High‐Efficiency Electrocatalytic Conversion of Nitrite to Ammonia Using Nickel Phthalocyanine

Chemistry - An Asian Journal, Год журнала: 2025, Номер unknown

Опубликована: Апрель 30, 2025

Nitrite (NO2 -) is a dangerous pollutant that often found in groundwater sources and endangers human health. In addition to nitrite removal requirements, electrocatalytic reduction reaction (eNO2RR) holds promise for value-added ammonia (NH3) production at room temperature. this study, solvothermal technique the preparation of nickel phthalocyanine (NiPc) used as highly active electrocatalyst conversion NO2 - NH3 under ambient conditions. The NiPc catalyst shows remarkable Faradaic efficiency (FE) 90.1% -0.9 V versus RHE with maximum yield rate 14667 µg h-1 mgcat. -1 -1.0 0.1 M Na2SO4 containing NaNO2 solution. Furthermore, exhibits exceptional long-term stability during chronoamperometry tests. These findings boost future from sustainable development.

Язык: Английский

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Ir NCs Embedded Co-MOF Nanosheets for Boosting Electrochemical Nitrate Reduction to Ammonia Performance

ACS Applied Materials & Interfaces, Год журнала: 2025, Номер 17(19), С. 28084 - 28093

Опубликована: Май 2, 2025

In this study, Ir nanoclusters adorned with abundant p-mercaptobenzoic acid (p-MBA) ligands were employed to fabricate an electrocatalytic material consisting of embedded within two-dimensional Co-MOF nanosheets (Ir NCs@Co-MOF) for the NO3- reduction reaction (NO3-RR). TEM analysis confirmed that are uniformly distributed in 2D nanosheets, average diameter about 1.8 nm. At a potential -0.8 V vs RHE, NCs@Co-MOF catalyst achieved nitrate conversion rate, ammonia selectivity, and yield 92.5, 81.4%, 230.1 μg·h-1·cm-2, respectively, over duration 120 min. The strong interaction between serves enhance activity accelerate rate reduction. Stability tests indicated after 20 cycles, both selectivity demonstrated relative stability, thereby indicating robust performance catalytic system. results EPR TBA quenching experiments indicate *H plays key role NO3-RR process. situ DEMS investigations revealed during process, pathway was as follows: *NO3 → *NO2 *NO *NOH *NH2OH *NH2 *NH3 NH3.

Язык: Английский

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Promoting Mn³⁺ Spin-State Transitions from t_2g to e_g through Ni Doping in Antiperovskite CuNMn₃ for Highly Efficient Ammonia Synthesis

The Journal of Physical Chemistry Letters, Год журнала: 2025, Номер unknown, С. 5025 - 5033

Опубликована: Май 13, 2025

The electrochemical nitrogen reduction reaction (e-NRR) offers a sustainable approach to ammonia synthesis under ambient conditions, with the potential replace energy-intensive Haber-Bosch process. Despite significant progress in this promising field, low NH3 yield rate and limited Faradaic efficiency (FE) remain formidable challenges. Here, we introduce antiperovskite Cu1-xNixNMn3, where partial substitution of Cu by Ni CuNMn3 is developed as an effective robust e-NRR electrocatalyst. Notably, Cu0.7Ni0.3NMn3 demonstrates outstanding performance, achieving 33.9 ± 1.1 μg h-1 mg-1, FE 19.2 0.62% at -0.4 V versus RHE, excellent long-term stability over 50 h electrolysis. In-depth mechanistic studies reveal that Ni/Cu exchange process Cu1-xNixNMn3 maintains structural integrity stabilizes valence states. atoms corner sites interact adjacent Mn face centers via antiferromagnetic interactions, altering original magnetic interactions. This modification triggers spin-state transition some Mn3+ ions from low-spin (t2g4eg0) high-spin (t2g3eg1) configuration. Density functional theory (DFT) calculations confirm improved eg orbital electronic configuration enhances N2 adsorption energy catalytic promotes hydrogenation form *NNH intermediates, thereby accounting for high activity Cu0.3Ni0.7NMn3 e-NRR.

