Cu–Bi Bimetallic Catalysts Derived from Metal–Organic Framework Arrays on Copper Foam for Efficient Glycine Electrosynthesis

Angewandte Chemie International Edition, Год журнала: 2024, Номер unknown

Опубликована: Сен. 30, 2024

Abstract Glycine as one of the most abundant amino acids in human proteins, with extensive applications both life and industry, is conventionally synthesized through complex procedures or toxic feedstocks. In this study, we present a facile benign electrochemical pathway for synthesis glycine reductive coupling glyoxylic acid nitrate over copper‐bismuth bimetal catalyst derived from metal–organic framework (MOF) array on copper foam (Cu/Bi−C@CF). Remarkably, Cu/Bi−C@CF achieves fantastic selectivity 89 %, corresponding high Faraday efficiency 65.9 %. From control experiments, introduction Bi caused binding energy Cu shift to lower state, which leads towards formation key intermediate hydroxylamine rather than ammonia product, facilitating oxime providing additional sites subsequent hydrogenation reaction way glycine. Moreover, derivation MOF arrays ensures effective dispersion enhances stability Cu/Bi−C@CF. This innovative approach not only presents sustainable pathways production value‐added organonitrogen compounds utilizing readily available carbon nitrogen sources, but also provides novel insights into design multistage structural catalysts sequential reactions.

Язык: Английский

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Highly Efficient One‐pot Electrosynthesis of Oxime Ethers from NOx over Ultrafine MgO Nanoparticles Derived from Mg‐based Metal‐Organic Frameworks

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(26)

Опубликована: Апрель 10, 2024

Oxime ethers are attractive compounds in medicinal scaffolds due to the biological and pharmaceutical properties, however, crucial widespread step of industrial oxime formation using explosive hydroxylamine (NH

Язык: Английский

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Electrocatalytic Reductive Amination of Aldehydes and Ketones with Aqueous Nitrite

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

Опубликована: Март 10, 2025

The electrocatalytic utilization of oxidized nitrogen waste for C-N coupling chemistry is an exciting research area with great potential to be adopted as a sustainable method generation organonitrogen molecules. most widely used reaction reductive amination. In this work, we develop alternative electrochemical amination that can proceed in neutral aqueous electrolyte nitrite the nitrogenous reactant and via oxime intermediate. We selection criterion reduction electrocatalysts suited electrosynthesis and, doing so, find Pd highly efficient catalyst reaction, reaching Faradaic efficiency 82% at -0.21 V vs reversible hydrogen electrode. aliphatic or aromatic structure carbonyl impacts efficacy catalyst, substrates leading suppressed formation detrimental alcohol. developed Pb/PbO electrocatalyst selectively performs electrolyte. With acetone model substrate, demonstrate one-pot, two-step conversion isopropyl amine 85% yield 50% global efficiency.

Язык: Английский

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Deciphering Indirect Nitrite Reduction to Ammonia in High‐Entropy Electrocatalysts Using In Situ Raman and X‐ray Absorption Spectroscopies

Small, Год журнала: 2024, Номер 20(29)

Опубликована: Апрель 11, 2024

This research adopts a new method combining calcination and pulsed laser irradiation in liquids to induce controlled phase transformation of Fe, Co, Ni, Cu, Mn transition-metal-based high-entropy Prussian blue analogs into single-phase spinel oxide face-centered cubic alloy (HEA). The synthesized HEA, characterized by its highly conductive nature reactive surface, demonstrates exceptional performance capturing low-level nitrite (NO

Язык: Английский

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Selective Synthesis of Organonitrogen Compounds via Electrochemical C–N Coupling on Atomically Dispersed Catalysts

ACS Nano, Год журнала: 2024, Номер 18(35), С. 23894 - 23911

Опубликована: Авг. 20, 2024

The C-N coupling reaction demonstrates broad application in the fabrication of a wide range high value-added organonitrogen molecules including fertilizers (e.g., urea), chemical feedstocks amines, amides), and biomolecules amino acids). electrocatalytic pathways from waste resources like CO

