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氟化程度对铁基催化剂中氧还原反应限制过程的影响：关于高铁酸钡对称薄膜的模型研究

On the Impact of the Degree of Fluorination on the ORR Limiting Processes within Iron Based Catalysts: A Model Study on Symmetrical Films of Barium Ferrate.

作者信息

Wollstadt Stephan, Clemens Oliver

机构信息

Fachgebiet Materialdesign durch Synthese, Institut für Materialwissenschaft, Technical University of Darmstadt, 64287 Darmstadt, Germany.

Institut für Nanotechnologie, Karlsruher Institut für Technologie, Hermann-von-Helmholtz-Platz 1, 76344 Eggenstein Leopoldshafen, Germany.

出版信息

Materials (Basel). 2020 Jun 3;13(11):2532. doi: 10.3390/ma13112532.

DOI:10.3390/ma13112532
PMID:32503126
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC7321444/
Abstract

In this study, symmetrical films of BaFeO, BaFeOF and BaFeOF were synthesized and the oxygen uptake and conduction was investigated by high temperature impedance spectroscopy under an oxygen atmosphere. The data were analyzed on the basis of an impedance model designed for highly porous mixed ionic electronic conducting (MIEC) electrodes. Variable temperature X-ray diffraction experiments were utilized to estimate the stability window of the oxyfluoride compounds, which yielded a degradation temperature for BaFeOF of 590 °C and a decomposition temperature for BaFeOF of 710 °C. The impedance study revealed a significant change of the catalytic behavior in dependency of the fluorine content. BaFeO revealed a bulk-diffusion limited process, while BaFeOF appeared to exhibit a fast bulk diffusion and a utilization region δ larger than the electrode thickness L (8 μm). In contrast, BaFeOF showed very area specific resistances due to the lack of oxygen vacancies. The activation energy for the uptake and conduction process of oxygen was found to be 0.07/0.29 eV (temperature range-dependent), 0.33 eV and 0.67 eV for BaFeO, BaFeOF and BaFeOF, respectively.

摘要

在本研究中，合成了BaFeO、BaFeOF和BaFeOF的对称薄膜，并在氧气气氛下通过高温阻抗谱研究了氧的吸收和传导。基于为高度多孔混合离子电子导电（MIEC）电极设计的阻抗模型对数据进行了分析。利用变温X射线衍射实验来估计氟氧化物化合物的稳定性窗口，得出BaFeOF的降解温度为590℃，BaFeOF的分解温度为710℃。阻抗研究表明，催化行为随氟含量的变化有显著改变。BaFeO显示出体扩散受限过程，而BaFeOF似乎表现出快速的体扩散，且利用区域δ大于电极厚度L（8μm）。相比之下，BaFeOF由于缺乏氧空位而显示出非常高的面积比电阻。发现BaFeO、BaFeOF和BaFeOF的氧吸收和传导过程的活化能分别为0.07/0.29eV（取决于温度范围）、0.33eV和0.67eV。

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本文引用的文献

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Anion Doping of Ferromagnetic Thin Films of LaSrMnO via Topochemical Fluorination.通过拓扑化学氟化对LaSrMnO铁磁薄膜进行阴离子掺杂
Materials (Basel). 2018 Jul 13;11(7):1204. doi: 10.3390/ma11071204.
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Proton Conduction in Grain-Boundary-Free Oxygen-Deficient BaFeO Thin Films.
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Materials (Basel). 2017 Dec 29;11(1):52. doi: 10.3390/ma11010052.
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Magnetic interactions in cubic-, hexagonal- and trigonal-barium iron oxide fluoride, BaFeO2F.
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