Construction of a Heterostructured Alloy–Molybdenum Nitride Catalyst for Enhanced NH₃ Production via Nitrate Electrolysis

Inorganic Chemistry, Год журнала: 2025, Номер unknown

Опубликована: Янв. 14, 2025

Here, we reported a highly efficient nitrate electroreduction (NO3RR) electrocatalyst that integrated alloying and heterostructuring strategies comprising FeCo alloy Mo0.82N (FeCo-Mo0.82N/NC). Notably, the maximum NH3 Faraday efficiency (FE) of 83.24%, yield 12.28 mg h-1 mgcat.-1, good stability were achieved over FeCo-Mo0.82N/NC. Moreover, Zn-NO3- battery assembled with FeCo-Mo0.82N/NC exhibited power density 0.87 mW cm-2, an 14.09 FE as high 76.31%.

Язык: Английский

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Asymmetric CuS₁N₄ as Axial Polarization Site Trigger Rapid Charge Transport Channels for Boosting Photosynthesis of Ammonia

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 10, 2025

Abstract Effective photogenerated charge transfer and utilization have been regarded as a critical factor for achieving highly efficient photosynthesis of ammonia. However, the lacks necessary driving force in many catalysts limit directly transfer. In this work, Cu porphyrin‐based monoatomic layer (PML‐Cu) is modified on face‐centered cubic structured defective CdIn 2 S 4 via solvothermal reaction, with strong coupled interfacial Cu─S bond constructed. Owing to formation axial CuS 1 N polarization site, local asymmetric configuration can be created between PML‐Cu form potential difference, inducing rapid transport from bond. Meantime, electron‐enriched site beneficial stabilization * NHOH intermediate state, then lowering NHO→ rate‐limiting step energy barrier. Benefiting these features, PML‐Cu/CdIn exhibit good NH 3 generation rate 1979.0 µmol g −1 h , apparent quantum efficiency 8.56% at 380 nm 7.40% 450 nm, respectively. This work provides an accessible pathway designing coupling boost photocatalysis.

Язык: Английский

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Bimetallic Cu11Ag3 Nanotips for Ultrahigh Yield Rate of Nitrate‐to‐Ammonium

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

Опубликована: Окт. 2, 2024

Electrochemical reduction of nitrate to ammonia (NRA) offers a sustainable approach for NH

Язык: Английский

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Reshape Iron Nanoparticles Using a Zinc Oxide Nanowire Array for High Efficiency and Stable Electrocatalytic Nitrogen Fixation

ACS Applied Materials & Interfaces, Год журнала: 2025, Номер unknown

Опубликована: Янв. 21, 2025

As a type of century-old catalyst, the use iron-based materials runs through Haber–Bosch process and electrochemical synthesis ammonia because its excellent capability, low cost, abundant reserves. How to continuously improve catalytic activity stability for nitrogen fixation has always been goal pursued by scientific researchers. Herein, we develop free-standing i.e., iron nanoparticles with zinc oxide nanowire array support (Fe/ZnO NA), which exhibits high yield ∼54.81 μg h–1 mgcat.–1 Faradaic efficiency (FE) ∼9.56% in 0.5 M potassium hydroxide solution, along good reusability durability. Its electrocatalytic ability is superior that commercial Fe most reported Fe-based catalysts, thus showing great competitiveness. This ZnO NA not only supplies stable homogeneous dispersion but also provides very beneficial synergy their activity. The work renews traditional catalysts significance promoting industrialization synthesis.

Язык: Английский

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The crucial roles of oxygen vacancies and homojunction in boosting the electrochemical nitrogen reduction of La-doping RGO/W18O49@WO3

Separation and Purification Technology, Год журнала: 2025, Номер 362, С. 131938 - 131938

Опубликована: Фев. 6, 2025

Язык: Английский

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Boosting the Electrocatalytic Dinitrogen Reduction Reaction with Selenium Vacancy in Transition Metal Dichalcogenides

Energy & Fuels, Год журнала: 2025, Номер unknown

Опубликована: Фев. 7, 2025

Язык: Английский

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Interfacial Asymmetrically Coordinated Zn−MOF for High‐Efficiency Electrosynthetic Oxime

