Accelerating proton coupled electron transfer by confined Cu-Ni bimetallic clusters for boosting electrochemical hydrodeoxygenation of nitrate

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125195 - 125195

Published: Feb. 1, 2025

Language: Английский

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Metastable Phase Noble-Metal-Free Core–Shell Structure for Efficient Electrocatalytic Nitrobenzene Transfer Hydrogenation

Nano Letters, Journal Year: 2025, Volume and Issue: 25(9), P. 3383 - 3390

Published: Feb. 19, 2025

In order to study the catalytic behavior of a metastable-phase catalyst in electrocatalytic hydrogenation, we report new noble-metal-free core–shell with metastable hexagonal closest packed (hcp) phase Ni as shell and face-centered-cubic (fcc) Cu core (Cu@hcp NPs) for hydrogenation nitrobenzene (Ph-NO2) aniline (Ph-NH2). Using H2O hydrogen source, it achieves up 99.63% Ph-NO2 conversion ∼100% Ph-NH2 selectivity, an improved activity turnover frequency (TOF: 6640 h–1), much higher than those hcp NPs (5183.7 h–1) commercial Pt/C (3537.6 h–1). It can also deliver variety aminoarenes outstanding selectivity excellent functional group compatibility several groups. Mechanistic studies have shown that introduction enhances Ni's ability dissociate water situ produce H* improves rate, resulting rapid final product Ph-NH2.

Language: Английский

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Multiple active site metal-based catalysts for C-N coupling reactions and the beyond

Next Materials, Journal Year: 2025, Volume and Issue: 8, P. 100555 - 100555

Published: Feb. 21, 2025

Language: Английский

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Balancing Hydrogen Evolution and Hydrogenation Reaction via Facet Engineering for Efficient Conversion of Nitrate to Ammonia in Actual Wastewater

Angewandte Chemie International Edition, Journal Year: 2025, Volume and Issue: unknown

Published: March 11, 2025

Abstract Due to the competitive relationship between nitrate reduction reaction (NO 3 − RR) and hydrogen evolution (HER), conventional approach improve Faradaic efficiency is select a catalyst without HER activity. Nevertheless, such strategy not only limits application of catalysts in NO RR, but also causes insufficient source, thereby sacrificing ammonia yield rate. We believe that should be excluded from hydrogenation reduction. Herein, taking traditional water electrolysis material Co O 4 as model system, we reveal oxygen vacancies on crystal facet can greatly promote dissociation capture intermediate for successfully shifting pathway hydrogenation. Beyond development, construct hybrid reactor achieve an recovery rate 1216.8 g‐N m −2 d −1 nuclear industry wastewater with ultra‐high concentration. This study breaks through limitation which provides significant insight into designing mechanism.

Language: Английский

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Asymmetric active sites in ultra-thin high-entropy metal oxides nanosheets for enhanced electrochemical synthesis of ammonia

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125248 - 125248

Published: March 1, 2025

Language: Английский

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Boosting Nitrate Electroreduction to Ammonia on Alloying of Cu With Au by Accelerated Proton Relay

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

Published: March 3, 2025

ABSTRACT Bimetallic nanoparticles (NPs) are recognized as effective catalysts for the nitrate reduction reaction (NO 3 – RR) to produce ammonia (NH ) due their multiple active sites and electron redistribution enabled by strong metal–metal interactions. An in‐depth analysis of mechanism is essential advancing efficient electrocatalysts. In this study, carbon‐supported Au Cu alloy (Au Cu/CC) were synthesized applied direct NO − NH . The generation rate achieved with Cu/CC was 1719.3 µg h −1 cm −2 , Faraday efficiency (FE) measured at 95.1% under an ultra‐low potential −0.5 V versus RHE. high activity attributed synergistic interactions between in relay catalysis, where exhibits selective *NO, while demonstrates excellent performance subsequent *NO Additionally, d–d orbital hybridization adjusts d–band center NPs, effectively modulating adsorption energies *N facilitate This electrocatalytic approach offers a novel strategy designing multifunctional RR catalysts.

