In Situ Raman Observation of Oxygen Activation and Reaction at Platinum–Ceria Interfaces during CO Oxidation,Journal of the American Chemical Society

当前位置： X-MOL 学术 › J. Am. Chem. Soc. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

In Situ Raman Observation of Oxygen Activation and Reaction at Platinum–Ceria Interfaces during CO Oxidation
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2021-09-20 , DOI: 10.1021/jacs.1c04590
Di-Ye Wei ₁ , Mu-Fei Yue ₁ , Si-Na Qin ₁ , Sa Zhang ₁ , Yuan-Fei Wu ₁ , Ge-Yang Xu ₁ , Hua Zhang ₁ , Zhong-Qun Tian ₁ , Jian-Feng Li _{1,

2}

Affiliation

Understanding the fundamental insights of oxygen activation and reaction at metal–oxide interfaces is of significant importance yet remains a major challenge due to the difficulty in in situ characterization of active oxygen species. Herein, the activation and reaction of molecular oxygen during CO oxidation at platinum–ceria interfaces has been in situ explored using surface-enhanced Raman spectroscopy (SERS) via a borrowing strategy, and different active oxygen species and their evolution during CO oxidation at platinum–ceria interfaces have been directly observed. In situ Raman spectroscopic evidence with isotopic exchange experiments demonstrate that oxygen is efficiently dissociated to chemisorbed O on Pt and lattice Ce–O species simultaneously at interfacial Ce³⁺ defect sites under CO oxidation, leading to a much higher activity at platinum–ceria interfaces compared to that at Pt alone. Further in situ time-resolved SERS studies and density functional theory simulations reveal a more efficient molecular pathway through the reaction between adsorbed CO and chemisorbed Pt–O species transferred from the interfaces. This work deepens the fundamental understandings on oxygen activation and CO oxidation at metal–oxide interfaces and offers a sensitive technique for the in situ characterization of oxygen species under working conditions.

中文翻译：

CO氧化过程中铂-二氧化铈界面氧活化和反应的原位拉曼观察

了解金属-氧化物界面处氧活化和反应的基本见解具有重要意义，但由于活性氧物质的原位表征困难，因此仍然是一个重大挑战。在此，通过借用策略使用表面增强拉曼光谱 (SERS) 原位探索了铂 - 氧化铈界面处 CO 氧化过程中分子氧的活化和反应，以及不同的活性氧物种及其在铂 - 氧化还原过程中的演变已直接观察到氧化铈界面。同位素交换实验的原位拉曼光谱证据表明，氧在界面 Ce ³⁺处同时有效地分解为化学吸附在 Pt 和晶格 Ce-O 物质上的 OCO氧化下的缺陷位点，导致铂-二氧化铈界面的活性比单独的铂高得多。进一步的原位时间分辨 SERS 研究和密度泛函理论模拟揭示了通过吸附的 CO 和从界面转移的化学吸附的 Pt-O 物种之间的反应的更有效的分子途径。这项工作加深了对金属-氧化物界面氧活化和 CO 氧化的基本理解，并为在工作条件下原位表征氧物质提供了一种灵敏的技术。

更新日期：2021-09-29

点击分享查看原文

点击收藏

阅读更多本刊最新论文本刊介绍/投稿指南11