Strong Metal–Support Interaction Mechanisms of Rh Supports in the CO–NO Reaction: Rh/Rh2O3 Interconversion in Promoting NO Dissociation and CO2 Generation,The Journal of Physical Chemistry C

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Strong Metal–Support Interaction Mechanisms of Rh Supports in the CO–NO Reaction: Rh/Rh2O3 Interconversion in Promoting NO Dissociation and CO2 Generation
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2022-10-16 , DOI: 10.1021/acs.jpcc.2c03808
Hiroki Nakayama _{1,

2} , Makoto Nagata ₁ , Toshihisa Tomie ₃ , Tomoaki Ishitsuka ₄ , Nobuyuki Matsubayashi ₄ , Yukihiro Shimizu ₂

Affiliation

In precious metal catalysts, the interaction between the precious metal and oxide support, denoted the strong metal–support interaction (SMSI), is closely related to catalytic activity. However, there are few studies of the effects of the SMSI on catalytic activity and the properties of catalytic active sites. Therefore, the valence band spectra of Rh catalysts on various supports were measured using X-ray photoelectron spectroscopy and a more surface-sensitive experimental technique, extreme ultraviolet-excited photoelectron spectroscopy. There is a good correlation between the catalytic activities of these Rh catalysts in the CO–NO reaction and the energy difference between the peaks of the Rh metal and Rh₂O₃ components in the valence band spectra. The cause of the difference in the activities of the Rh catalysts on various supports is analyzed based on density functional theory calculations using two models: Rh metal/support and Rh₂O₃/support. Rh metal and Rh₂O₃ contribute to the activity of the CO–NO reaction. NO dissociation is promoted on the Rh metal surface, where the SMSI induces enhanced oxygen adsorption. Conversely, CO oxidation is promoted on the Rh₂O₃ surface, where the oxygen bonding is weakened by the SMSI. This study reveals the critical mechanisms whereby SMSIs contribute to oxygen-mediated reactions on catalyst surfaces.

中文翻译：

Rh 载体在 CO-NO 反应中的强金属-载体相互作用机制：Rh/Rh2O3 相互转化促进 NO 解离和 CO2 生成

在贵金属催化剂中，贵金属与氧化物载体之间的相互作用，称为强金属-载体相互作用（SMSI），与催化活性密切相关。然而，关于SMSI对催化活性和催化活性位点性质的影响的研究很少。因此，使用 X 射线光电子能谱和对表面更敏感的实验技术——极紫外激发光电子能谱测量了各种载体上 Rh 催化剂的价带光谱。_{这些Rh催化剂在CO-NO反应中的催化活性与Rh金属和Rh 2} O ₃峰之间的能量差之间存在良好的相关性价带光谱中的成分。基于密度泛函理论计算，使用Rh金属/载体和Rh ₂ O ₃ /载体两种模型分析了Rh催化剂在各种载体上活性差异的原因。Rh金属和Rh ₂ O ₃有助于CO-NO反应的活性。在 Rh 金属表面促进 NO 解离，其中 SMSI 诱导增强的氧吸附。相反，CO 氧化在 Rh ₂ O ₃表面被促进，其中氧键被 SMSI 削弱。这项研究揭示了 SMSIs 有助于催化剂表面上的氧介导反应的关键机制。

更新日期：2022-10-16

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