Abstract
Small amounts of nearly 2-nm Pd nanoparticles (0.01–0.03 wt.%) were deposited onto the surface of the ZSM-5 and BEA zeolites by laser electrodispersion. Materials thus prepared were studied by low-temperature nitrogen adsorption, thermo-programmed desorption of ammonia, transmission electron microscopy, and X-ray photoelectron spectroscopy. They were also tested in total catalytic oxidation of CO and CH4. It was demonstrated that the oxidation state of Pd and the character of distribution of isolated metal particles or their aggregates over the external surface or in the bulk of the zeolite is affected by the palladium content and by the zeolite nature. The activity of the Pd/ZSM-5 catalysts decreases with increasing Si/Al ratio of the zeolite and depends on the oxidation state of the metal. In the most active catalysts 65–75% of Pd occur as metal, whereas 35–25% make up oxidized palladium. The oxidation of carbon monoxide on the ZSM-5 catalyst (Si/Al = 15, 0.01 wt.% Pd) whose surface is uniformly covered with isolated Pd nanoparticles begins at 90 °C, which is 70–80 °C lower compared to CO oxidation on other Pd-modified ZSM-5 and BEA zeolites containing aggregates of palladium nanoparticles.
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Funding
The catalysts were synthesized by LED within the framework of the State Assignment to the Ioff e Physico-Technical Institute, Russian Academy of Sciences (Project No. 0040-2014-0010). The physicochemical properties of materials were analyzed within the framework of the State Assignment to the Lomonosov Moscow State University (Project No. AAAA-A21- 121011590090-7). Catalytic tests were performed within the framework of the State Assignment to the Semenov Federal Research Center for Chemical Physics, Russian Academy of Sciences (Project No. 0082-2019-0011 “Fundamental Laws of Heterogeneous and Homogeneous Catalysis”). Structural studies were carried out using the equipment purchased within the framework of the Lomonosov Moscow State University Development Program.
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No human or animal subjects were used in this research.
The authors declare no competing interests.
Based on the materials of the XXXIII Symposium “Modern Chemical Physics” (September 24–October 4, 2021, Tuapse, Russia).
Published in Russian in Izvestiya Akademii Nauk. Seriya Khimicheskaya, No. 6, pp. 1179–1193, June, 2022.
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Rostovshchikova, T.N., Nikolaev, S.A., Krotova, I.N. et al. ZSM-5 and BEA zeolites modified with Pd nanoparticles by laser electrodispersion. The structure and catalytic activity in CO and CH4 oxidation. Russ Chem Bull 71, 1179–1193 (2022). https://doi.org/10.1007/s11172-022-3519-x
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DOI: https://doi.org/10.1007/s11172-022-3519-x