Язык: Английский

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A self-reactivated PdCu catalyst for aldehyde electro-oxidation with anodic hydrogen production

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Ноя. 14, 2024

The low-potential aldehyde oxidation reaction can occur at low potential (~0 VRHE) and release H2 the anode, enabling hydrogen production with less than one-tenth of energy consumption required for water splitting. Nevertheless, activity stability Cu catalysts remain inadequate due to oxidative deactivation Cu-based materials. Herein, we elucidate reactivation cycle electrocatalyst develop a self-reactivating PdCu catalyst that exhibits significantly enhanced stability. Initially, in-situ Raman spectroscopy confirm involved in electrochemical non-electrochemical reduction. Subsequently, X-ray absorption fine structure reveal Pd component accelerates rate reduction, thereby enhancing electrocatalyst. Finally, bipolar device is assembled utilizing electrocatalyst, which deliver current 400 mA cm−2 0.42 V operate continuously 120 h. This work offers guidance enhance system. A dual-side system more efficient splitting but suffers from issues. Here, authors report operates stably h, offering an alternative solution energy-efficient production.

Язык: Английский

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A perspective on renewable production of amino acids from biomass through the chemocatalytic method

Green Chemistry, Год журнала: 2024, Номер 26(8), С. 4468 - 4476

Опубликована: Янв. 1, 2024

This perspective showcases recent advances in amino acid synthesis from biomass through the chemocatalytic method.

Язык: Английский

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Boosting Amino Acid Synthesis with WO_x Sub‐Nanoclusters

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 12, 2025

Abstract The conversion of nitrate‐rich wastewater and biomass‐derived blocks into high‐value products using renewably generated electricity is a promising approach to modulate the artificial carbon nitrogen cycle. Here, new synthetic strategy WO x sub‐nanoclusters reported supported on materials as novel efficient electrocatalysts for nitrate reduction its coupling with α‐keto acids. In acidic solutions, NH 3 ‐NH 2 OH selectivity can also optimized by adjusting potential, total FE exceeding 80% over wide potential range. After introducing acids, /D‐CB electrode achieves remarkable activity toward C ‐C 6 amino For glycine alanine, impressive FEs 49.34% 38.22% based transitional metal oxides be obtained, surpassing those nanoclusters larger size. situ analysis mechanistic studies reveal critical role in reducing energy barriers key steps alanine synthesis. This work opens up insights rational design cluster catalysts promote electrochemical acid

Язык: Английский

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Single-atom catalysts for electrocatalytic conversion of biomass-derived small molecules

Coordination Chemistry Reviews, Год журнала: 2025, Номер 534, С. 216576 - 216576

Опубликована: Март 6, 2025

Язык: Английский

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Multifunctional Carbon‐Based Metal‐Free Catalysts for Cascade Electrochemical‐Chemical Coupling Catalyses

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Март 10, 2025

Abstract Cascade electrochemical‐chemical coupling (CECC) involves sequential electrochemical and chemical reactions, using intermediates from processes as reactants for subsequent transformations to enhance the efficiency selectivity sustainable syntheses of complex chemicals. Despite its economic environmental benefits, CECC still faces multiple challenges, including a low utilization intermediate reactants, competitive side difficulties in design scale‐up catalysts, leading yield. To ensure economically viable CECC, it is imperative rationally develop cost‐efficient high‐performance such carbon‐based metal‐free electrocatalysts (C‐MFECs) certain carbon‐supported transition metal with high activity atomic precision desirable products. In this review, an overview recent advancements doping C‐MFECs provided enhancing their catalytic toward CECC. Three major systems based on are discussed; they hydrogen peroxide coupling, carbon dioxide upgrading, redox‐mediated systems. Current challenges future perspectives emerging field also addressed.

Язык: Английский

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