Stabilized Bi(III) Sites Direct *NH₂OH Pathway for Efficient Cyclohexanone Oxime Electrosynthesis.

Authors

Zichao Xi, Yan Du, Haijing Li, Jian Shang, Jinxiao Wu, Peng Li, Huimin Yu, Tianyi Ma, Huanyu Jin

Published in

Advanced materials (Deerfield Beach, Fla.). Pages e73997. Jul 07, 2026. Epub Jul 07, 2026.

Abstract

Coupling electrocatalytic nitrite reduction reaction (NO₂ ^-RR) with cyclohexanone conversion enables a sustainable route to cyclohexanone oxime (CHO) electrosynthesis, a key feedstock for the nylon-6 industry. However, this approach is fundamentally constrained by the difficulty of sustaining selective *NH₂OH intermediate formation. Here, we reveal for the first time that the Bi(III) sites can enable the catalytic system to efficiently follow the *NH₂OH pathway, avoiding the undesired *N pathway. Accordingly, a BiPO₄/SiO_x interface was designed in which amorphous SiO_x functions as an electron-buffer to stabilize Bi(III) active sites. As a result, the BiPO₄/SiO_x catalyst exhibits a high faradaic efficiency (FE_CHO) of 77.0 ± 3.4% and a CHO yield rate of 0.64 ± 0.01 mmol h^-1 cm^-2, surpassing all previously reported catalysts in H-cellMoreover, the BiPO₄/SiO_x catalyst delivers a nearly 100% carbon and nitrogen selectivity to CHO and retains 91.8% of its initial efficiency after extended cycling, substantially outperforming pristine BiPO₄. Combined experimental and theoretical analyses reveal that the stabilized Bi(III) site suppresses the formation of surface K⁺ H₂O, effectively suppressing competing hydrogen evolution and over hydrogenation, thereby enabling efficient CHO electrosynthesis.

PMID:
42411152
Bibliographic data and abstract were imported from PubMed on 07 Jul 2026.

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