On mechanism of formation of SBA-15/furfuryl alcohol-derived mesoporous carbon replicas and its relationship with catalytic activity in oxidative dehydrogenation of ethylbenzene

摘要

A series of CMK-3-like carbon replicas was synthesized by precipitation polycondensation of furfuryl alcohol in an aqueous slurry of SBA-15 at a polymer/SiO2 mass ratio of 0.50-2.00. Changes in textural and structural parameters of SBA-15 after polymer deposition were studied by N-2 adsorption and X-ray diffraction. Morphology of the replicas was investigated by transmission electron microscopy, while their surface composition was determined by temperature-programmed desorption and X-ray photoelectron spectroscopy. The mechanism of deposition of poly(furfuryl alcohol) (PFA) onto silica surface was elucidated. It was found that PFA accumulates in SBA-15 pores randomly; certain channels are completely filled, while others remain partially empty. The incomplete filling of mesopores results in "pseudo-CMK-3" structures featuring the bimodal porosity (the typical mesopores of CMK-3 are accompanied by broader ones formed by the coalescence of adjacent partially hollow pores). The total filling of pores with PFA leads to the formation of good-quality CMK-3. The carbon replicas exhibited the presence of abundant amounts of superficial oxygen-containing moieties. These entities are responsible for high activity of the materials in the oxidative dehydrogenation (ODH) of ethylbenzene, bringing evidence supporting the mechanism of active coke, considered as governing the catalytic performance of carbon materials in ODH of alkanes.