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dc.contributor.authorWang, Zichun
dc.contributor.authorLing, Huajuan
dc.contributor.authorShi, Jeffrey
dc.contributor.authorStampfl, Catherine
dc.contributor.authorYu, Aibing
dc.contributor.authorHunger, Michael
dc.contributor.authorHuang, Jun
dc.date.accessioned2021-01-22T02:04:42Z
dc.date.available2021-01-22T02:04:42Z
dc.date.issued2018en_AU
dc.identifier.urihttps://hdl.handle.net/2123/24355
dc.description.abstractUsing solid acid catalysts to replace liquid acids in the liquid-phase Beckmann rearrangement of cyclohexanone oxime (CHO) into ɛ-caprolactam (CPL) is crucial for the environmentally friendly production of synthetic fibers, such as Nylon-6. In this work, we prepared aluminum-containing MCM-41 catalysts under ultrasonic irradiation with various Si/Al ratios for this purpose. Quantitative 1H MAS NMR investigations show that ultrasonic irradiation significantly promotes the formation of active Brønsted acid sites (BAS) on the [Al]MCM-41 catalysts up to 8 times higher than those prepared at the same conditions without ultrasonic irradiation, and up to 12 times higher BAS density than those reported in the literatures. The catalytic performance of [Al]MCM-41 catalysts can be strongly improved with increasing the BAS density, particularly to the ratio of BAS/(weakly acidic SiOH groups). Moreover, [Al]MCM-41 catalysts dehydrated at 393 K obtained two time higher CHO conversion and CPL yield than that dehydrated at 473 K. Hydrogen-bonded water molecules retained at low dehydration temperature may block surface SiOH groups and promote the reaction process. With higher BAS density resulting from ultrasonic irradiation, [Al]MCM-41 catalyst (Si/Al = 10) in this work obtained the highest CPL yield among all [Al]MCM-41 materials reported for liquid-phase Beckmann rearrangement up to now. Finally, the reusability of [Al]MCM-41 catalyst was tested and no significant activity loss can be observed after five reaction cycles.en_AU
dc.language.isoenen_AU
dc.publisherElsevieren_AU
dc.relation.ispartofJournal of Catalysisen_AU
dc.titleAcidity enhanced [Al]MCM-41 via ultrasonic irradiation for the Beckmann rearrangement of cyclohexanone oxime to ɛ-caprolactamen_AU
dc.typeArticleen_AU
dc.identifier.doihttps://doi.org/10.1016/j.jcat.2017.11.013
dc.rights.otherThis manuscript version is made available under the CC-BY-NC-ND 4.0 license https://creativecommons.org/licenses/by-nc-nd/4.0
usyd.facultySeS faculties schools::Faculty of Engineeringen_AU
usyd.citation.volume358en_AU
usyd.citation.spage71en_AU
usyd.citation.epage79en_AU
workflow.metadata.onlyNoen_AU


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