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用于理解和开发SOx储存催化剂的原位S K边X射线吸收光谱法。

In situ S K-edge X-ray absorption spectroscopy for understanding and developing SOx storage catalysts.

作者信息

Dathe Hendrik, Jentys Andreas, Lercher Johannes A

机构信息

Department of Chemistry, Technische Universität München, Lichtenbergstrasse 4, D-85747 Garching, Germany.

出版信息

J Phys Chem B. 2005 Nov 24;109(46):21842-6. doi: 10.1021/jp054336c.

Abstract

In situ S K-edge XANES experiments were carried out on second-generation SO(x)() trapping materials under oxidizing and reducing conditions. The experiments clearly show that the strong release of SO(2) under rich conditions at plug flow conditions is caused by the facilitated reduction of sulfite species on Pt. In the absence of Pt the sulfite species were stable under reducing conditions, while maintaining a similar total SO(2) uptake capacity. Thus, SO(x)() trapping materials without a noble metal are a clearly better option. The enhancing effect on the SO(x)() storage process of water present in the gas mixture is attributed to the formation of a higher sulfate fraction in the samples. The application of the in situ S K-edge XANES technique clearly reveals new information and insights on the behavior of the sulfur in the trapping process compared to that from the ex situ measurements and is therefore essential for designing new SO(x)() trapping materials.

摘要

在氧化和还原条件下,对第二代SO(x)捕集材料进行了原位S K边X射线吸收近边结构(XANES)实验。实验清楚地表明,在塞流条件下富氧条件下SO(2)的强烈释放是由于Pt上亚硫酸盐物种的还原促进所致。在没有Pt的情况下,亚硫酸盐物种在还原条件下是稳定的,同时保持相似的总SO(2)吸收能力。因此,不含贵金属的SO(x)捕集材料显然是更好的选择。气体混合物中存在的水对SO(x)储存过程的增强作用归因于样品中形成了更高的硫酸盐分数。与非原位测量相比,原位S K边XANES技术的应用清楚地揭示了捕集过程中硫行为的新信息和见解,因此对于设计新型SO(x)捕集材料至关重要。

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