Cyclohexanone ammoximation via in situ H2O2 production using TS-1 supported catalysts. Issue 24 (14th September 2022)

• Record Type: Journal Article
• Authors: Lewis, Richard J.; Ueura, Kenji; Fukuta, Yukimasa; Davies, Thomas E.; Morgan, David J.; Paris, Charlie B.; Singleton, James; Edwards, Jennifer. K.; Freakley, Simon J.; Yamamoto, Yasushi; Hutchings, Graham J.
• Is Part Of: Green chemistry. Volume 24:Issue 24(2022)
• Page Start: 9496
• Page End: 9507
• Publication Date: 2022-09-14
• Subjects: Environmental chemistry -- Industrial applications -- Periodicals; Environmental management -- Periodicals; 660
• DOI: 10.1039/d2gc02689a
• Languages: English
• ISSNs: 1463-9262

Abstract

Abstract : The in situ synthesis of H2 O2 offers an attractive alternative to the current industrial route to cyclohexanone oxime, a major precursor to Nylon-6. Abstract : The ammoximation of cyclohexanone to the corresponding oxime via in situ H2 O2 formation offers an attractive alternative to the current industrial means of production, overcoming the significant economic and environmental concerns associated with the manufacture of a key reagent, H2 O2 . Herein we demonstrate the efficacy of a composite catalyst, consisting of precious metal nanoparticles supported on a commercial TS-1, towards the in situ synthesis of cyclohexanone oxime, bridging the wide condition gap that exists between the two distinct reaction pathways: H2 O2 direct synthesis and cyclohexanone ammoximation. In particular, the alloying of Au with Pd and the introduction of low concentrations of Pt into AuPd nanoalloys are found to be key in promoting high catalytic performance. The improved catalytic activity of optimal catalysts is found to result from a combination of a disruption of contiguous Pd ensembles and the modification of Pd oxidation states, which in turn dictate catalytic activity towards the production and subsequent degradation of H2 O2 .