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原位X射线吸收近边结构揭示低温CO氧化过程中氧化铁单层的化学状态。

Operando XANES Reveals the Chemical State of Iron-Oxide Monolayers During Low-Temperature CO Oxidation.

作者信息

Gajdek Dorotea, Wallander Harald J, Abbondanza Giuseppe, Harlow Gary S, Gustafson Johan, Blomberg Sara, Carlsson Per-Anders, Just Justus, Lundgren Edvin, Merte Lindsay R

机构信息

Department of Materials Science and Applied Mathematics, Malmö University, SE-205 06, Malmö, Sweden.

NanoLund, Lund University, Box 118, SE-221 00, Lund, Sweden.

出版信息

Chemphyschem. 2025 Jan 14;26(2):e202400835. doi: 10.1002/cphc.202400835. Epub 2024 Nov 20.

DOI:10.1002/cphc.202400835
PMID:39403857
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11733406/
Abstract

We have used grazing incidence X-ray absorption near edge spectroscopy (XANES) to investigate the behavior of monolayer FeO films on Pt(111) under near ambient pressure CO oxidation conditions with a total gas pressure of 1 bar. Spectra indicate reversible changes during oxidation and reduction by O and CO at 150 °C, attributed to a transformation between FeO bilayer and FeO trilayer phases. The trilayer phase is also reduced upon heating in CO+O , consistent with a Mars-van-Krevelen type mechanism for CO oxidation. At higher temperatures, the monolayer film dewets the surface, resulting in a loss of the observed reducibility. A similar iron oxide film prepared on Au(111) shows little sign of reduction or oxidation under the same conditions. The results highlight the unique properties of monolayer FeO and the importance of the Pt support in this reaction. The study furthermore demonstrates the power of grazing-incidence XAFS for in situ studies of these model catalysts under realistic conditions.

摘要

我们利用掠入射X射线吸收近边光谱（XANES）研究了在总气压为1 bar的近常压CO氧化条件下，Pt(111)上单层FeO薄膜的行为。光谱表明，在150 °C下，薄膜在被O和CO氧化和还原过程中发生了可逆变化，这归因于FeO双层和FeO三层相之间的转变。在CO + O中加热时，三层相也会被还原，这与Mars-van-Krevelen型CO氧化机理一致。在较高温度下，单层薄膜会从表面脱湿，导致观察到的还原性丧失。在相同条件下，在Au(111)上制备的类似氧化铁薄膜几乎没有还原或氧化的迹象。这些结果突出了单层FeO的独特性质以及Pt载体在该反应中的重要性。此外，该研究还证明了掠入射XAFS在实际条件下对这些模型催化剂进行原位研究的能力。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5e01/11733406/d9f95f4c43e7/CPHC-26-e202400835-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5e01/11733406/a3f94a39a6ea/CPHC-26-e202400835-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5e01/11733406/3532a0124bf4/CPHC-26-e202400835-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5e01/11733406/b2505842048c/CPHC-26-e202400835-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5e01/11733406/265d6e3f8db6/CPHC-26-e202400835-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5e01/11733406/624b72c55de3/CPHC-26-e202400835-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5e01/11733406/d9f95f4c43e7/CPHC-26-e202400835-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5e01/11733406/a3f94a39a6ea/CPHC-26-e202400835-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5e01/11733406/3532a0124bf4/CPHC-26-e202400835-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5e01/11733406/b2505842048c/CPHC-26-e202400835-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5e01/11733406/265d6e3f8db6/CPHC-26-e202400835-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5e01/11733406/624b72c55de3/CPHC-26-e202400835-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5e01/11733406/d9f95f4c43e7/CPHC-26-e202400835-g003.jpg

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本文引用的文献

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