Inorganic Chemistry Frontiers, Год журнала: 2023, Номер 10(22), С. 6489 - 6505
Опубликована: Янв. 1, 2023
For electrocatalytic water splitting, MOFs can be optimized through structural modification, plane design and synergetic composite systems, the annealing process further expands types of MOF-based materials.
Язык: Английский
Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(45)
Опубликована: Сен. 18, 2023
Alanine is widely employed for synthesizing polymers, pharmaceuticals, and agrochemicals. Electrocatalytic coupling of biomass molecules waste nitrate attractive the removal alanine production under ambient conditions. However, reaction efficiency relatively low due to activation stable substrates, two reactive intermediates remains challenging. Herein, we realize integrated tandem electrochemical-chemical-electochemical synthesis from biomass-derived pyruvic acid (PA) (NO3- ) catalyzed by PdCu nano-bead-wires (PdCu NBWs). The overall pathway demonstrated as a multiple-step catalytic cascade process via NH2 OH PA on catalyst surface. Interestingly, in this electrochemical-chemical-electrochemical process, Cu facilitates electrochemical reduction intermediates, which chemically couple with form oxime, Pd promotes oxime desirable alanine. This work provides green strategy convert NO3- wealth enriches substrate scope renewable feedstocks produce high-value amino acids.
Язык: Английский
Процитировано
57
Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(45)
Опубликована: Сен. 20, 2023
Pyridine oximes produced from aldehyde or ketone with hydroxylamine (NH2 OH) have been widely applied in pharmaceutics, enzymatic and sterilization. However, the important raw material NH2 OH exhibits corrosive unstable properties, leading to substantial energy consumption during storage transportation. Herein, this work presents a novel method for directly synthesizing highly valuable pyridine using situ generated electrocatalytic NO reduction well-design nanofiber membranes (Al-NFM) derived -MIL-53(Al). Particularly, 2-pyridinealdoxime, precursor of antidote pralidoxime (2-PAM) nerve agents suffering scarcity high cost, was achieved Faraday efficiency up 49.8 % yield 92.1 %, attributing selectivity production on Al-NFM, further easily reacted iodomethane produce 2-PAM. This study proposes creative approach, having wide universality other range functional groups, which not only facilitates conversion exhaust gas (NO) waste water (NO2- ) into chemicals especially utilization through electrochemistry, but also holds significant potential synthesis neuro detoxifying drugs humanity security.
Язык: Английский
Процитировано
56
SusMat, Год журнала: 2024, Номер 4(2)
Опубликована: Март 12, 2024
Abstract The electrocatalytic synthesis of C–N coupling compounds from CO 2 and nitrogenous species not only offers an effective avenue to achieve carbon neutrality reduce environmental pollution, but also establishes a route synthesize valuable chemicals, such as urea, amide, amine. This innovative approach expands the application range product categories beyond simple carbonaceous in reduction, which is becoming rapidly advancing field. review summarizes research progress urea synthesis, using N , NO − 3 species, explores emerging trends electrosynthesis amide amine nitrogen species. Additionally, future opportunities this field are highlighted, including amino acids other containing bonds, anodic reactions water oxidation, catalytic mechanism corresponding reactions. critical captures insights aimed at accelerating development electrochemical reactions, confirming superiority method over traditional techniques.
Язык: Английский
Процитировано
48
Angewandte Chemie International Edition, Год журнала: 2023, Номер 63(3)
Опубликована: Окт. 13, 2023
Inorganic nitrogen oxide (NO
Язык: Английский
Процитировано
45
Journal of the American Chemical Society, Год журнала: 2024, Номер 146(14), С. 10084 - 10092
Опубликована: Март 26, 2024
Glycine is a nonessential amino acid that plays vital role in various biological activities. However, the conventional synthesis of glycine requires sophisticated procedures or toxic feedstocks. Herein, we report an electrochemical pathway for via reductive coupling oxalic and nitrate nitrogen oxides over atomically dispersed Fe–N–C catalysts. A selectivity 70.7% achieved Fe–N–C-700 at −1.0 V versus RHE. Synergy between FeN3C structure pyrrolic facilitates reduction to glyoxylic acid, which crucial producing oxime glycine, could reduce energy barrier *HOOCCH2NH2 intermediate formation thus accelerating conversion glycine. This new approach value-added chemicals using simple carbon sources provide sustainable routes organonitrogen compound production.
