Enhancing Compatibility of Two‐Step Tandem Catalytic Nitrate Reduction to Ammonia Over P‐Cu/Co(OH)₂

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 11, 2024

Abstract Electrochemical nitrate reduction reaction (NO 3 RR) is a promising approach to realize ammonia generation and wastewater treatment. However, the transformation from NO − NH involves multiple proton‐coupled electron transfer processes by‐products 2 , H etc.), making high selectivity challenge. Herein, two‐phase nanoflower P‐Cu/Co(OH) electrocatalyst consisting of P‐Cu clusters P‐Co(OH) nanosheets designed match two‐step tandem process ) more compatible, avoiding excessive accumulation optimizing whole reaction. Focusing on initial 2e process, inhibited * desorption Cu sites in gives rise appropriate released electrolyte. Subsequently, exhibits superior capacity for trapping transforming desorbed during latter 6e due thermodynamic advantage contributions active hydrogen. In 1 m KOH + 0.1 leads yield rate 42.63 mg h cm Faradaic efficiency 97.04% at −0.4 V versus reversible hydrogen electrode. Such well‐matched achieves remarkable synthesis performance perspective catalytic reaction, offering novel guideline design RR electrocatalysts.

Language: Английский

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Homogeneously Mixed Cu–Co Bimetallic Catalyst Derived from Hydroxy Double Salt for Industrial-Level High-Rate Nitrate-to-Ammonia Electrosynthesis

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(40), P. 27417 - 27428

Published: Aug. 23, 2024

Electrocatalytic nitrate reduction reaction (NO

Language: Английский

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Promoting active hydrogen supply for kinetically matched tandem electrocatalytic nitrate reduction to ammonia

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 360, P. 124528 - 124528

Published: Aug. 24, 2024

Language: Английский

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Achieving efficient urea electrosynthesis through improving the coverage of a crucial intermediate across a broad range of nitrate concentrations

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(14), P. 5183 - 5190

Published: Jan. 1, 2024

A novel Ru–Cu 9 Bi/CNT multi-site alloy is synthesised for electrocatalytic C–N coupling to generate urea across a broad range of NO 3 − concentrations. By improving the coverage key intermediate *NHO, ensure subsequent electrosynthesis urea.

Language: Английский

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Ammonia electrosynthesis from nitrate using a stable amorphous/crystalline dual-phase Cu catalyst

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: Jan. 21, 2025

Renewable energy-driven electrocatalytic nitrate reduction reaction presents a low-carbon and sustainable route for ammonia synthesis under mild conditions. Yet, the practical application of this process is currently hindered by unsatisfactory activity long-term stability. Herein we achieve high-rate electrosynthesis using stable amorphous/crystalline dual-phase Cu catalyst. The partial current density formation rate reach 3.33 ± 0.005 A cm-2 15.5 0.02 mmol h-1 at low cell voltage 2.6 0.01 V, respectively. Remarkably, catalyst can maintain production with Faradaic efficiency around 90% high 1.5 up to 300 h. scale-up demonstration an electrode size 100 cm2 achieves as 11.9 0.5 g total 160 A. impressive performance ascribed presence amorphous domains which promote adsorption hydrogenation nitrogen-containing intermediates, thus improving kinetics formation. This work underscores importance stabilizing metastable structures reactivity

Language: Английский

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Interfacial Water Regulation for Nitrate Electroreduction to Ammonia at Ultralow Overpotentials

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

Published: Jan. 8, 2025

Abstract Nitrate electroreduction is promising for achieving effluent waste‐water treatment and ammonia production with respect to the global nitrogen balance. However, due impeded hydrogenation process, high overpotentials need be surmounted during nitrate electroreduction, causing intensive energy consumption. Herein, a hydroxide regulation strategy developed optimize interfacial H 2 O behavior accelerating conversion of at ultralow overpotentials. The well‐designed Ru─Ni(OH) electrocatalyst shows remarkable efficiency 44.6% +0.1 V versus RHE nearly 100% Faradaic NH 3 synthesis 0 RHE. In situ characterizations theoretical calculations indicate that Ni(OH) can regulate structure promoted dissociation process contribute spontaneous hydrogen spillover boosting NO − Ru sites. Furthermore, assembled rechargeable Zn‐NO /ethanol battery system exhibits an outstanding long‐term cycling stability charge–discharge tests high‐value‐added ammonium acetate, showing great potential simultaneously removal, conversion, chemical synthesis. This work not only provide guidance in extensive reactions but also inspire design novel hybrid flow multiple functions.

