Synthesis of Hydroxylamine via Ketone-Mediated Nitrate Electroreduction

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(15), С. 10934 - 10942

Опубликована: Апрель 6, 2024

Hydroxylamine (HA, NH2OH) is a critical feedstock in the production of various chemicals and materials, its efficient sustainable synthesis great importance. Electroreduction nitrate on Cu-based catalysts has emerged as promising approach for green ammonia (NH3) production, but electrosynthesis HA remains challenging due to overreduction NH3. Herein, we report first work ketone-mediated using water. A metal–organic-framework-derived Cu catalyst was developed catalyze reaction. Cyclopentanone (CP) used capture situ form CP oxime (CP-O) with C═N bonds, which prone hydrolysis. could be released easily after electrolysis, regenerated. It demonstrated that CP-O formed an excellent Faradaic efficiency 47.8%, corresponding formation rate 34.9 mg h–1 cm–2, remarkable carbon selectivity >99.9%. The hydrolysis release regeneration also optimized, resulting 96.1 mmol L–1 stabilized solution, significantly higher than direct reduction. Detailed characterizations, control experiments, theoretical calculations revealed surface reconstruction reaction mechanism, showed coexistence Cu0 Cu+ facilitated protonation reduction *NO2 *NH2OH desorption, leading enhancement production.

Язык: Английский

In-situ reconstruction to regulate electronic state for dilute nitrate electroreduction

Separation and Purification Technology, Год журнала: 2025, Номер unknown, С. 132609 - 132609

Опубликована: Март 1, 2025

CO2/NOx-involved Electrochemical C-N Coupling Reactions

Chemical Research in Chinese Universities, Год журнала: 2024, Номер 40(5), С. 764 - 775

Опубликована: Июнь 18, 2024

Язык: Английский