Язык: Английский
Процитировано
41
Journal of the American Chemical Society, Год журнала: 2024, Номер 146(19), С. 13527 - 13535
Опубликована: Май 1, 2024
Closing the carbon and nitrogen cycles by electrochemical methods using renewable energy to convert abundant or harmful feedstocks into high-value C- N-containing chemicals has potential transform global landscape. However, efficient conversion avenues have date been mostly realized for independent reduction of CO2 NO3–. The synthesis more complex C–N compounds still suffers from low efficiency due inability find effective catalysts. To this end, here we present amorphous bismuth–tin oxide nanosheets, which effectively reduce barrier catalytic reaction, facilitating highly selective urea production. With enhanced adsorption activation on catalyst, a coupling pathway based *CO2 rather than traditional *CO is realized. optimized orbital symmetry (*CO2) (*NO2) intermediates promotes significant increase in Faraday production an outstanding value 78.36% at −0.4 V vs RHE. In parallel, selectivity formation also 90.41% 95.39%, respectively. results insights provide valuable reference further development new catalysts CO2.
Язык: Английский
Процитировано
37
Advanced Materials, Год журнала: 2024, Номер 36(18)
Опубликована: Янв. 25, 2024
The artificial disturbance in the nitrogen cycle has necessitated an urgent need for nitric oxide (NO) removal. Electrochemical technologies NO conversion have gained increasing attention recent years. This comprehensive review presents advancements selective electrocatalytic of to high value-added chemicals, with specific emphasis on catalyst design, electrolyte composition, mass diffusion, and adsorption energies key intermediate species. Furthermore, explores synergistic electrochemical co-electrolysis carbon source molecules, enabling synthesis a range valuable chemicals C─N bonds. It also provides in-depth insights into intricate reaction pathways underlying mechanisms, offering perspectives challenges prospects electrolysis. By advancing comprehension fostering awareness balance, this contributes development efficient sustainable systems from NO.
Язык: Английский
Процитировано
32
Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(15)
Опубликована: Янв. 16, 2024
Abstract Chemical manufacturing utilizing renewable sources and energy emerges as a promising path towards sustainability carbon neutrality. The electrocatalytic reactions involving nitrogen oxides (NO x ) offered potential strategy for synthesizing various nitrogenous chemicals. However, it is currently hindered by low selectivity/efficiency limited reaction pathways, mainly due to the difficulties in controllable generation utilization of intermediates. In this minireview, focusing on intermediates NO ‐involved reactions, we discuss newly developed methodologies studying controlling generation, conversion, intermediates, which enable recent developments that yield products, including ammonia (NH 3 ), organonitrogen molecules, compounds exhibiting unconventional oxidation states. Furthermore, also make an outlook highlight future directions emerging field reactions.
Язык: Английский
Процитировано
21
Advanced Energy Materials, Год журнала: 2024, Номер 14(28)
Опубликована: Фев. 21, 2024
Abstract Electrocatalytic C−N couplings are promising alternatives to construct bonds and synthesize vital chemicals, including amine, amide, amino acid, oxime, imine, nitrile, under ambient conditions. In recent years, the electrocatalytic coupling has attracted a wide range of research interest achieved considerable developments. Here, is systematically reviewed aiming at reductive cathode oxidative anode. cathodic part, reaction systems, corresponding design principles electrocatalysts for different mechanism studies from experimental theoretical aspects, application‐oriented devices summarized. Anodic offers potential approach replace conventional energy‐demand synthesis protocols, an indispensable part green controllable construction unsaturated C = N C≡N bonds. According principle that electron transfer crucial point in anodic coupling, reactions sorted out based on direct indirect paths, respectively. Finally, challenges outlooks this field proposed. appealing topic electrochemistry possesses infinite possibilities future.
Язык: Английский
Процитировано
21
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