Citation: ZHENG Fang-Fang, LI Qian, ZHANG Hong, WENG Wei-Zheng, YI Xiao-Dong, ZHENG Yan-Ping, HUANG Chuan-Jing, WAN Hui-Lin. Preparation and Characterization of Sinter-Resistant Rh-Sm₂O₃/SiO₂ Catalyst and Its Performance for Partial Oxidation of Methane to Syngas[J]. Acta Physico-Chimica Sinica, ;2017, 33(8): 1689-1698. doi: 10.3866/PKU.WHXB201704243 shu

Preparation and Characterization of Sinter-Resistant Rh-Sm₂O₃/SiO₂ Catalyst and Its Performance for Partial Oxidation of Methane to Syngas

State Key Laboratory of Physical Chemistry of Solid State Surfaces, National Engineering Laboratory for Green Chemical Productions of Alcohols, Ethers and Esters, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian Province, P. R. China

Received Date: 21 February 2017
Revised Date: 7 April 2017

Fund Project: The project was supported by the National Key Basic Research Program of China (2013CB933102), National Natural Science Foundation of China (21473144, 21373168), National Talent Development of Basic Research Program of China (J1310024) and Program for Innovative Research Team in University, China (IRT_14R31).

Rh/SiO₂ and Rh-Sm₂O₃/SiO₂ catalysts were synthesized by the conventional impregnation method using rhodium acetylacetonate (Rh(acac)₃) and samarium acetylacetonate (Sm(acac)₃) as precursors. The preparation and catalytic properties, as well as the interaction between Rh and Sm₂O₃, were characterized in detail by in situ infrared spectroscopy (IR), thermogravimetric analysis (TG), N₂ physisorption (Brunauer-Emmett-Teller (BET) method), X-ray powder diffraction (XRD), transmission electron microscopy (TEM), temperature-programmed reduction (H₂-TPR) and X-ray photoelectron spectroscopy (XPS). The performance of the catalysts for the partial oxidation of methane (POM) to syngas was also investigated. The results showed that a sinter-resistant Rh-Sm₂O₃/SiO₂ catalyst with an average Rh particle size of ~2.3 nm could be synthesized using the conventional impregnation method with Rh(acac)₃ and Sm(acac)₃ as precursors. The surface silanol groups of SiO₂ acted as the centers to interact with M(acac)₃ (M=Rh, Sm) molecules when SiO₂ was impregnated in the M(acac)₃ solution, leading to the formation of a hydrogen-bonded M(acac)₃ layer on the SiO₂ surface. In this experiment, the monolayer coverage of Sm(acac)₃ on the SiO₂ surface was equal to a Sm(acac)₃ loading (mass fraction) of approximately 31%, which in turn corresponded to a Sm₂O₃ loading of approximately 15%. When a Sm(acac)₃/SiO₂ sample with Sm(acac)₃ loading below 31% was heated in air to approximately 360℃, the monolayer Sm(acac)₃ species decomposed into highly dispersed Sm₂O₃ species on the SiO₂ surface, which displayed superior stability against sintering at high temperature. No aggregation of the Sm₂O₃ species was observed even when the sample was heated to 800℃ in air. The strong interaction between the highly dispersed Sm₂O₃ and Rh plays a key role in increasing the dispersion of Rh species in the catalyst and preventing the Rh species from sintering under high temperature conditions. This factor should also be responsible for the superior activity and stability of the Rh-Sm₂O₃/SiO₂ catalyst with extremely low Rh loading for the catalytic partial oxidation of methane to syngas.
- Rh-Sm₂O₃/SiO₂,
- Rh(acac)₃,
- Sm(acac)₃,
- Sinter-resistant,
- Partial oxidation of methane,
- Syngas
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Preparation and Characterization of Sinter-Resistant Rh-Sm₂O₃/SiO₂ Catalyst and Its Performance for Partial Oxidation of Methane to Syngas