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

Опубликована: Фев. 21, 2025

Abstract Oximes are important intermediates for various chemicals synthesis such as pharmaceuticals, among which one vital precursor producing neurological disease, antimicrobial and anticancer agents is piperidone oxime (PDO). Compared with conventional thermocatalytic method, it's more attractive to synthesize PDO via green electrocatalytic technology especially utilizing waste nitrogen oxides gas source. However, there great challenges in catalyst design high‐efficiency electrosynthetic due the low electron transport rate multiple competing reactions. Herein, we propose an interfacial coordination strategy based on metal–organic frameworks (MOF) electrocatalyst first time promote electrosynthesis, by building Zn−O bridges between graphite felt (GF) zeolitic imidazolate framework (ZIF‐7/CGF). Specially, ZIF‐7/CGF delivers a Faraday efficiency (FE) of 75.9 % yield up 73.1 1‐methyl‐4‐piperidone oxime, far superior without (a FE 10.7 10.3 %). In‐depth mechanism study shows that introducing can transfer induce Zn sites transforming into distorted tetrahedron (Zn‐N 3 O) mode, benefits adsorption conversion. The developed presents wide universalities towards oximes electrosynthesis adapts other MOF materials (ZIF‐8, ZIF‐4). This work provides new insights organic upgrading cycle through rational surficial coordinated electrocatalysts.

Язык: Английский

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Interfacial Asymmetrically Coordinated Zn−MOF for High‐Efficiency Electrosynthetic Oxime

Angewandte Chemie, Год журнала: 2025, Номер unknown

Опубликована: Фев. 21, 2025

Abstract Oximes are important intermediates for various chemicals synthesis such as pharmaceuticals, among which one vital precursor producing neurological disease, antimicrobial and anticancer agents is piperidone oxime (PDO). Compared with conventional thermocatalytic method, it's more attractive to synthesize PDO via green electrocatalytic technology especially utilizing waste nitrogen oxides gas source. However, there great challenges in catalyst design high‐efficiency electrosynthetic due the low electron transport rate multiple competing reactions. Herein, we propose an interfacial coordination strategy based on metal–organic frameworks (MOF) electrocatalyst first time promote electrosynthesis, by building Zn−O bridges between graphite felt (GF) zeolitic imidazolate framework (ZIF‐7/CGF). Specially, ZIF‐7/CGF delivers a Faraday efficiency (FE) of 75.9 % yield up 73.1 1‐methyl‐4‐piperidone oxime, far superior without (a FE 10.7 10.3 %). In‐depth mechanism study shows that introducing can transfer induce Zn sites transforming into distorted tetrahedron (Zn‐N 3 O) mode, benefits adsorption conversion. The developed presents wide universalities towards oximes electrosynthesis adapts other MOF materials (ZIF‐8, ZIF‐4). This work provides new insights organic upgrading cycle through rational surficial coordinated electrocatalysts.

Язык: Английский

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Modifying Microenvironment in Van der Waals Gap by Cu/N Co‐Doping Strategy for Highly Efficient Nitrite Reduction to Ammonia

Advanced Science, Год журнала: 2025, Номер unknown

Опубликована: Фев. 24, 2025

Abstract Electroreduction of nitrite to ammonia has significant promise for economical NH 3 electrosynthesis and wastewater treatment. Herein, sulfur vacancies rich Cu─N co‐doped SnS 2 nanosheet is designed as a highly active durable NO RR catalyst. Benefiting from the strategy, Cu/N‐SnS 2‐x achieves highest yield rate 18.15mg h −1 mg cat at −0.935 V (vs RHE) excellent Faradaic Efficiency 95.73% −0.835 RHE). In situ FT‐IR in XPS proves that greater capacity atomic hydrogen generation, which facilitates conversion maintains structural stability during process. Theoretical calculations reveal introduced effectively expose metal atoms inside make them adsorb efficiently, accelerates transformation ammonia. Besides, Cu N can form new electronic structure, induces an electron‐deficient state promotes adsorption reaction intermediates on Cu, reduces energy barrier reduction surface. The current exploration presents fresh prospects rational development effective electrocatalyst synthesizing nitrite.

Язык: Английский

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Enabling Unconventional “Alternating‐Distal” N₂ Reduction Pathway for Efficient Ammonia Electrosynthesis

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

Опубликована: Март 10, 2025

The general understanding on the reaction path is that electrocatalytic N2 reduction follows either individual associative alternating or distal pathways, where efficient activation and selective NH3 production are very challenging. Herein, an unconventional "alternating-distal" pathway was achieved by shifting "*NHNH2→*NH2NH2" to "*NHNH2→*NH + NH3" step boost synthesis with amorphous CeMnOx electrocatalyst. In this process, realized through π back donation Mn site, while Mn/Ce dual active sites could regulate intermediate configurations avoid nitrogen-containing by-product formation. Such affirmed in situ spectroscopic analyses theoretical calculations. a neutral media, average ammonia rate of 82.8 µg h-1 mg-1 outstanding Faradaic efficiency 37.3% were attained. This work validated mechanism synthesis, which might be extended other catalytic process multiple possible paths.

Язык: Английский

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