丙烷脱氢过程中 Rh/Al2O3 的表面动力学

IF 15.7 1区 化学 Q1 CHEMISTRY, APPLIED
Shuyi Li, Changle Mu, Nianqiu He, Jie Xu, Yanping Zheng, Mingshu Chen
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引用次数: 0

摘要

异相催化剂的表面结构对催化性能有很大影响,尤其是对结构敏感的反应。在本研究中,我们采用了低能离子散射光谱、X 射线光电子能谱和以 CO 为探针的傅立叶变换红外光谱(CO-FTIR)等表面技术来研究用于丙烷脱氢(PDH)的 Rh/Al2O3 催化剂的表面动力学。我们在 Rh/Al2O3 催化剂上观察到了明显的 PDH 诱导过程,其特点是丙烷转化率、甲烷和丙烯选择性的显著变化。这些变化归因于大量焦炭的形成。畸变校正高角度环形暗场扫描透射电子显微镜)和 CO-FTIR 揭示了表面上 Rh 纳米颗粒、团簇和单原子的共存。通过各种动态准原位表征,我们发现焦炭优先覆盖了 Rh 簇,从而抑制了 C-C 键的断裂和甲烷的形成。同时,Rh 单原子受焦炭覆盖的影响较小,仍作为 PDH 的活性和选择性位点暴露在外,有利于丙烯的生成。这项研究强调了 PDH 对 Rh 物种大小的敏感性,孤立的 Rh 单原子可促进丙烯的形成。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Surface dynamics of Rh/Al2O3 during propane dehydrogenation

The surface structures of heterogeneous catalysts significantly impact catalytic performance, especially for structure-sensitive reactions. In this study, we employed surface techniques such as low-energy ion scattering spectroscopy, X-ray photoelectron spectroscopy, and Fourier transform infrared spectroscopy with CO as a probe (CO-FTIR) to investigate the surface dynamics of Rh/Al2O3 catalysts for propane dehydrogenation (PDH). We observed a notable induction process for PDH on Rh/Al2O3 catalysts, marked by significant variations in propane conversion, methane, and propylene selectivities. These changes were attributed to substantial coke formation. Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy) and CO-FTIR revealed the coexistence of Rh nanoparticles, clusters, and single atoms on the surface. Through various dynamic quasi in-situ characterizations, we found that coke preferentially covered Rh clusters, thereby inhibiting C–C bond breaking and methane formation. Meanwhile, Rh single atoms were less affected by coke coverage and remained exposed as active and selective sites for PDH, favoring propylene production. This work underscores the sensitivity of PDH to the sizes of Rh species, with isolated Rh single atoms promoting propylene formation.

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来源期刊
Chinese Journal of Catalysis
Chinese Journal of Catalysis 工程技术-工程:化工
CiteScore
25.80
自引率
10.30%
发文量
235
审稿时长
1.2 months
期刊介绍: The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.
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