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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Tandem Active Sites in Cu/Mo‐WO₃ Electrocatalysts for Efficient Electrocatalytic Nitrate Reduction to Ammonia

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 5, 2025

Abstract Electrocatalytic NO 3 − reduction to NH is a promising technique for both ammonia synthesis and nitrate wastewater treatment. However, this conversion involves tandem processes of H 2 O dissociation hydrogenation, leading inferior Faraday efficiency (FE) yield rate. Herein, catalyst by anchoring atomically dispersed Cu species on Mo‐doped WO (Cu 5 /Mo 0.6 ‐WO ) the RR constructed, which achieves superior FE N 98.6% rate 26.25 mg h −1 cat at −0.7 V (vs RHE) in alkaline media, greatly exceeding performance Mo /WO counterparts. Systematic electrochemical measurement results reveal that promoted activation sites, accompanying accelerated water producing active hydrogens are responsible performance. In situ infrared spectroscopy theoretical calculation further demonstrate sites accelerate , dopant activates adjacent resulting decreased energy barrier * stepwise hydrogenation processes, making thermodynamically favorable. This work demonstrates critical role atomic level enhancing electrocatalytic paving feasible avenue developing high‐performance electrocatalysts.

Язык: Английский

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Efficient nitrate electroreduction to ammonia via synergistic cascade catalysis at Cu/Fe2O3 hetero-interfaces

CHINESE JOURNAL OF CATALYSIS (CHINESE VERSION), Год журнала: 2025, Номер 68, С. 404 - 413

Опубликована: Янв. 1, 2025

Язык: Английский

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Cu‐Co Dual Sites Tandem Synergistic Effect Boosting Neutral Low Concentration Nitrate Electroreduction to Ammonia

Advanced Science, Год журнала: 2025, Номер unknown

Опубликована: Фев. 17, 2025

Abstract Electrochemical nitrate reduction reaction (NO 3 − RR) has emerged as an alternative strategy for wastewater treatment and ammonia production in neutral low‐concentration nitrate. However, the electrocatalyst faces challenge of limited NO distribution deficient active hydrogen (H ads ) on catalyst surface resulting from low concentration difficulty water splitting under conditions. Here, a Cu‐Co dual sites tandem synergistic catalysis mechanism been proposed by doping Cu into CoP to facilitate adsorption conversion accelerate leading significantly high RR performance. The designed Cu‐CoP exhibits yield 7.65 mg h −1 cm −2 Faraday efficiency 85.1% at −1.0 V (10 m M ), which is highest reported data. In situ characterization theoretical calculations confirm effect, site favors activation form 2 , concurrently modulates electronic structure Co with optimized H enhanced

Язык: Английский

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Dynamically Restructuring Nanoporous Cu–Co Electrocatalyst for Efficient Nitrate Electroreduction to Ammonia

ACS Catalysis, Год журнала: 2024, Номер 14(16), С. 12251 - 12259

Опубликована: Авг. 1, 2024

The electrochemical nitrate (NO3–) reduction reaction (NITRR) to ammonia (NH3) offers an environmentally friendly alternative for NH3 synthesis but suffers from limited yield and low Faradaic efficiency (FE) due the sluggish kinetics of hydrogenation process. Herein, nanoporous Cu/CoOOH heterostructure is reported as efficient electrocatalyst NITRR. catalyst achieves a high rate 275.9 μmol h–1 cm–2 (689.8 mmol gcat–1) 836.8 (2092.0 gcat–1), with corresponding FE values 85.3 91.5% in 200 1400 ppm NO3–-N electrolyte, respectively. In situ Raman spectra reveal that derived synergistic chemical/electrochemical redox between NO3– CuCo alloy during NITRR Theoretical simulations indicate exhibits enhanced *NO2 affinity reduces energy barrier rate-determining *NO2H formation step, effectively facilitating NH3.

