Direct In Situ Raman Spectroscopic Evidence of Oxygen Reduction Reaction Intermediates at High-Index Pt(hkl) Surfaces,Journal of the American Chemical Society

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Direct In Situ Raman Spectroscopic Evidence of Oxygen Reduction Reaction Intermediates at High-Index Pt(hkl) Surfaces
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2019-12-30 , DOI: 10.1021/jacs.9b12803
Jin-Chao Dong ₁ , Min Su ₁ , Valentín Briega-Martos ₂ , Lang Li ₁ , Jia-Bo Le ₁ , Petar Radjenovic ₁ , Xiao-Shun Zhou ₃ , Juan Miguel Feliu ₂ , Zhong-Qun Tian ₁ , Jian-Feng Li ₁

Affiliation

The study of the oxygen reduction reaction (ORR) at high-index Pt(hkl) single crystal surfaces has received considerable interest due to their well-ordered, typical atomic structures and superior catalytic activities. However, it is difficult to obtain direct spectral evidence of ORR intermediates during reaction processes, especially at high-index Pt(hkl) surfaces. Herein, in situ Raman spectroscopy has been employed to investigate ORR processes at high-index Pt(hkl) surfaces containing the [011 ̅] crystal zone - i.e. Pt(211) and Pt(311). Through control and isotope substitution experiments, we successfully obtained in situ spectral evidences of OH and OOH at Pt(211) and Pt(311) surfaces. After detailed analysis based on the Raman spectra, it was deduced that the difference in adsorption of OOH at high-index surfaces has a significant effect on the ORR activity. This research illuminates and deepens the understanding of the ORR mechanism on high-index Pt(hkl) surfaces and provides theoretical guidance for the rational design of high activity ORR catalysts.

中文翻译：

氧还原反应中间体在高指数 Pt(hkl) 表面的直接原位拉曼光谱证据

高指数 Pt(hkl) 单晶表面氧还原反应 (ORR) 的研究由于其有序、典型的原子结构和优异的催化活性而受到广泛关注。然而，在反应过程中很难获得 ORR 中间体的直接光谱证据，尤其是在高指数 Pt(hkl) 表面。在此，原位拉曼光谱已被用于研究包含 [011 ̅] 晶区的高指数 Pt(hkl) 表面的 ORR 过程 - 即 Pt(211) 和 Pt(311)。通过对照和同位素取代实验，我们成功地获得了 Pt(211) 和 Pt(311) 表面 OH 和 OOH 的原位光谱证据。根据拉曼光谱进行详细分析后，据推断，OOH 在高指数表面的吸附差异对 ORR 活性有显着影响。该研究阐明并加深了对高指数Pt(hkl)表面ORR机理的理解，为合理设计高活性ORR催化剂提供了理论指导。

更新日期：2019-12-30

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