Substoichiometric tungsten oxide single-crystal nanosheets are successfully prepared via the exfoliation of layered tungstic acid and subsequent introduction of oxygen vacancies. The combination of different strategies, i.e., 2D-structure construction, the introduction of surface oxygen vacancies, and the creation of localized surface plasmon resonance can promote the light-harvesting performance of tungsten oxide through accumulative and synergistic effects.
Nanocrystalline Sn-Beta zeolites have been successfully prepared via an improved two-step postsynthesis strategy, which consists of creating vacant T sites with associated silanol groups by dealumination of parent H-Beta and subsequent dry impregnation of the resulting Si-Beta with organometallic dimethyltin dichloride. Characterization results from UV−vis, XPS, Raman, and 119 Sn solid-state MAS NMR reveal that most Sn species have been successfully incorporated into the framework of Beta zeolite through the postsynthesis process and exist as isolated tetrahedral Sn(IV) in open arrangement. The creation of strong Lewis acid sites upon Sn incorporation is confirmed by FTIR spectroscopy with pyridine adsorption. The Sn-Beta Lewis acid catalysts are applied in the ring-opening hydration of epoxides to the corresponding 1,2-diols under near ambient and solvent-free conditions, and remarkable activity can be obtained. The impacts of Lewis acidity, preparation parameters, and reaction conditions on the catalytic performance of Sn-Beta zeolites are discussed in detail.
Little is known on the early stages of the methanol-to-olefin (MTO) conversion over H-SAPO-34, before the steady-state with highly active polymethylbenzenium cations as most important intermediates is reached. In this work, the formation and evolution of carbenium ions during the early stages of the MTO conversion on a H-SAPO-34 model catalyst were clarified via 1 H MAS NMR and 13 C MAS NMR. Several initial species (i.e., three-ring compounds, dienes, polymethylcyclopentenyl, and polymethylcyclohexenyl cations) were, for the first time, directly verified during the MTO conversion. Their detailed evolution network was established from theoretical calculations. On the basis of these results, an olefin-based catalytic cycle is proposed to be the primary reaction pathway during the early stages of the MTO reaction over H-SAPO-34. After that, an aromatic-based cycle may be involved in the MTO conversion for long times on stream.
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