Surface dynamics of Rh/Al2O3 during propane dehydrogenation

被引：4

作者：

Li, Shuyi ^{[1
]}

Mu, Changle ^{[1
]}

He, Nianqiu ^{[1
]}

Xu, Jie ^{[1
]}

Zheng, Yanping ^{[1
]}

Chen, Mingshu ^{[1
]}

机构：

[1] Xiamen Univ, Coll Chem & Chem Engn, Dept Chem, State Key Lab Phys Chem Solid Surfaces, Xiamen 361005, Fujian, Peoples R China

来源：

CHINESE JOURNAL OF CATALYSIS | 2024年 / 62卷

基金：

中国国家自然科学基金;

关键词：

Propane dehydrogenation; Rhodium; Coke; Single atom; Quasi in - situ spectroscopy; Surface dynamics; SINGLE-ATOM CATALYST; LIGHT ALKANES; ADSORPTION; PLATINUM; METALS; CO; HYDROFORMYLATION; NANOPARTICLES; NANOSHEETS; GRAPHENE;

D O I：

10.1016/S1872-2067(24)60063-X

中图分类号：

O69 [应用化学];

学科分类号：

081704 ;

摘要：

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 2 O 3 catalysts for propane dehydrogenation (PDH). We observed a notable induction process for PDH on Rh/Al2O3 2 O 3 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 - 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. (c) 2024, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.

引用

页码：145 / 155

页数：11

共 65 条

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