Nickel-copper alloying arrays realizing efficient Co-electrosynthesis of adipic acid and hydrogen

Journal of Energy Chemistry, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 1, 2024

Language: Английский

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Spatially Separated Cu/Ru on Ordered Mesoporous Carbon for Superior Ammonia Electrosynthesis from Nitrate over a Wide Potential Window

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(36), P. 24966 - 24977

Published: Aug. 28, 2024

Nitrate (NO3–) in wastewater poses a serious threat to human health and the ecological environment. The electrocatalytic NO3– reduction ammonia (NH3) reaction (NO3–RR) emerges as promising carbon-free energy route for enabling removal sustainable NH3 synthesis. However, it remains challenge achieve high Faraday efficiencies at wide potential window due complex multiple-electron process. Herein, spatially separated dual-metal tandem electrocatalysts made of nitrogen-doped ordered mesoporous carbon support with ultrasmall high-content Cu nanoparticles encapsulated inside large low-content Ru dispersed on external surface (denoted Ru/Cu@NOMC) are designed. In NO3–RR, sites can quickly convert adsorbed NO2– (*NO2–), while efficiently produce active hydrogen (*H) enhance kinetics converting *NO2– sites. Due synergistic effect between sites, Ru/Cu@NOMC exhibits maximum Faradaic efficiency (FENH3) approximately 100% −0.1 V vs reversible electrode (RHE) yield rate 1267 mmol gcat–1 h–1 −0.5 RHE. Finite element method (FEM) simulation electrochemical situ Raman spectroscopy revealed that framework intermediate concentration confinement effect. Thanks Cu–Ru mesopore effect, 500 mV FENH3 over 90% superior stability production 156 h be achieved catalyst.

Language: Английский

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Interface Engineering of the Cu_1.5Mn_1.5O₄/CeO₂ Heterostructure for Highly Efficient Electrocatalytic Nitrate Reduction to Ammonia

Nano Letters, Journal Year: 2024, Volume and Issue: 24(29), P. 8964 - 8972

Published: July 10, 2024

The electrochemical nitrate reduction reaction (NO

Language: Английский

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Boosting Electrochemical Urea Synthesis via Cooperative Electroreduction Through the Parallel Reduction

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 16, 2025

Abstract Despite recent achievements in the co‐reduction electrosynthesis of urea from nitrogen wastes and CO 2 , selectivity yield products remain fairly average because competition NITRR, RR, HER. Here, a strategy involving FeNC catalysts disperse with oxygen‐vacancy‐rich CeO (FeNC‐Ce) is illustrated, which reversible hydrogenation defects, bimetallic catalytic centers enable spontaneous switching between reduction paths NO 3 − . The FeNC‐Ce electrocatalyst exhibits an extremely high Faraday efficiency (FE) 20969.2 µg mg −1 h 89.3%, respectively, highly superior to most reported values (maximum 200–2300 FE max 11.5%–83.4%). study findings, rationalize by situ spectroscopy theoretical calculations, are rooted evolution dynamic NITRR RR protons, alleviating overwhelming single‐system reactants thereby minimizing formation by‐products.

Language: Английский

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Bimetal anchoring porous MXene nanosheets for driving tandem catalytic high‐efficiency electrochemical nitrate reduction

AIChE Journal, Journal Year: 2024, Volume and Issue: 71(2)

Published: Oct. 17, 2024

Abstract Electrochemical nitrate reduction reaction (NO 3 RR) is considered a promising strategy for ammonia synthesis and removal, in which catalyst development crucial. Herein, series of bimetal (Co Cu) anchoring porous MXene nanosheets x Cu y @PM) catalysts were prepared by combining etching strategy. On the one hand, Co bimetals provided tandem catalytic active sites NO RR. other in‐plane PM exhibited good electrical conductivity multiple transport pathways. Consequently, optimized 7 @PM achieved high yield 7.43 mg h −1 cat. an excellent Faraday efficiency (FE) 95.9%. The mechanism RR was investigated analyzing electrolysis products situ Fourier transform infrared spectroscopy. Furthermore, based ZnNO − battery superior power density 5.59 mW cm −2 NH FE 92.3%. This work presents effective to design MXene‐based high‐performance electrocatalysts.

