Unveiling Ionized Interfacial Water‐Induced Localized H* Enrichment for Electrocatalytic Nitrate Reduction

Angewandte Chemie International Edition, Год журнала: 2024, Номер 64(1)

Опубликована: Сен. 4, 2024

Electrocatalytic nitrate reduction reaction (NO

Язык: Английский

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Bi₁‐CuCo₂O₄ Hollow Carbon Nanofibers Boosts NH₃ Production from Electrocatalytic Nitrate Reduction

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Авг. 6, 2024

Abstract Ammonia, as a high‐energy‐density carrier for hydrogen storage, is in great demand worldwide. Electrocatalytic nitrate reduction reaction (NO 3 RR) provides green NH production process. However, the complex pathways NO RR to and difficulty controlling intermediate products limit Herein, by incorporating atomic‐level bismuth (Bi) into CuCo 2 O 4 hollow carbon nanofibers, catalytic activity of electrocatalyst enhanced. The maximum Faradaic efficiency Bi 1 ‐CuCo 95.53%, with an yield 448.74 µmol h −1 cm −2 at −0.8 V versus RHE. Density Functional Theory calculations show that presence lowers barrier hydrogenation step from *NO H, while promoting mass transfer on release *NH reactivation surface‐active sites. Differential charge density also after doping, supplied catalyst − increases 0.62 0.72 e ‐ , thus reasoned enhanced activity. established nitrate‐Zn battery shows energy 2.81 mW implying potential application.

Язык: Английский

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FeIr Alloy Optimizes the Trade‐Off Between Nitrate Reduction and Active Hydrogen Generation for Efficient Electro‐Synthesis of Ammonia in Neutral Media

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Фев. 10, 2025

Abstract Electrochemically promoted nitrate reduction reaction (NITRR) holds great potential for the “green” synthesis of ammonia (NH 3 ). However, NITRR in neutral media, though close to practical scenario, is often limited by an insufficient supply active hydrogen (*H) due sluggish water cleavage. In this work, it demonstrated that a bimetallic alloy FeIr can optimize trade‐off between and *H formation media. As result, exhibits excellent catalytic performance toward with Faradaic efficiency NH up 97.3% high yield rate 11.67 mg h −1 cm −2 at low working −0.6 V (versus reversible electrode (RHE)), surpassing monometallic catalysts as well majority Fe‐based state‐of‐the‐art. It also found displays remarkable electron rearrangement hetero‐atoms their significant orbital hybridization, which benefits not only but process. Moreover, coupling FeIr‐based methanol oxidation (MOR) results sustainable productions formate combined FE nearly 200% cell‐voltage 2 V. This work thus demonstrates promising strategy designing efficient NITRR.

Язык: Английский

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Recent Breakthroughs in Electrocatalytic Reduction of Nitrogen-Oxyanions for Environmentally Benign Ammonia Synthesis

Nano Energy, Год журнала: 2025, Номер unknown, С. 110683 - 110683

Опубликована: Янв. 1, 2025

Язык: Английский

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Asymmetric spin exchange interaction induced by orderly bimetal atomic-hybridization optimizes nitrate reduction electrocatalysis

Surfaces and Interfaces, Год журнала: 2025, Номер unknown, С. 106078 - 106078

Опубликована: Фев. 1, 2025

Язык: Английский

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Efficient Electrocatalytic Semi‐Hydrogenation of Alkynes by Interfacial Engineering of Atomically Precise Silver Nanoclusters

Angewandte Chemie International Edition, Год журнала: 2025, Номер unknown

Опубликована: Март 6, 2025

Owing to its green energy and hydrogen sources, electrocatalytic semi-hydrogenation of alkynes is an attractive alternative for industrial alkene production. However, broad application hindered by low selectivity Faradaic efficiency (FE) due side reactions like over-hydrogenation alkanes. Here, we demonstrate that atomically precise Ag25(MHA)18 nanoclusters (NCs) can electrocatalyze alkyne with 98 % conversion, 99 selectivity, 85 FE, in a substrate pool. This achieved engineering the local environment at catalytically active sites. We leverage amphiphilic MHA (6-mercaptohexanoic acid) ligands pre-concentrate water molecules near ligand-layer/Ag25 interface. Long-chain disrupt hydrogen-bond network interface, high negative charge Ag25 attract weakly hydrogen-bonded through counterions promote generation (H*), while enzyme-like catalytic pockets on surface NCs facilitate adsorption terminal via σ-bonding Ag atoms. Density functional theory calculations confirmed preference model further revealed facile release product alkene. work not only exemplifies interface strategy control sites optimized activity selectivity.

