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NiO-based ceramic structured catalysts for ethylene production: Substrates and active sites
Catalysis Today ( IF 5.3 ) Pub Date : 2020-09-15 , DOI: 10.1016/j.cattod.2020.09.005
P. Brussino , E.D. Banús , M.A. Ulla , J.P. Bortolozzi

Structured catalysts have important advantages compared to powder formulations and they are required for processes intensification. In this work, three different ceramic structures: a cordierite monolith, an alumina foam and an alumina-silica paper were used as substrates for the deposition of a NiO-Al2O3 coating and tested in the oxidative dehydrogenation of ethane to produce ethylene. For comparison, a NiO-Al2O3 powder catalyst was also prepared. Nickel oxide species with different physicochemical features were obtained over each structure, evidenced by morphological (SEM-EDX) and physicochemical characterization (XRD, LRS and XPS). The best distributions of the catalytic coatings and NiO physicochemical properties were obtained when the monolith and the foam were used as substrates. These led to higher NiO-Al2O3 interactions and consequently to high ethylene selectivity values, 70–90 %, corresponding to the former an ethane conversion of 22 % and to the latter a 5 %. The distribution of the active phase on the ceramic paper was heterogeneous, with NiO agglomerations and poor NiO-support interaction thus achieving low olefin selectivity (∼ 30 %). The addition of a second element such as cerium was also studied in those structured catalysts with high selectivity, resulting in both cases in an increment of ethane conversion but a decrease in ethylene selectivity. This behavior was attributed to the generation of electrophilic oxygen species.



中文翻译:

用于乙烯生产的 NiO 基陶瓷结构催化剂:底物和活性位点

与粉末配方相比,结构化催化剂具有重要优势,并且它们是工艺强化所必需的。在这项工作中,三种不同的陶瓷结构:堇青石整料、氧化铝泡沫和氧化铝-二氧化硅纸被用作沉积 NiO-Al 2 O 3涂层的基材,并在乙烷的氧化脱氢生产乙烯中进行测试。为了比较,NiO-Al 2 O 3还制备了粉末催化剂。通过形态学 (SEM-EDX) 和物理化学表征 (XRD、LRS 和 XPS) 证明,在每个结构上都获得了具有不同物理化学特征的氧化镍物质。当整料和泡沫用作基材时,获得了催化涂层和 NiO 理化性质的最佳分布。这些导致更高的 NiO-Al 2 O 3相互作用,因此达到高乙烯选择性值,70-90%,对应于前者的乙烷转化率为 22%,后者为 5%。陶瓷纸上活性相的分布是不均匀的,具有 NiO 团聚和较差的 NiO 载体相互作用,从而实现了低烯烃选择性(~30%)。在那些具有高选择性的结构化催化剂中还研究了添加第二元素如铈,导致乙烷转化率增加但乙烯选择性降低。这种行为归因于亲电氧物种的产生。

更新日期:2020-09-15
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