Язык: Английский

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Boosting the ammonia synthesis with alternating magnetic field

Applied Catalysis B Environment and Energy, Год журнала: 2025, Номер unknown, С. 125536 - 125536

Опубликована: Май 1, 2025

Язык: Английский

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Electrocatalytic Urea Synthesis via C‐N Coupling over Fe‐Based Catalyst

ChemCatChem, Год журнала: 2024, Номер unknown

Опубликована: Ноя. 14, 2024

Abstract Electrochemical urea synthesis under ambient conditions offers a promising alternative to traditional methods, yet suffers from inefficient production due poor binding of reactants the catalyst surface, leading competitive pathways. In this study, we report an electrochemical route for by dual reduction CO 2 and N gases using iron phthalocyanine (FePc) catalyst. The FePc electrocatalyst showed yield rate 357 µmol h −1 g cat with Faradaic efficiency (FE) 14.36% at −0.4 V versus RHE. This work awareness into development efficient electrosynthesis via C─N coupling.

Язык: Английский

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Enhancement of Selective Electrocatalytic NO₃^– Reduction to NH₃ Over rGO-Coated Cu₂O Nanoparticles

ACS Applied Energy Materials, Год журнала: 2024, Номер 7(22), С. 10596 - 10604

Опубликована: Ноя. 14, 2024

It is a green and feasible approach to realize artificial nitrogen cycling through the electrocatalytic reduction of nitrate (NO3–) into ammonia (NH3). Nevertheless, electrochemical nitrate-to-ammonia reaction (NO3–RR) has been greatly hindered by low Faradaic efficiency high applied overpotential. Herein, few-layer reduced graphene oxide (rGO)-coated Cu2O nanocrystal composite (denoted as Cu2O@rGO) successfully constructed simple hydrothermal methodology enhance catalytic performance NO3–RR NH3. Benefiting from synergistic effects rapid electron migration, enriched oxygen vacancies, intimate interface, obtained Cu2O@rGO catalyst accelerates adsorption NO3– some key intermediates inhibits hydrogen evolution (HER) during NO3–RR. Consequently, optimized exhibits NH3 (FE) 91.8% at −0.9 V, selectivity up 99%, yield rate 0.25 mmol·h–1·mgcat–1, much outperforming most reported Cu-based catalysts. Moreover, in situ infrared spectroscopy (FT-IR) displays formation pathway process discloses mechanism. This work presents effective improve activity electrocatalysts for production.

Язык: Английский

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Spin‐Electrochemistry of Transition Metal Oxides for Energy Storage: Concepts, Advances and Perspectives

Chemistry - A European Journal, Год журнала: 2024, Номер unknown

Опубликована: Ноя. 14, 2024

Abstract Developing high‐capacity and cyclically stable transition metal (TM)‐based electrode materials for energy storage devices, such as aqueous ion systems, is crucial addressing the growing issue of scarcity. The spin state, or configuration d‐electrons, plays a vital role in electrochemical performance these materials. However, there has been lack systematic descriptions regarding configurations to date. This review aims elucidate advantages controlling states centers enhance highlights recent progress employing state regulation storage. Additionally, it covers various characterization techniques used determine states. Finally, we discuss future prospects challenges within this emerging field, with aim accelerating development spin‐based technologies. also seeks provide clear reliable directions design preparation novel

Язык: Английский

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Oxygen‐Vacancy‐Rich Heterostructured CeO₂‐CuO Nanowires for Urea Electrosynthesis via Co‐Reduction of Nitrate and CO₂

Advanced Sustainable Systems, Год журнала: 2024, Номер unknown

Опубликована: Дек. 1, 2024

Abstract The mild electrosynthesis of urea presents a promising approach to replace the energy‐intensive conventional manufacturing processes, and identifying highly active selective electrocatalysts is paramount importance. Herein, synthesis oxygen‐vacancy‐rich CeO 2 ‐CuO heterostructure nanowires on copper foam (CeO ‐CuO/CF) are reported. CuO‐CeO notably enhances electron transfer quickens reaction dynamics, increased oxygen vacancies greatly promote C‐N coupling nitrate CO urea. As such, ‐CuO/CF achieves remarkable faraday efficiency 31.96% yield 720.9 µg cm −2 h −1 , along with outstanding stability. This research offers electrocatalyst for sustainable on‐site production

Язык: Английский

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Atomically dispersed iron & iron clusters synergistically accelerate electrocatalytic ammonia synthesis

Chemical Engineering Journal, Год журнала: 2024, Номер unknown, С. 158785 - 158785

Опубликована: Дек. 1, 2024

Язык: Английский

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