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钆掺杂二氧化铈模型体系在还原气氛中的硫中毒行为

The Sulphur Poisoning Behaviour of Gadolinia Doped Ceria Model Systems in Reducing Atmospheres.

作者信息

Gerstl Matthias, Nenning Andreas, Iskandar Riza, Rojek-Wöckner Veronika, Bram Martin, Hutter Herbert, Opitz Alexander Karl

机构信息

Institute of Chemical Technologies and Analytics, TU Wien, Getreidemarkt 9/164-EC, Vienna A-1060, Austria.

Christian Doppler Laboratory for Interfaces in Metal-Supported Electrochemical Energy Converters, Getreidemarkt 9/164-EC, Vienna 1060, Austria.

出版信息

Materials (Basel). 2016 Aug 2;9(8):649. doi: 10.3390/ma9080649.

DOI:10.3390/ma9080649
PMID:28773771
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC5509099/
Abstract

An array of analytical methods including surface area determination by gas adsorption using the Brunauer, Emmett, Teller (BET) method, combustion analysis, XRD, ToF-SIMS, TEM and impedance spectroscopy has been used to investigate the interaction of gadolinia doped ceria (GDC) with hydrogen sulphide containing reducing atmospheres. It is shown that sulphur is incorporated into the GDC bulk and might lead to phase changes. Additionally, high concentrations of silicon are found on the surface of model composite microelectrodes. Based on these data, a model is proposed to explain the multi-facetted electrochemical degradation behaviour encountered during long term electrochemical measurements. While electrochemical bulk properties of GDC stay largely unaffected, the surface polarisation resistance is dramatically changed, due to silicon segregation and reaction with adsorbed sulphur.

摘要

一系列分析方法，包括使用布鲁瑙尔-埃米特-特勒（BET）法通过气体吸附测定表面积、燃烧分析、X射线衍射（XRD）、飞行时间二次离子质谱（ToF-SIMS）、透射电子显微镜（TEM）和阻抗谱，已被用于研究掺杂氧化钆的二氧化铈（GDC）与含硫化氢的还原气氛之间的相互作用。结果表明，硫掺入到GDC体相中，并可能导致相变。此外，在模型复合微电极表面发现了高浓度的硅。基于这些数据，提出了一个模型来解释长期电化学测量过程中遇到的多方面电化学降解行为。虽然GDC的电化学体相性质在很大程度上未受影响，但由于硅的偏析以及与吸附硫的反应，表面极化电阻发生了显著变化。

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