Language: Английский

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Tailoring Electronic and Morphology Features of Iron‐Doped Ni₂P Nanoflowers for Enhanced Ammonia Electrosynthesis in Solid Electrolyte Reactors

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

Published: Feb. 13, 2025

Abstract Electrochemical nitrate (NO 3 − ) reduction to ammonia (NH presents a promising route for both wastewater treatment and generation but still suffers from sluggish catalytic activity, insufficient mass transfer, the reliance on high‐concentration supporting electrolytes. This work reports an innovative efficient electrosynthesis reactor by integrating self‐assembled iron‐doped Ni 2 P (Fe‐Ni P/NF) nanoflower cathode with solid‐electrolyte (SE). The SE design eliminates need electrolytes, providing highly ion‐conducting pathway enabling direct production of NH NO . Through tailoring electronic surface characteristics Fe‐Ni P/NF, this achieves complete reduction, 96.7% selectivity, 81.8% faradaic efficiency concentration 100 m at current density mA −2 Density functional theory (DFT) calculations reveal that phosphating Fe doping synergistically enhance adsorption increase availability active hydrogen, thus favoring low energy barrier 0.695 eV. Additionally, superhydrophilicity P/NF catalyst promotes transfer facilitating electrolyte access ensuring rapid gas bubble release. study provides sustainable scalable method converting ‐laden into valuable products.

Language: Английский

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Subnanometric Nickel Phosphide Heteroclusters with Highly Active Ni^δ+–P^δ− Pairs for Nitrate Reduction toward Ammonia

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: March 26, 2025

The development of efficient electrocatalysts for the neutral nitrate reduction reaction (NO3–RR) toward ammonia (NH3) is essential to address environmental issues caused by NO3– but remains considerably challenging owing sluggish kinetics NO3–RR in media. Herein, we report subnanometric heteroclusters with strongly coupled nickel–phosphorus (Ni–P) dual-active sites as boost NO3–RR. Experimental and theoretical results reveal that feature Ni–P promotes electron transfer from Ni P, generating Niδ+–Pδ− active pairs, which Niδ+ species are highly Pδ− tunes interfacial water hydrogen bonding network promote dissociation step accelerate proton during Consequently, NO3–RR, exhibit a large NH3 yield rate 0.61 mmol h–1 cm–2 at −0.8 V versus reversible electrode, 2.8- 3.3-fold larger than those on nanoparticles clusters, respectively, generated exists NH4+ electrolytes. This study offers an approach boosting electrocatalytic reactions multiple intermediates designing sites.

Language: Английский

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Regulating the Electrochemical Nitrate Reduction Performance with Controllable Distribution of Unconventional Phase Copper on Alloy Nanostructures

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 6, 2024

Abstract Electrochemical nitrate reduction reaction (NO 3 RR) is emerging as a promising strategy for removal and ammonia (NH ) production using renewable electricity. Although great progresses have been achieved, the crystal phase effect of electrocatalysts on NO RR remains rarely explored. Here, epitaxial growth unconventional 2H Cu hexagonal close‐packed ( hcp IrNi template, resulting in formation three IrNiCu@Cu nanostructures, reported. IrNiCu@Cu‐20 shows superior catalytic performance, with NH Faradaic efficiency (FE) 86% at −0.1 (vs reversible hydrogen electrode [RHE]) yield rate 687.3 mmol g −1 h , far better than common face‐centered cubic Cu. In sharp contrast, IrNiCu@Cu‐30 IrNiCu@Cu‐50 covered by shell display high selectivity toward nitrite 2 − ), FE above 60% 0.1 RHE). Theoretical calculations demonstrated that has optimal electronic structures due to highest d‐band center strongest trend lowest energy barriers. The electroactivity originates from abundant low coordination sites surface, which guarantees fast electron transfer accelerate intermediate conversions. This work provides feasible tactic regulate product distribution engineering electrocatalysts.

Language: Английский

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In‐situ Reconstruction of Catalyst in Electrocatalysis

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 22, 2024

Abstract Reconstruction of catalysts is now well recognized as a common phenomenon in electrocatalysis. As the reconstructed structure may promote or hamper electrochemical performance, how to achieve designed active surface for highly enhanced catalytic activity through reconstruction needs be carefully investigated. In this review, genesis and effects various processes, such hydrogen evolution reaction (HER), oxygen (OER), carbon dioxide reduction (CO 2 RR), nitrate (NO 3 RR) are first described. Then, strategies optimizing reconstruction, valence states control, phase retention, engineering, poisoning prevention comprehensively discussed. Finally, general rules optimization summarized give perspectives future study. It believed that review shall provide deep insights into electrocatalytic mechanisms guide design pre‐catalysts with improved activity.

Language: Английский

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