Acidity enhanced [Al]MCM-41 via ultrasonic irradiation for the Beckmann rearrangement of cyclohexanone oxime to ɛ-caprolactam
Field | Value | Language |
dc.contributor.author | Wang, Zichun | |
dc.contributor.author | Ling, Huajuan | |
dc.contributor.author | Shi, Jeffrey | |
dc.contributor.author | Stampfl, Catherine | |
dc.contributor.author | Yu, Aibing | |
dc.contributor.author | Hunger, Michael | |
dc.contributor.author | Huang, Jun | |
dc.date.accessioned | 2021-01-22T02:04:42Z | |
dc.date.available | 2021-01-22T02:04:42Z | |
dc.date.issued | 2018 | en_AU |
dc.identifier.uri | https://hdl.handle.net/2123/24355 | |
dc.description.abstract | Using 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.iso | en | en_AU |
dc.publisher | Elsevier | en_AU |
dc.relation.ispartof | Journal of Catalysis | en_AU |
dc.title | Acidity enhanced [Al]MCM-41 via ultrasonic irradiation for the Beckmann rearrangement of cyclohexanone oxime to ɛ-caprolactam | en_AU |
dc.type | Article | en_AU |
dc.identifier.doi | https://doi.org/10.1016/j.jcat.2017.11.013 | |
dc.rights.other | This manuscript version is made available under the CC-BY-NC-ND 4.0 license https://creativecommons.org/licenses/by-nc-nd/4.0 | |
usyd.faculty | SeS faculties schools::Faculty of Engineering | en_AU |
usyd.citation.volume | 358 | en_AU |
usyd.citation.spage | 71 | en_AU |
usyd.citation.epage | 79 | en_AU |
workflow.metadata.only | No | en_AU |
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