Язык: Английский

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Self-Triggering a Locally Alkaline Microenvironment of Co₄Fe₆ for Highly Efficient Neutral Ammonia Electrosynthesis

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

Опубликована: Фев. 28, 2025

Electrochemical nitrate reduction reaction (eNO3-RR) to ammonia (NH3) holds great promise for the green treatment of NO3- and ambient NH3 synthesis. Although Fe-based electrocatalysts have emerged as promising alternatives, their excellent eNO3-RR-to-NH3 activity is usually limited harsh alkaline electrolytes or alloying noble metals with Fe in sustainable neutral electrolytes. Herein, we demonstrate an unusual self-triggering localized alkalinity Co4Fe6 electrocatalyst efficient media, which breaks down conventional pH-dependent kinetics restrictions shows a 98.6% Faradaic efficiency (FE) 99.9% selectivity at -0.69 V vs RHE. The synergetic Co-Fe dual sites were demonstrated enable optimal free energies species balance water dissociation protonation adsorbed NO2-. Notably, can attain high current density 100 mA cm-2 FE surpassing 96% long-term stability over 500 h membrane electrode assembly (MEA) electrolyzer. This work provides insight into tailoring self-reinforced local-alkalinity on alloy thus avoids practical upcycling technology.

Язык: Английский

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Palladium Married with MBene Multilayers: Enabling Intensified Hydrogen Spillover for Efficient Nitrite‐to‐Ammonia Electroreduction

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Апрель 8, 2025

Abstract Electrochemical nitrite reduction reaction (NO 2 RR) has emerged as a promising alternative approach for ammonia (NH 3 ) production, offering both energy efficiency and environmental sustainability. The rational regulation of active hydrogen (*H) is pivotal NO − ‐to‐NH conversion, yet it remains significant challenge in the context RR. In this study, molybdenum boride (MBene) multilayers are introduced an electronic support to integrate with palladium (Pd) nanoparticles, creating dual catalytic sites that effectively balance adsorption *H *NO , thereby enabling synergistic catalysis Theoretical experimental analyses revealed efficiently generated on Pd subsequently undergoes spillover ‐adsorbed MBene surfaces, facilitating accelerated hydrogenation NH synthesis. Consequently, Pd/MBene catalyst demonstrated exceptional performance, achieving high Faradaic 89%, yield rate 16.9 mg h −1 cat remarkable cycling stability at low applied potential ‐0.3 V versus RHE. Motivated by outstanding RR further utilized cathode construct Zn‐nitrite formaldehyde‐nitrite batteries. These systems functionality simultaneous production electricity generation, highlighting versatile efficient sustainable conversion.

Язык: Английский

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Engineering Nickel Dopants in Atomically Thin Molybdenum Disulfide for Highly Efficient Nitrate Reduction to Ammonia

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Сен. 16, 2024

Abstract The electrocatalytic nitrate reduction reaction (NO 3 − RR) presents a promising pathway for achieving both ammonia (NH ) electrosynthesis and water pollutant removal simultaneously. Among various electrocatalysts explored, 2D materials have emerged as candidates due to their ability regulate electronic states active sites through doping. However, the impact of doping effects in on mechanism NO RR remains relatively unexplored. Here, Ni‐doped MoS 2 (Ni‐MoS nanosheets are investigated model system, demonstrating enhanced performance compared undoped counterparts. By controlling concentration, Ni‐MoS achieve remarkable faradic efficiency (FE) 92.3% NH at −0.3 V RHE with excellent stability. mechanistic studies reveal that elevation performances originates from generation more hydrogen acceleration nitrite facilitated by Ni Combining experimental observations theoretical calculations it is revealed appropriate level can enhance *NO adsorption strength, thereby facilitating subsequent steps. Together demonstration Zn−NO battery devices, work provides new insights into design regulation material catalysts efficient RR.

Язык: Английский

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Highly Efficient Electrocatalytic Nitrate Reduction to Ammonia: Group VIII-Based Catalysts

ACS Nano, Год журнала: 2024, Номер unknown

Опубликована: Окт. 4, 2024

The accumulation of nitrates in the environment causes serious health and environmental problems. electrochemical nitrate reduction reaction (e-NO

Язык: Английский

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Electrocatalysis for sustainable nitrogen management: materials innovation for sensing, removal and upcycling technologies

Science China Chemistry, Год журнала: 2024, Номер unknown

Опубликована: Сен. 9, 2024

Язык: Английский

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