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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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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Interface Engineering on Heterostructural Nanosheets for Efficient Electrocatalytic-Paired Upcycling of Waste Plastics and Nitrate

ACS Catalysis, Год журнала: 2024, Номер unknown, С. 18095 - 18106

Опубликована: Ноя. 22, 2024

Язык: Английский

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In Situ Reconstructed Cu/β‐Co(OH)₂ Tandem Catalyst for Enhanced Nitrate Electroreduction to Ammonia in Ampere‐Level

Advanced Energy Materials, Год журнала: 2024, Номер 14(41)

Опубликована: Авг. 7, 2024

Abstract The electrochemical nitrate reduction for green ammonia production is attracting increasing attention, where the catalysts are widely investigated by controlling compositions or structures to achieve high performance. However, their reconstructions under potentials inevitable and uncontrollable, leading uncertain performance, a confused understanding of mechanism. In this work, strategy proposed pre‐catalyst's reconstruction chemistry toward reaction (e‐NO 3 RR) with superior activity stability. To demonstrate idea, pre‐catalyst fabricated α ‐Co(OH) 2 Cu(OH) ( /Cu(OH) ), which in situ reconstructed tandem catalyst Cu β (Cu/ β‐ Co(OH) ) working potential. Cu/ achieves an optimal Faraday efficiency 97.7% yield rate 3.9 mmol h −1 cm −2 at −0.5 V, outperforming other reported metal‐hydroxide catalysts. experimental theoretical results that catalytic mechanism responsible exceptional performance: 1) functions as donor nitrite; 2) serves active sites generating hydrogen reducing nitrogen‐containing groups. This work highlights controllable improved performance can be realized, provides insightful mechanism, helpful developing stable various applications.

Язык: Английский

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

AIChE Journal, Год журнала: 2024, Номер 71(2)

Опубликована: Окт. 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.

Язык: Английский

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Regulating Interfacial H₂O Activity and H₂ Bubbles by Core/Shell Nanoarrays for 800 h Stable Alkaline Seawater Electrolysis

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Март 24, 2025

Abstract The catalytic activity and stability under high current densities for hydrogen evolution reactions (HER) are impeded by firm adherence coverage of H 2 bubbles to the sites. Herein, we systematically synthesize core/shell nanoarrays engineer bubble transport channels, which further remarkably regulate interfacial O activity, swift generation release. self‐supported catalyst holds uniform ultra‐low Ru active sites 0.38 wt% promotes rapid formation plentiful small bubbles, rapidly released upright mitigating blockage avoiding surface damage from movements. As a result, these achieve ultralow overpotentials 18 24 mV reach 10 mA cm −2 HER in 1 M KOH freshwater seawater, respectively. Additionally, assembled electrolyzer demonstrates stable durability over 800 hours with density A seawater. techno‐economic analysis (TEA) indicates that unit cost production system is nearly half DOE's (Department Energy) 2026 target. Our work addresses challenges highlights its potential as sustainable economically feasible solution large‐scale

Язык: Английский

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Two‐Step Tandem Catalysis for High‐Efficiency Ammonia Synthesis Via Nitrate Reduction on Anion‐Intercalated CoNi LDH and Cu/Cu₂O

Advanced Science, Год журнала: 2025, Номер unknown

Опубликована: Апрель 15, 2025

Abstract Ammonia is essential across industry, agriculture, and as a future carbon‐free energy carrier. Electrocatalytic nitrate reduction (NitRR) offers sustainable path for removing contaminants from wastewater groundwater while using abundant ions nitrogen sources under eco‐friendly conditions. However, the NitRR pathway, which involves sequential reactions, poses challenges in synchronizing rate of nitrate‐to‐nitrite conversion with subsequent nitrite to ammonia, particularly initial step rate‐limiting. This study presents CoNi layered double hydroxide (LDH) approach finely control hydrogen radical (*H) supply, paired Cu/Cu 2 O redox coupling, achieve optimal matching. LDH engineered various anion intercalations (NO 3 − , Cl SO 4 2− MoO WO ) regulate *H capacity. By integrating LDH, tandem kinetic descriptors, including volcano curve, are employed predict constants, facilitating ideal matching efficient ammonia synthesis. The optimized ‐CoNi LDH/CuO NW/CF electrode demonstrated exceptional performance, achieving 99.78% Faraday efficiency, yield 1.12 mmol cm −2 h −1 at −0.2 V vs. RHE, robust 14‐h stability. model descriptors effectively elucidated linking reaction rates factors impacting production.

Язык: Английский

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

Journal of Colloid and Interface Science, Год журнала: 2024, Номер 682, С. 703 - 714

Опубликована: Ноя. 29, 2024

Язык: Английский

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Preparation of a branched hierarchical Co3O4@Fe2O3 core–shell structure with high-density catalytic sites for efficient catalytic conversion of nitrate in wastewater to ammonia

Chemical Engineering Journal, Год журнала: 2024, Номер 499, С. 156495 - 156495

Опубликована: Окт. 9, 2024

Язык: Английский

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Precise structural regulation of copper-based electrocatalysts for sustainable nitrate reduction to ammonia

Environmental Research, Год журнала: 2024, Номер 266, С. 120422 - 120422

Опубликована: Ноя. 22, 2024

Язык: Английский

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