Multiple Secondary Bond-Mediated C–N Coupling over N-Doped Carbon Electrocatalysts DOI

Xiaoying Lü,

Ze‐Cheng Yao, Xinbo Ma

и другие.

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Май 19, 2025

Electrocatalytic C-N reductive coupling offers a sustainable and eco-friendly approach to producing value-added oximes. The challenge lies in the overstrong chemisorption of N-containing intermediates carbonyl compounds on metal-based catalysts, which causes low Faradaic efficiency yield rates, as well undesired byproducts. Here, we propose multiple secondary bond-mediated strategy for toward benzaldoxime nitrogen-doped graphene-like carbon catalyst (NC). Integrating theoretical experimental analyses, demonstrate that graphitic-N-C sites NC promote nitrite reduction into hydroxylamine via weak electrostatic interaction. Moreover, hydrogen bonds π-π stacking interactions among NC, hydroxylamine, benzaldehyde synergistically enrich key surface inhibit side reactions, leading highly selective process. Remarkably, achieves high 73 ± 1% rate 6.8 0.1 mol h-1 m-2 electrosynthesis at an economically viable current density A cm-2, revealed by technoeconomic analysis. Our results appealing route high-performance with enhanced economic feasibility.

Язык: Английский

Multiple Secondary Bond-Mediated C–N Coupling over N-Doped Carbon Electrocatalysts DOI

Xiaoying Lü,

Ze‐Cheng Yao, Xinbo Ma

и другие.

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Май 19, 2025

Electrocatalytic C-N reductive coupling offers a sustainable and eco-friendly approach to producing value-added oximes. The challenge lies in the overstrong chemisorption of N-containing intermediates carbonyl compounds on metal-based catalysts, which causes low Faradaic efficiency yield rates, as well undesired byproducts. Here, we propose multiple secondary bond-mediated strategy for toward benzaldoxime nitrogen-doped graphene-like carbon catalyst (NC). Integrating theoretical experimental analyses, demonstrate that graphitic-N-C sites NC promote nitrite reduction into hydroxylamine via weak electrostatic interaction. Moreover, hydrogen bonds π-π stacking interactions among NC, hydroxylamine, benzaldehyde synergistically enrich key surface inhibit side reactions, leading highly selective process. Remarkably, achieves high 73 ± 1% rate 6.8 0.1 mol h-1 m-2 electrosynthesis at an economically viable current density A cm-2, revealed by technoeconomic analysis. Our results appealing route high-performance with enhanced economic feasibility.

Язык: Английский

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