Language: Английский

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Cu‐Ru Bicenter Synergistically Triggers Tandem Catalytic Effect for Electroreduction of Nitrate to Ammonium

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 10, 2025

Abstract The electrochemical transformation of nitrate (NO 3 − ) into ammonia (NH holds significant promise to addresses nitration contamination and offers a sustainable alternative the Haber–Bosch process. However, sluggish kinetics hinders its large‐scale application. Herein, Cu‐doped SrRuO synergetic tandem catalyst is designed synthesized, which demonstrates exceptional performance in converting NO NH . Specifically, this achieves maximum Faradaic efficiency 95.4% for production, along with high yield rate 7196 µg h −1 mg cat. A series detailed characterizations reveals that doped Cu ions modify local electronic environment Ru 4 d e g orbital , thereby facilitating highly efficient electron transfer processes. In situ delta X‐ray absorption near‐edge structure (ΔXANES), synchrotron radiation‐based Fourier transform infrared (SR‐FTIR) Raman spectroscopy identified * 2 generated on active sites subsequently hydrogenated sites. Combined theoretical studies, it confirmed significantly reduces energy barriers rate‐determining step ( NOH), enhancing synthesis. This work not only fundamental insights mechanisms cation substitution regulating perovskite catalysts, but also provides promising avenue electro‐synthesis ammonia.

Language: Английский

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Boosting electrocatalytic nitrate reduction to ammonia with a Cu/Ag-Ru tandem catalyst at industrial-scale current density

Journal of Materials Chemistry A, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

For a tandem electrode of (Cu 7 /Ag 3 ) -Ru /C, the heterostructure maximized formation NO 2 − , and Ru nanoparticles exhibited excellent adsorption water dissociation, facilitating hydrogenation avoiding HER.

Language: Английский

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Gelatin‐Induced Synthesis of Strain‐Engineered Spherical Cu₂O Nanoparticles for Efficient Nitrate Reduction to Ammonia

Small, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 29, 2025

The electrochemical reduction of nitrate to ammonia offers an environmentally sustainable pathway for nitrogen fixation. However, achieving both efficiency and selectivity in presents a formidable challenge, due the involvement sluggish multielectron transfer processes. Herein, successful synthesis spherical Cu₂O nanoparticles (s-Cu₂O) exhibiting significant compressive strain effects, achieved through one-pot method using gelatin as structural modifier, is reported. s-Cu₂O catalyst demonstrates exceptional performance reaction (NO3RR), Faradaic (FENH3) 95.07%, 92.03%, conversion rate 97.77%, yield 284.83 µmol h⁻¹ cm⁻2 at -0.8 V versus reversible hydrogen electrode (vs. RHE) production. Structural characterization density functional theory calculations reveal that plays critical role modulating electronic structure catalyst, thereby activating *NO intermediate potential determining step effectively suppressing evolution reaction. Furthermore, it implemented Zn-NO3 - battery, test results indicate battery peak power 3.95 mW cm-2 0.129 (vs Zn/Zn2⁺), illustrating its excellent efficacy. This work introduces novel strategy rational design high-performance electrocatalysts engineering, offering broad implications energy-efficient synthesis, cycling.

Language: 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, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 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).

Language: Английский

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Regulation of Active Hydrogen and Nitrate Concentration: Pulsed Potential Strategies in Nitrate Electroreduction Microenvironments

Research Square (Research Square), Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 20, 2025

The electrochemical reduction of nitrate (NO₃RR) plays a significant role in the nitrogen cycle and environmental remediation. dynamics active hydrogen NO₃RR were studied depth by varying concentration applying pulsed-potential approach. effect both factors on regulation degree hydrogenation intermediates product distribution was evaluated. Density functional theory (DFT) calculations indicated that elevated levels decrease energy barrier for *NO to *N conversion, enhancing *N₂ formation. experimental results indicate under high concentrations, copper-palladium (CuPd) catalysts exhibit faster reaction kinetics higher selectivity. In-situ characterizations illuminated critical intermediates. CuPd catalyst achieved 95% NO₃-N conversion 99% N₂ selectivity at 1 M pulse potential modulation surface. Finite element analysis (FEA) verified pulsed potentials modulate local ion concentrations. present work brings closer practical applications, aiding protection balance cycle.

Language: Английский

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