Язык: Английский

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Dipropyne‐Modified N‐Heterocyclic Carbene Stabilized Atomically Precise Copper(I) Nanocluster Catalysts for CO₂ Electroreduction

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Фев. 25, 2025

Abstract Atomically precise copper(I) nanoclusters with stable active sites are highly sought‐after catalysts for the electrocatalytic CO₂ reduction reaction (CO₂RR), providing an exceptional platform to elucidate structure–activity relationships. However, rational synthesis of robust copper as effective electrocatalysts and understanding relationship between a more realistic site its performance remain significant challenge due their inherent instability. Here, novel dipropyne‐modified NHC ligand is elaborately devised two atomically nanoclusters, [Cu 17 H 6 (NHC ) 4 (dppm) ] 3+ ( Cu17a Ph Cu17b ), both exhibiting distinct unique square orthobicupola Cu core J 28 , Johnson solid). The σ‐ π‐bonding ligands imparts ultrahigh stability while coordination pattern μ 7 ‐ η σ 1 : π 2 facilitates exposure neighboring atoms, generating accessible catalytic sites. Electrocatalytic CO experiments show that achieves highest Faradaic efficiency ethylene production among reported nanoclusters. tandem mechanism RR elucidated through combination theoretical calculations attenuated total reflection‐surface‐enhanced IR absorption spectroscopy (ATR‐SEIRAS). This work not only introduces synthesizing but also offers critical insights into molecular design principles catalysts.

Язык: Английский

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Lighting up metal nanoclusters by the H2O-dictated electron relaxation dynamics

Nature Communications, Год журнала: 2025, Номер 16(1)

Опубликована: Март 7, 2025

Abstract The modulation of traps has found attractive attention to optimize the performance luminescent materials, while understanding trap-involved photoluminescence management metal nanoclusters greatly lags behind, thus extensively impeding their increasing acceptance as promising chromophores. Here, we report an efficient passivation structural oxygen vacancies in AuAg by leveraging H 2 O molecules, achieving a sensitive color tuning from 536 480 nm and remarkably boosting quantum yield 5.3% (trap-state emission) 91.6% (native-state emission). In detail, favored electron transfer relevant contributes weak trap-state emission, which is capable being restrained molecules taking Au-O Ag-O bonds. This scenario allows dominated native-state emission with faster radiative rate. parallel, can rigidify landscape on hydrogen bonding, enabling suppression electron-optical phonon coupling decelerated non-radiative presented study deepens tailoring properties manipulating surface trap chemistry relaxation dynamics, would shed new light customizable performance.

Язык: Английский

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Efficient urea synthesis by coupling catalyst of nickel-single-atom and copper-cluster

Journal of Material Science and Technology, Год журнала: 2025, Номер unknown

Опубликована: Март 1, 2025

Язык: Английский

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Cu‐Based Nanomaterials for Oxime Electrosynthesis: Advances, Challenges, and Perspectives

cMat., Год журнала: 2025, Номер 2(1)

Опубликована: Март 1, 2025

ABSTRACT Cu‐based nanomaterials have demonstrated great potential for catalyzing the electrosynthesis of oxime compounds, a type organonitrogen molecule that finds versatile applications in pharmaceutical industry, medicine production, chemical feedstocks, and other fields. This review first explains significance compounds compares conventional synthetic approach with emerging electrochemical method. Then, including compounds/composites, bimetallic alloys, high entropy single‐atom catalysts are described some explicit examples to elucidate structure‐performance relationship clearly. Finally, current challenges future perspectives this rapidly developing evolving field analyzed critical thoughts. is anticipated stimulate more research efforts be dedicated fast‐growing yet quite promising field.

Язык: Английский

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