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通过X射线光电子能谱法理解金属有机框架负载的铂纳米颗粒上的一氧化碳氧化反应。

Understanding the CO Oxidation on Pt Nanoparticles Supported on MOFs by XPS.

作者信息

Vakili Reza, Gibson Emma K, Chansai Sarayute, Xu Shaojun, Al-Janabi Nadeen, Wells Peter P, Hardacre Christopher, Walton Alex, Fan Xiaolei

机构信息

School of Chemical Engineering and Analytical Science The University of Manchester Oxford Road Manchester M13 9PL UK.

School of Chemistry University of Glasgow University Avenue Glasgow G12 8QQ UK.

出版信息

ChemCatChem. 2018 Oct 9;10(19):4238-4242. doi: 10.1002/cctc.201801067. Epub 2018 Aug 13.

DOI:10.1002/cctc.201801067
PMID:31007773
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC6470863/
Abstract

Metal-organic frameworks (MOFs) are playing a key role in developing the next generation of heterogeneous catalysts. In this work, near ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) is applied to study in the CO oxidation on Pt@MOFs (UiO-67) and Pt@ZrO catalysts, revealing the same Pt surface dynamics under the stoichiometric CO/O ambient at 3 mbar. Upon the ignition at . 200 °C, the signature Pt binding energy (BE) shift towards the lower BE (from 71.8 to 71.2 eV) is observed for all catalysts, confirming metallic Pt nanoparticles (NPs) as the active phase. Additionally, the plug-flow light-off experiments show the superior activity of the Pt@MOFs catalyst in CO oxidation than the control Pt@ZrO catalyst with . 28 % drop in the light-off temperature, as well as high stability, due to their sintering-resistance feature. These results provide evidence that the uniqueness of MOFs as the catalyst supports lies in the structural confinement effect.

摘要

金属有机框架材料(MOFs)在开发下一代多相催化剂方面发挥着关键作用。在这项工作中,近常压X射线光电子能谱(NAP-XPS)被用于研究Pt@MOFs(UiO-67)和Pt@ZrO催化剂上的CO氧化反应,揭示了在3毫巴的化学计量比CO/O环境下相同的Pt表面动力学。在200 °C点火时,所有催化剂都观察到标志性的Pt结合能(BE)向较低BE(从71.8到71.2 eV)的移动,证实金属Pt纳米颗粒(NPs)为活性相。此外,活塞流起燃实验表明,Pt@MOFs催化剂在CO氧化反应中的活性优于对照Pt@ZrO催化剂,起燃温度下降了28 %,并且由于其抗烧结特性而具有高稳定性。这些结果证明了MOFs作为催化剂载体的独特性在于其结构限制效应。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/49a5/6470863/4c0c1f3d9e2e/CCTC-10-4238-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/49a5/6470863/a7699b8e7818/CCTC-10-4238-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/49a5/6470863/07389f2f9b1c/CCTC-10-4238-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/49a5/6470863/178b7e8e5155/CCTC-10-4238-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/49a5/6470863/4c0c1f3d9e2e/CCTC-10-4238-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/49a5/6470863/a7699b8e7818/CCTC-10-4238-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/49a5/6470863/07389f2f9b1c/CCTC-10-4238-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/49a5/6470863/178b7e8e5155/CCTC-10-4238-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/49a5/6470863/4c0c1f3d9e2e/CCTC-10-4238-g004.jpg

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