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

Advanced Science, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 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

Language: Английский

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Nanoflower‐Like CuPd/CuO Heterostructure for an Energy‐Output Electrocatalytic System Coupling Ammonia Electrosynthesis and Zinc‐Nitrate Battery

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

Published: March 18, 2025

Abstract Electrochemical nitrate reduction reaction (NO 3 RR) can effectively alleviate pollution and simultaneously realize ammonia electrosynthesis at room temperature. However, it remains a significant challenge for NO RR to achieve high Faradic efficiency in full concentration range. Herein, nanoflower‐like copper‐palladium alloy/CuO heterostructure (CuPd/CuO@NF) is successfully fabricated by the hydrothermal synthesis of CuO nanoflowers subsequent formation CuPd alloy. The as‐obtained CuPd/CuO@NF exhibits remarkable electrochemical performance − ‐N range from 20 1400 ppm, especially with conversion rate 97.8% NH selectivity 99.3% 94.2% yield 1.37 mmol h −1 cm −2 ppm. In‐situ Fourier transform infrared spectroscopy Raman spectra reveal that first catalyzes 2 , which rapidly reduced forming *NH, *NH OH intermediates. Density functional theory calculations suggest NHO route thermodynamically favorable. When applied zinc‐nitrate battery, demonstrates maximum power density 53.7 mW 99.9% 94.4%. This work offers valuable insights into design novel electrocatalysts batteries.

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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Enabling High Performance in a Positive Potential of Nitrate‐to‐Ammonia Electrocatalysis Over Mesoporous Core@Shell Cu₂O/Cu@PdCu Nanozyme

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

Published: April 2, 2025

Electrocatalytic tandem nitrate reduction to ammonia (NO3 --to-NH3) offers a promising pathway for energy and environmental sustainability. Although considerable efforts have been presented modulate the reaction pathways enhanced NO3 --to-NH3 electrocatalysis, these advances often require relatively high overpotentials balance yield rate selectivity of NH3, resulting in remarkable inefficiency. Inspired by enzyme catalysis nature, herein enzyme-like electrocatalyst is designed consisting core Cu2O/Cu heterojunction surrounded mesoporous PdCu shell (Cu2O/Cu@mesoPdCu) that accelerated electrocatalysis positive potentials. Impressively, Cu2O/Cu@mesoPdCu nanozymes hold superior performance robust NH3 electrosynthesis fairly potential 0.10 V (versus reversible hydrogen electrode), having Faraday efficiency 96.2%, 13.3 mg h-1 mg-1, half-cell 46.0%. Kinetic studies, situ spectra density functional theory calculations revealed preferentially adsorbed - further reduced *NO2, while active radicals enriched on promoted multistep hydrodeoxygenation *NO2 within "semi-closed" microenvironment, both which synergistically enabled Moreover, this disclosed better more energy-efficient manner when coupling with thermodynamically favorable ethanol oxidation reaction.

Language: Английский

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A Cu/Fe3O4@CN tandem catalyst for efficient ammonia electrosynthesis from nitrate reduction

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 682, P. 703 - 714

Published: Nov. 29, 2024

Language: Английский

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