
作者：
Watanabe, Ryo;Hirata, Nozomu;Fukuhara, Choji
考察了载体（SiO2、γ-Al 2 O3、ZrO 2、CeO 2、MgO）对过渡金属（Fe、Co、Ni）催化剂在H2S共进料下丙烷脱氢反应性能的影响。催化剂活性的评价表明，惰性SiO2是PDH催化剂的合适载体。SiO2负载的Fe催化剂表现出最高的活性和选择性之间的调查催化剂。为了阐明载体种类对催化剂组分的结构和电子状态的影响，使用X射线衍射（XRD）、X射线吸收精细结构（XAFS）和X射线光电子能谱（XPS）来表征各种Fe负载的催化剂。从Fe的K边X射线吸收近边结构（XANES）分析可知，Fe处于较高氧化态的催化剂具有较好的加氢性能。当使用SiO2和Al 2 O3作为载体时，通过XPS分析检测到二价和三价Fe阳离子。这种高价Fe物质可以接受来自中间物质的电子，从而增强脱氢性能。
This study investigated the effect of catalyst supports (SiO2, gamma-Al2O3, ZrO2, CeO2, MgO) on the performance of transition metal (Fe, Co, Ni) catalysts for propane dehydrogenation (PDH) with co-feeding of hydrogen sulfide (H2S). Evaluation of the catalyst activity indicated that inert SiO2 is a suitable support for the PDH catalysts. The SiO2-supported Fe catalysts showed the highest activity and selectivity among the investigated catalysts. In order to clarify the effect of the support species on the structure and electronic state of the catalyst components, X-ray diffraction (XRD), X-ray absorption fine structure (XAFS), and X-ray photoelectron spectroscopy (XPS) were used to characterize the various Fe-loaded catalysts. From Fe K-edge X-ray absorption near edge structure (XANES) analysis, it is deduced that the catalysts in which Fe was in a higher oxidation state showed better performance for PDH with co-feeding of H2S. When SiO2 and Al2O3 were used as the supports, divalent and trivalent Fe cations were detected by XPS analysis. Such high-valence Fe species can accept an electron from an intermediate species, thereby enhancing the dehydrogenation performance.