Applied Catalysis B Environment and Energy, Год журнала: 2023, Номер 340, С. 123161 - 123161
Опубликована: Авг. 10, 2023
Язык: Английский
Journal of the American Chemical Society, Год журнала: 2025, Номер unknown
Опубликована: Март 4, 2025
Electrocatalyzed reduction of CO2 and NO3- to synthesize urea is a highly desirable, but challenging reaction. The bottleneck this reaction the C-N coupling intermediates. In particular, uncertainty multielectron intermediates severely affects selectivity activity processes involving multiple electron proton transfers. Here, we present novel tandem catalyst with two compatible single-atom active sites Au Cu on red phosphorus (RP-AuCu) that efficiently converts urea. Experimental theoretical prediction results confirmed center promotes transfer between molecules phosphorus, thereby regulating activation produce electrophilic *COOH. addition, can enhance attack *COOH species *NH2, thus promoting selective formation bonds. Consequently, RP-AuCu exhibited yield 22.9 mmol gcat.-1 h-1 Faraday efficiency 88.5% (-0.6 VRHE), representing one highest levels electrocatalytic synthesis. This work deepens understanding mechanism provides an interesting design approach for efficient sustainable production compounds.
Язык: Английский
Процитировано
4
Advanced Materials, Год журнала: 2025, Номер unknown
Опубликована: Янв. 23, 2025
Abstract The co‐electrolysis of CO 2 and NO 3 − to synthesize urea has become an effective pathway alternate the conventional Bosch‐Meiser process, while complexity C‐/N‐containing intermediates for C−N coupling results in electrosynthesis unsatisfactory efficiency. In this work, electronic spin state modulation maneuver with oxygen vacancies (Ov) is unveiled effectively meliorate oriented generation key * NH coupling, furnishing ultrahigh yield 2175.47 µg mg −1 h Faraday efficiency 70.1%. Mechanistic studies expound that Ov can induce conversion high‐spin Ni 2+ (t 2g 6 e g ) Ni@CeO 2−x low‐spin 3+ 1 ), which markedly enhances hybridization degree 3d N 2p orbitals NO, facilitating selective formation . Notably, situ generated serve as a localized proton donor promote electroreduction on adjacent site Ce −O exclusively afford CO, followed by each other efficiently urea. strategy tailored switching active provides reliable reference rectify structure electrocatalysts directional valorization.
Язык: Английский
Процитировано
3
Environmental Science & Technology, Год журнала: 2025, Номер unknown
Опубликована: Янв. 6, 2025
As primary air pollutants from fossil fuel combustion, the excess emission of nitric oxides (NOx) results in a series atmospheric environmental issues. Although selective catalytic reduction technology has been confirmed to be effective for NOx removal, green purification and value-added conversion under ambient conditions are still facing great challenges, especially nitrogen resource recovery. To address that, photo-/electrocatalysis offers sustainable routes efficient upcycling temperature pressure, which received considerable attention scientific communities. In this review, recent advances critically summarized. The target products reaction mechanisms systems, together with responsible active sites, discussed, respectively. Then, realistic practicability is proposed, including strict performance evaluation criteria application by photo-/electrocatalysis. Finally, current challenges future opportunities proposed terms catalyst design, enhancement, mechanism understanding, practical conditions, product separation techniques.
Язык: Английский
Процитировано
2
ACS Sustainable Chemistry & Engineering, Год журнала: 2025, Номер unknown
Опубликована: Фев. 10, 2025
Язык: Английский
Процитировано
2
Applied Catalysis B Environment and Energy, Год журнала: 2023, Номер 340, С. 123161 - 123161
Опубликована: Авг. 10, 2023
Язык: Английский
Процитировано
36