In Situ Probe of the Hydrogen Oxidation Reaction Intermediates on PtRu a Bimetallic Catalyst Surface by Core–Shell Nanoparticle-Enhanced Raman Spectroscopy,Nano Letters

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In Situ Probe of the Hydrogen Oxidation Reaction Intermediates on PtRu a Bimetallic Catalyst Surface by Core–Shell Nanoparticle-Enhanced Raman Spectroscopy
Nano Letters ( IF 9.6 ) Pub Date : 2022-06-14 , DOI: 10.1021/acs.nanolett.2c01744
Xiu-Mei Lin _{1,

2} , Xiao-Ting Wang ₂ , Yong-Liang Deng ₂ , Xing Chen ₂ , Hao-Ning Chen ₂ , Petar M Radjenovic ₂ , Xia-Guang Zhang ₃ , Yao-Hui Wang ₂ , Jin-Chao Dong ₂ , Zhong-Qun Tian _{2,

4} , Jian-Feng Li _{2,

4,

5,

6}

Affiliation

In situ monitoring of the evolution of intermediates and catalysts during hydrogen oxidation reaction (HOR) processes and elucidating the reaction mechanism are crucial in catalysis and energy science. However, spectroscopic information on trace intermediates on catalyst surfaces is challenging to obtain due to the complexity of interfacial environments and lack of in situ techniques. Herein, core–shell nanoparticle-enhanced Raman spectroscopy was employed to probe alkaline HOR processes on representative PtRu surfaces. Direct spectroscopic evidence of an OH_ad intermediate and RuO_x (Ru(+3)/Ru(+4)) surface oxides is simultaneously obtained, verifying that Ru doping onto Pt promotes OH_ad adsorption on the RuO_x surface to react with H_ad adsorption on the Pt surface to form H₂O. In situ Raman, XPS, and DFT results reveal that RuO_x coverage tunes the electronic structure of PtRuO_x to optimize the adsorption energy of OH_ad on catalyst surfaces, leading to an improvement in HOR activity. Our findings provide mechanistic guidelines for the rational design of HOR catalysts with high activity.

中文翻译：

核壳纳米粒子增强拉曼光谱对 PtRu 双金属催化剂表面的氢氧化反应中间体进行原位探测

在氢氧化反应 (HOR) 过程中原位监测中间体和催化剂的演变并阐明反应机理在催化和能源科学中至关重要。然而，由于界面环境的复杂性和缺乏原位技术，催化剂表面上痕量中间体的光谱信息难以获得。在此，核-壳纳米颗粒增强拉曼光谱用于探测代表性 PtRu 表面上的碱性 HOR 过程。_{同时获得了 OH ad}中间体和 RuO _x (Ru(+3)/Ru(+4)) 表面氧化物的直接光谱证据，证实了 Ru 掺杂到 Pt 上促进了 OH _{ad在 RuO}_x上的吸附表面与Pt 表面吸附的H _{ad反应形成 H}₂ O。原位拉曼、XPS 和 DFT 结果表明，RuO _x覆盖率调整了 PtRuO _x_{的电子结构，以优化 OH ad}在催化剂表面的吸附能，导致 HOR 活动的改善。我们的研究结果为合理设计高活性 HOR 催化剂提供了机理指导。

更新日期：2022-06-14

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