Construction of ternary alloy Cu-Ni-Co catalysts with highly active sites to enhance the initial adsorption process of nitrate reduction to ammonia

Electrochimica Acta, Год журнала: 2024, Номер 486, С. 144124 - 144124

Опубликована: Март 15, 2024

Язык: Английский

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Conductivity-mediated in situ electrochemical reconstruction of CuO_x for nitrate reduction to ammonia

Nanoscale, Год журнала: 2024, Номер 16(29), С. 13895 - 13904

Опубликована: Янв. 1, 2024

CP/CuO x with suitable copper valence states obtained by fine-tuning the conductivity of electrochemical reconstruction may provide a competitive cathode catalyst for achieving excellent activity and selectivity NO 3 − -to-NH conversion.

Язык: Английский

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Single-, Double-, and Triple-atom Catalysts on PC6 for Nitrate Reduction to Ammonia: A Computational Screening

Electrochimica Acta, Год журнала: 2024, Номер 504, С. 144915 - 144915

Опубликована: Авг. 15, 2024

Язык: Английский

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A Cascade Jet Plasma Oxidation─electroreduction System Using Pd‐Ni Dual‐Site Catalyst for Sustainable Ammonia Production from Air

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Авг. 2, 2024

Abstract Electrocatalytic N 2 reduction reaction (eNRR) has been deemed as an alternative approach to the Haber‐Bosch (H‐B) process for ammonia (NH 3 ) production, but it remains a huge challenge. Here jet plasma oxidation of is reported in air into NO x and subsequently − coupling with electrochemical (pN ─eNO RR) over PdNi alloying nanoparticles on N‐doped carbon nanotubes (PdNi/N‐CNTs) NH synthesis. The results demonstrate that reactor possesses excellent gas reforming capacity achieve largest yield rate 30.46 mmol h −1 low energy consumption 2.66 kWh mol . For subsequent eNO RR, PdNi/N‐CNTs can afford 34.96 mg cat. faradaic efficiency (FE) 98.21% at −0.38 0.02 V (vs RHE), respectively. In situ spectroscopic characterizations combined theoretical calculations unveil provide Pd Ni dual active sites, enabling activation site H * provision facilitate RR. A cascade pN ‐eNO RR system constructed sustainable achieving stable 25.56 , average FE >85%, well conversion 44.62% constant ampere‐level current finally collection gram‐level 4 SO product.

Язык: Английский

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Optimizing Nitrate Reduction to Ammonia via Modulating Adsorption–Desorption Dynamics with High-Entropy CuNiCoZnMn Alloy Catalysts

ACS Applied Materials & Interfaces, Год журнала: 2024, Номер 16(33), С. 43526 - 43534

Опубликована: Авг. 8, 2024

NO3RR synthesis of ammonia is a complex eight-electron reaction involving multiple steps and intermediates, in which NO3– adsorption NH3 desorption are crucial. The Cu-based high entropy quinary alloy catalyst has good surface ability for the reduction nitric acid to ammonia. Here, catalytic sites were coordinated by constructing CuNiCoZnMn alloys adjust electronic structure facilitate substrate thus optimize whole path. Based on ternary CuNiCo, introduction Zn element continues reduce energy barrier, Mn enhance initial so that target product can be quickly held released accelerate production yield Faraday efficiency obtained reached 723.7 μmol h–1 cm–2 96.6%, respectively, at −0.35 V vs RHE potential. density functional theory calculations showed (NO3– *NO3–) adsorption-free change (*NH3 NH3) desorption-free −2.50, 0.072 eV, significantly better than those CuNiC quaternary CuNiCoZn −2.02, 0.544 eV −1.97, 0.217 eV.

