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Selective Ammoximation of Ketones via In Situ H 2 O 2 Synthesis

2023; American Chemical Society; Volume: 13; Issue: 3 Linguagem: Inglês

10.1021/acscatal.2c05799

2155-5435

Richard J. Lewis, Kenji Ueura, Xi Liu, Yukimasa Fukuta, Tian Qin, Thomas E. Davies, David Morgan, Alex Stenner, James Singleton, Jennifer K. Edwards, Simon J. Freakley, Christopher J. Kiely, Liwei Chen, Yasushi Yamämoto, Graham J. Hutchings,

Carbon dioxide utilization in catalysis

The ammoximation of ketones to the corresponding oxime via the in situ production of H2O2 offers a viable alternative to the current means of industrial-scale production, in particular for the synthesis of cyclohexanone oxime, a key precursor to Nylon-6. Herein, we demonstrate that using a bifunctional catalyst, consisting of Pd-based bimetallic nanoparticles immobilized onto a TS-1 carrier, it is possible to bridge the considerable condition gap that exists between the two key distinct reaction pathways that constitute an in-situ approach (i.e., the direct synthesis of H2O2 and ketone ammoximation). The formation of PdAu nanoalloys is found to be crucial in achieving high reactivity and in promoting catalytic stability, with the optimal formulation significantly outperforming both alternative Pd-based materials and the monometallic Pd analogue.