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In-depth structural and analytical study of the washcoating layer of a Mn-Cu monolithic catalyst using STEM-FIB, EDX and EELS. Insights into stability under working conditions
Applied Surface Science ( IF 6.3 ) Pub Date : 2021-06-08 , DOI: 10.1016/j.apsusc.2021.150318
Maria R. Morales , Luc Lajaunie , José Juan Calvino , Miguel Ángel Cauqui , Luis E. Cadus , Juan Carlos Hernández-Garrido

The texture, structure, composition, and electronic state of new and used monolithic Mn-Cu catalysts were studied. Characterisation was performed at different scales and spatial resolution by combining STEM-FIB and imaging techniques (STEM-HAADF) and spectroscopy (STEM-EDX and EELS of space resolution). A thickness of the alumina layer that varies between 1 and 2 µm was observed, while the thickness of the Mn-Cu catalyst layer varies linearly with the number of charges between 1 µm and 2 µm, for 1 and 2 charges, respectively. In both fresh and used catalysts, the migration of both phases was observed to a different extent, depending on the number of charges of the Mn-Cu phase. This was associated with the synthesis conditions or the catalytic behaviour in the combustion of the n -hexane. The STEM-EDX analyses showed a homogeneous distribution of Mn and Cu, with values like the theoretical one. At the nanoscale, the SR-EELS analyses detected the presence of nanometric patches with lower Cu content, chemically inhomogeneous with a higher Mn oxidation state than the rest of the material. The advanced characterisation techniques used in this work allowed the precise identification of part of the constitutive phases of the Mn-Cu system generated in-situ on the monolith. Among them, manganese oxides with different oxidation states (MnO, Mn3O4, Mn2O3), Mn3Cu3O8 and CuO were detected.



中文翻译:

使用 STEM-FIB、EDX 和 EELS 对 Mn-Cu 整体催化剂的洗涂层进行深入的结构和分析研究。深入了解工作条件下的稳定性

研究了新的和已使用的整体式 Mn-Cu 催化剂的织构、结构、组成和电子状态。通过结合 STEM-FIB 和成像技术 (STEM-HAADF) 和光谱学(空间分辨率的 STEM-EDX 和 EELS),在不同尺度和空间分辨率下进行表征。观察到氧化铝层的厚度在 1 到 2 µm 之间变化,而 Mn-Cu 催化剂层的厚度随电荷数在 1 µm 到 2 µm 之间线性变化,分别为 1 和 2 次充电。在新鲜和用过的催化剂中,根据 Mn-Cu 相的电荷数,观察到两相的迁移程度不同。这与合成条件或正己烷燃烧中的催化行为有关。STEM-EDX 分析显示 Mn 和 Cu 的均匀分布,其值与理论值相似。在纳米尺度上,SR-EELS 分析检测到存在具有较低 Cu 含量的纳米片,化学上不均匀,具有比其他材料更高的 Mn 氧化态。这项工作中使用的先进表征技术允许精确识别在整体上原位生成的 Mn-Cu 系统的部分组成相。其中,不同氧化态的锰氧化物(MnO、Mn 这项工作中使用的先进表征技术允许精确识别在整体上原位生成的 Mn-Cu 系统的部分组成相。其中,不同氧化态的锰氧化物(MnO、Mn 这项工作中使用的先进表征技术允许精确识别在整体上原位生成的 Mn-Cu 系统的部分组成相。其中,不同氧化态的锰氧化物(MnO、Mn3 O 4、Mn 2 O 3 )、Mn 3 Cu 3 O 8和CuO被检测到。

更新日期:2021-06-13
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