Revealing Dynamics and Competitive Mechanism of Gas-Induced Surface Segregation of PdFe0.08 Dilute Alloy by Multi-Dimensional Imaging.

IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL The Journal of Physical Chemistry Letters Pub Date : 2024-11-15 DOI:10.1021/acs.jpclett.4c02903
Yafeng Zhang, Hong Li, Fang Liu, Mengwei Li, Yong Zhang, Jinming Cai, Yangsheng Li, Fan Yang, Feng Yin, Junling Lu, Tao Zhang, Bing Yang
{"title":"Revealing Dynamics and Competitive Mechanism of Gas-Induced Surface Segregation of PdFe<sub>0.08</sub> Dilute Alloy by Multi-Dimensional Imaging.","authors":"Yafeng Zhang, Hong Li, Fang Liu, Mengwei Li, Yong Zhang, Jinming Cai, Yangsheng Li, Fan Yang, Feng Yin, Junling Lu, Tao Zhang, Bing Yang","doi":"10.1021/acs.jpclett.4c02903","DOIUrl":null,"url":null,"abstract":"<p><p>The restructuring of dilute alloys under gas environments has shown a great impact on their catalytic performance due to intriguing structural sensitivity, but the structural dynamics and underlying mechanism remains elusive. Herein, we directly resolved the distinct dynamic behaviors of PdFe<sub>0.08</sub> dilute alloys under CO or O<sub>2</sub> environment by multidimensional imaging. The stronger binding of gaseous CO with Fe atoms stimulates Fe segregation out of the PdFe<sub>0.08</sub>, resulting in 3D growth of Fe islands, whereas the dissociative adsorption of O<sub>2</sub> results in 2D layer-by-layer growth of segregated FeO as encapsulation overlayers that bind strongly with the Pd surface underneath. Such varied structures remarkably tune the catalytic activity for CO oxidation, showing a considerably high activity for a CO-treated sample. Our results reveal the competitive mechanism between adsorbate-metal and metal-metal interaction for gas-induced surface segregation, which should be highly considered for the rational design of dilute alloys with dynamically tuned structure and reactivity.</p>","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":4.8000,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"The Journal of Physical Chemistry Letters","FirstCategoryId":"1","ListUrlMain":"https://doi.org/10.1021/acs.jpclett.4c02903","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0

Abstract

The restructuring of dilute alloys under gas environments has shown a great impact on their catalytic performance due to intriguing structural sensitivity, but the structural dynamics and underlying mechanism remains elusive. Herein, we directly resolved the distinct dynamic behaviors of PdFe0.08 dilute alloys under CO or O2 environment by multidimensional imaging. The stronger binding of gaseous CO with Fe atoms stimulates Fe segregation out of the PdFe0.08, resulting in 3D growth of Fe islands, whereas the dissociative adsorption of O2 results in 2D layer-by-layer growth of segregated FeO as encapsulation overlayers that bind strongly with the Pd surface underneath. Such varied structures remarkably tune the catalytic activity for CO oxidation, showing a considerably high activity for a CO-treated sample. Our results reveal the competitive mechanism between adsorbate-metal and metal-metal interaction for gas-induced surface segregation, which should be highly considered for the rational design of dilute alloys with dynamically tuned structure and reactivity.

Abstract Image

查看原文
分享 分享
微信好友 朋友圈 QQ好友 复制链接
本刊更多论文
通过多维成像揭示 PdFe0.08 稀合金气体诱导表面偏析的动力学和竞争机制
稀合金在气体环境下的结构重组因其结构敏感性而对其催化性能产生了巨大影响,但其结构动力学及其内在机理仍然难以捉摸。在此,我们通过多维成像直接解析了 PdFe0.08 稀合金在 CO 或 O2 环境下的不同动态行为。气态 CO 与铁原子的较强结合刺激了铁从 PdFe0.08 中离析出来,导致铁岛的三维生长,而 O2 的离解吸附则导致离析的 FeO 作为封装覆盖层的二维逐层生长,并与下面的 Pd 表面紧密结合。这种不同的结构显著地调整了 CO 氧化的催化活性,在 CO 处理过的样品中显示出相当高的活性。我们的研究结果揭示了气体诱导的表面偏析中吸附金属与金属之间以及金属与金属之间相互作用的竞争机制,在合理设计具有动态调节结构和反应活性的稀合金时应高度重视这一点。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
求助全文
约1分钟内获得全文 去求助
来源期刊
The Journal of Physical Chemistry Letters
The Journal of Physical Chemistry Letters CHEMISTRY, PHYSICAL-NANOSCIENCE & NANOTECHNOLOGY
CiteScore
9.60
自引率
7.00%
发文量
1519
审稿时长
1.6 months
期刊介绍: The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.
期刊最新文献
Signature of Proton–Hole Transfer in Hydrogen-Bonded Solids at 10 K Cu-Supported ZnO under Conditions of CO2 Reduction to Methanol: Why 0.2 ML Coverage? Ferroelectric, Switchable Dielectric and Nonlinear Optical Properties in Inorganic-Organic Lead-Free 1D Hybrids Based on Bi(III) and Azetidine: (C3NH8)2[BiCl5], (C3NH8)2[BiBr5]. Predicting Long-Term Stability from Short-Term Measurement: Insights from Modeling Degradation in Perovskite Solar Cells during Voltage Scans and Impedance Spectroscopy. Revealing Dynamics and Competitive Mechanism of Gas-Induced Surface Segregation of PdFe0.08 Dilute Alloy by Multi-Dimensional Imaging.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
已复制链接
已复制链接
快去分享给好友吧!
我知道了
×
扫码分享
扫码分享
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1