Язык: Английский

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High-entropy FeCoNiCuRu solid solutions triggered cocktail effect to achieve fine-tuning adsorption energy for boosting nitrate electroreduction to ammonia

Chemical Engineering Journal, Год журнала: 2024, Номер 500, С. 157426 - 157426

Опубликована: Ноя. 1, 2024

Язык: Английский

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Stepwise H*-Mediated and Non-H* Reduction Processes for Highly Selective Transformation of Nitrate to Nitrogen Gas Using a ZVAl-Based Material

Environmental Science & Technology, Год журнала: 2025, Номер unknown

Опубликована: Фев. 6, 2025

Improving the reduction efficiency and N2 selectivity is important for nitrate decontamination. A novel ternary ball-milled Al-Cu-AC material reported to achieve a highly selective of N2. The process, driven by continuous dissolution zero-valent aluminum (ZVAl), demonstrated stepwise scheme. interesting shift in electron-donating pathways was ascribed spontaneous change microenvironmental pH from neutral alkaline. (1:1:5 mass ratio) completely removed 30 mg/L NO3--N over wide range (5-9), achieving 83% TN removal N2-selectivity, without detectable copper leaching. atomic hydrogen (H*)-mediated occurring on Cu component proven be crucial fast transformation NO3- NO2-, while non-H* process dominated electrochemical NO2- AC cathode Al || microgalvanic cells formed material. primary route identified as *NOH pathway, superiority toward verified with actual wastewater. This study revealed how influenced ZVAl provides new approach maximize performance metals.

Язык: Английский

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A Cu‐Cu₂O/Ni₂P Heterostructure for Efficient Tandem Catalysis of Electrosynthesis of Ammonia from Nitrate Reduction Reaction in Neutral Medium

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Фев. 9, 2025

Abstract Electrochemical nitrate reduction to ammonia (eNO 3 RR) in neutral conditions is an effective and sustainable method for production while treating pollution. Nevertheless, it still faces a great challenge due the complicated multiple proton‐coupled‐electron process eNO RR. Herein, efficient heterostructure electrocatalyst Cu‐Cu 2 O/Ni P has been successfully fabricated electrosynthesis from reduction. exhibits outstanding RR performance with Faradaic efficiency (FE) as high 96.4% yield rate of 14636 µg·h −1 ·cm −2 at −1.0 V (vs RHE) 0.1 m PBS solution, which outperforms most reported electrocatalysts media. More importantly, catalyst demonstrates exceptional stability 30 consecutive electrolysis cycles durability even large current density 440 mA cm flow cell. The tandem catalysis mechanism NO − → NH by synergism two components O Ni verified experimental theoretical calculations. strong adsorption capacity can be reduced into , facilitate water splitting, promotes abundant *H production, thus boosting subsequent hydrogenation during whilst inhibiting competitive hydrogen evolution reaction (HER).

Язык: Английский

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Electrodeposited P‐Doped CuNi Alloy from Deep Eutectic Solvent for Efficient and Selective Nitrate‐to‐Ammonia Electroreduction

Small, Год журнала: 2025, Номер unknown

Опубликована: Март 7, 2025

Electrochemical nitrate reduction reaction (NO3RR) offers a promising alternative for ammonia production using electricity generated from renewable energy sources. Active electrocatalysts with high selectivity and yield are required to selectively catalyze NO3RR ammonia. Here, P-doped Cu0.51Ni0.49 alloy thin films electrodeposited deep eutectic solvent of choline chloride-ethylene glycol (ChCl/EG). The P-Cu0.51Ni0.49 produces 1616.94 µg h-1 cm-2 at -0.55 VRHE (V versus reversible hydrogen electrode), Faradaic efficiency 98.38% 97.84% -0.25 VRHE, much better than the P-Ni P-Cu prepared under similar condition. rate, originated number electrochemically active sites more facile kinetics. Mechanistic study density functional theory calculation proves that exhibits higher conductivity NO3 - adsorption compared P-Cu, induced by electron interaction. Characterizations after cycling show crystallinity decreases, content divalent metal ions increases surface. is an stable material electrocatalyze in neutral aqueous solutions.

Язык: Английский

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Surface reconstruction induced Cu2O/FeO heterojunction towards efficient nitrate-containing wastewater remediation

Journal of Colloid and Interface Science, Год журнала: 2025, Номер unknown, С. 137318 - 137318

Опубликована: Март 1, 2025

Язык: Английский

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