Dynamics of CeO2-supported Pt nanoparticles in CO oxidation reaction revealed by millisecond time-resolved HERFD-XANES spectroscopy†

IF 4.2 3区化学 Q2 CHEMISTRY, PHYSICAL

Catalysis Science & Technology Pub Date : 2025-02-21 DOI:10.1039/d4cy01406e

Junya Ohyama , Mizuki Sato , Masayuki Tsushida , Keisuke Awaya , Masato Machida , Tomoya Uruga , Kotaro Higashi

{"title":"Dynamics of CeO2-supported Pt nanoparticles in CO oxidation reaction revealed by millisecond time-resolved HERFD-XANES spectroscopy†","authors":"Junya Ohyama , Mizuki Sato , Masayuki Tsushida , Keisuke Awaya , Masato Machida , Tomoya Uruga , Kotaro Higashi","doi":"10.1039/d4cy01406e","DOIUrl":null,"url":null,"abstract":"<div><div>The dynamics of CeO<sub>2</sub>-supported 1.5 nm Pt nanoparticles (Pt/CeO<sub>2</sub>) during catalysis for CO oxidation at 50 °C were observed. High-energy resolution fluorescence-detected (HERFD) Pt L<sub>3</sub>-edge X-ray absorption near-edge structure (XANES) spectroscopy with millisecond time resolution was used for this observation. A series of time-resolved spectra of Pt/CeO<sub>2</sub> during CO oxidation were fitted by linear combinations of spectra corresponding to bare, CO-adsorbed, and surface-oxidised Pt nanoparticles. The analysis revealed that after O<sub>2</sub> pulse injection into CO-adsorbed Pt nanoparticles, all adsorbed CO was oxidised within 0.5 s, forming a bare Pt surface. Subsequently, the bare Pt surface was oxidised at a much slower rate, approximately 10 s, compared with the oxidation of adsorbed CO. These findings demonstrate the utility of time-resolved HERFD-XANES spectroscopy in studying catalytic processes. This reveals variations in the Pt surface state and the kinetics of CO and Pt oxidation on Pt/CeO<sub>2</sub> during the CO oxidation reaction.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 8","pages":"Pages 2544-2550"},"PeriodicalIF":4.2000,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Catalysis Science & Technology","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/org/science/article/pii/S2044475325001200","RegionNum":3,"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 dynamics of CeO₂-supported 1.5 nm Pt nanoparticles (Pt/CeO₂) during catalysis for CO oxidation at 50 °C were observed. High-energy resolution fluorescence-detected (HERFD) Pt L₃-edge X-ray absorption near-edge structure (XANES) spectroscopy with millisecond time resolution was used for this observation. A series of time-resolved spectra of Pt/CeO₂ during CO oxidation were fitted by linear combinations of spectra corresponding to bare, CO-adsorbed, and surface-oxidised Pt nanoparticles. The analysis revealed that after O₂ pulse injection into CO-adsorbed Pt nanoparticles, all adsorbed CO was oxidised within 0.5 s, forming a bare Pt surface. Subsequently, the bare Pt surface was oxidised at a much slower rate, approximately 10 s, compared with the oxidation of adsorbed CO. These findings demonstrate the utility of time-resolved HERFD-XANES spectroscopy in studying catalytic processes. This reveals variations in the Pt surface state and the kinetics of CO and Pt oxidation on Pt/CeO₂ during the CO oxidation reaction.

Abstract Image

查看原文本刊更多论文

毫秒级时间分辨 HERFD-XANES 光谱揭示 CeO2-supported Pt 纳米粒子在 CO 氧化反应中的动力学特性†。

观察了负载CeO2的1.5 nm Pt纳米粒子（Pt/CeO2）在50℃下催化CO氧化的动力学过程。采用毫秒时间分辨率的高能分辨率荧光检测（HERFD） Pt l3边缘x射线吸收近边缘结构（XANES）光谱进行观察。利用裸Pt纳米粒子、CO-吸附Pt纳米粒子和表面氧化Pt纳米粒子对应的线性组合，拟合了CO氧化过程中Pt/CeO2的一系列时间分辨光谱。分析表明，在CO- Pt纳米颗粒中注入O2脉冲后，吸附的CO在0.5 s内全部氧化，形成裸Pt表面。随后，裸Pt表面的氧化速度比吸附CO的氧化速度要慢得多，约为10 s。这些发现证明了时间分辨HERFD-XANES光谱在研究催化过程中的实用性。这揭示了CO氧化反应过程中Pt表面状态的变化以及CO和Pt在Pt/CeO2上氧化的动力学。

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分钟内获得全文求助全文

来源期刊

Catalysis Science & Technology CHEMISTRY, PHYSICAL-

CiteScore

8.70

自引率

6.00%

发文量

587

审稿时长

1.5 months

期刊介绍： A multidisciplinary journal focusing on cutting edge research across all fundamental science and technological aspects of catalysis. Editor-in-chief: Bert Weckhuysen Impact factor: 5.0 Time to first decision (peer reviewed only): 31 days