Language: Английский

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Defect‐Enriched Cobalt‐Based Coordination Polymers for Selective and Efficient Nitrate Electroreduction to Ammonia

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

Published: March 3, 2025

Abstract Electrocatalytic nitrate reduction to ammonia (NRA) offers an arousing route for converting widespread pollutant under mild conditions. Among other NRA catalysts, single‐atom catalyst (SAC) has emerged as a promising candidate due its numerous advantages such maximum metal‐atom‐utilization efficiency, homogeneous and tailorable active sites, which still encounters formidable challenge accelerate the kinetics simultaneously suppress competitive hydrogen evolution reaction, especially when operated in electrolytes with low concentration nitrate. Herein, general strategy is reported prepare defect‐enriched coordination polymer catalysts featuring well‐defined unsaturated metal can exhibit exceptional performance even at surpass SACs toward catalysis. Taking cobalt (Co) example, Co‐based polymers (d‐CoCP) counterpart CoCP without defects are investigated proof‐of‐concept study. Both experimental theoretical results elucidate that elaborately‐engineered d‐CoCP markedly decrease thermodynamic barrier reducing *NO *HNO rate‐limiting step along pathway, thus accelerating adsorption of promoting kinetics.

Language: Английский

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Balancing Hydrogen Evolution and Hydrogenation Reaction via Facet Engineering for Efficient Conversion of Nitrate to Ammonia in Actual Wastewater

Angewandte Chemie, Journal Year: 2025, Volume and Issue: unknown

Published: March 12, 2025

Abstract Due to the competitive relationship between nitrate reduction reaction (NO 3 − RR) and hydrogen evolution (HER), conventional approach improve Faradaic efficiency is select a catalyst without HER activity. Nevertheless, such strategy not only limits application of catalysts in NO RR, but also causes insufficient source, thereby sacrificing ammonia yield rate. We believe that should be excluded from hydrogenation reduction. Herein, taking traditional water electrolysis material Co O 4 as model system, we reveal oxygen vacancies on crystal facet can greatly promote dissociation capture intermediate for successfully shifting pathway hydrogenation. Beyond development, construct hybrid reactor achieve an recovery rate 1216.8 g‐N m −2 d −1 nuclear industry wastewater with ultra‐high concentration. This study breaks through limitation which provides significant insight into designing mechanism.

Language: Английский

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^*H Species Regulation of Heterostructured Cu₂O/NiO Nanoflowers Boosting Tandem Nitrite Reduction for High‐Efficiency Ammonia Production

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

Published: March 18, 2025

Abstract Ambient electrocatalytic reduction of NO 2 − to NH 3 (NO RR) provides a reliable route for migrating pollutants and simultaneously generating valuable 3. However, the RR involves multistep electron transfer complex intermediates, rendering achievement high selectivity major challenge. In this contribution, heterostructured Cu O/NiO nanoflowers are explored incorporating advantages dual active sites as highly selective catalyst. Combined theoretical calculations in situ FTIR/EPR spectroscopy analysis, it is revealed synergistic effect O NiO promote energetics heterostructure electrocatalyst through tandem catalysis pathway, where activates initial absorption deoxygenation boosting * formation, while generated on then transferred substrate with abundant hydrogen conversion. Moreover, formation enhances H retention capacity, promoting consumed inhibiting inter‐ species binding. As result, equipped flow cell displays superior yield rate 128.2 mg h −1 cm −2 Faradaic efficiency 97.1% at current density −1.25 A . Further, designed system proven be adaptable other electrochemical production reactions including reduction.

Language: Английский

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Tailored High-Entropy Alloy Nanomaterials for Electrocatalytic Applications

EnergyChem, Journal Year: 2025, Volume and Issue: unknown, P. 100155 - 100155

Published: March 1, 2025

Language: Английский

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