Carbon-stabilized mesoporous MoS₂ — Structural and surface characterization with spectroscopic and catalytic tools

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• 作者：Mykola Polyakov ; Martha Poisot ; Maurits W.E. van den Berg ; Thomas Drescher ; Andriy Lotnyk ; Lorenz Kienle ; Wolfgang Bensch ; Martin Muhler ; Wolfgang Grü ; nert
• 刊名：Catalysis Communications
• 出版年：2010
• 出版时间：December 2010
• 年：2010
• 卷：12
• 期：3
• 页码：231-237
• 全文大小：892 K

文摘

Structural and surface properties of carbon-containing mesoporous MoS₂ and of a reference MoS₂ were studied with various techniques including XRD, elemental analysis, TEM, XPS, EXAFS, nitrogen physisorption, oxygen chemisorption (OCS), determination of exchangeable surface hydrogen, and kinetic study of test reactions like ethene hydrogenation and H₂/D₂ exchange. The study was made before and after use of these catalysts in the hydrodesulfurization of dibenzothiophene. The microstructure of carbon-stabilized MoS₂ is characterized by nanoslabs of ≈ 2 nm average stacking height embedded in an amorphous matrix with a very broad pore-size distribution. Thermal stress induced a collapse of the microporous structure leading to the formation of mainly mesopores. The carbon is well-distributed over the bulk, without any signature of carbide species detected neither in XPS nor in EXAFS measurements. The activity patterns of both materials (related to the OCS capacity) were similar despite the differing sulfur content, with the carbon-stabilized MoS₂ being more sulfur deficient. This suggests that the catalytic properties of the latter material were caused by near-stoichiometric MoS₂ apparently present in the nanoslabs, whereas the sulfur vacancies in the sulfur-deficient amorphous phase were blocked by strongly adsorbed carbon residues. Interestingly, the HDS reaction did not cause significant changes of the properties of the carbon-stabilized MoS₂. Conversely, the reference MoS₂ was strongly activated, in particular with respect to ethene hydrogenation, which can be explained by a pronounced sulfur loss during the HDS reaction, without significant site blockage by the coke deposited.