A Bi‐Co Corridor Construction Effectively Improving the Selectivity of Electrocatalytic Nitrate Reduction toward Ammonia by Nearly 100%

Advanced Materials, Год журнала: 2023, Номер 35(48)

Опубликована: Сен. 22, 2023

Improving the selective ammonia production capacity of electrocatalytic nitrate reduction reaction (NO3 RR) at ambient conditions is critical to future development and industrial application electrosynthesis ammonia. However, involves multi-proton electron transfer as well desorption underutilization intermediates, posing a challenge selectivity NO3 RR. Here electrodeposition site Co modulated by depositing Bi bottom catalyst, thus obtaining Co+Bi@Cu NW catalyst with Bi-Co corridor structure. In 50 mm NO3- , exhibits highest Faraday efficiency ≈100% (99.51%), an yield rate 1858.2 µg h-1 cm-2 high repeatability -0.6 V versus reversible hydrogen electrode. Moreover, change NO2- concentration on surface observed in situ reflection absorption imaging intermediates RR process detected electrochemical Raman spectroscopy together verify trapping effect It believed that measure modulating deposition loading element easy-to-implement general method for improving NH3 corresponding scientific research applications.

Язык: Английский

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Modulating Metal‐Nitrogen Coupling in Anti‐Perovskite Nitride via Cation Doping for Efficient Reduction of Nitrate to Ammonia

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(38)

Опубликована: Авг. 1, 2023

The complexes of metal center and nitrogen ligands are the most representative systems for catalyzing hydrogenation reactions in small molecule conversion. Developing heterogeneous catalysts with similar active metal-nitrogen functional centers, nevertheless, still remains challenging. In this work, we demonstrate that coupling anti-perovskite Co4 N can be effective modulated by Cu doping to form Co3 CuN, leading strongly promoted process during electrochemical reduction nitrate (NO3- RR) ammonia. combination advanced spectroscopic techniques density theory calculations reveal dopants strengthen Co-N bond upshifted d-band towards Fermi level, promoting adsorption NO3- *H facilitating transition from *NO2 /*NO H/*NOH. Consequently, CuN delivers noticeably better RR activity than pristine N, optimal Faradaic efficiency 97 % ammonia yield 455.3 mmol h-1 cm-2 at -0.3 V vs. RHE. This work provides an strategy developing high-performance catalyst synthesis.

Язык: Английский

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Critical review in electrocatalytic nitrate reduction to ammonia towards a sustainable nitrogen utilization

Chemical Engineering Journal, Год журнала: 2024, Номер 483, С. 148952 - 148952

Опубликована: Янв. 22, 2024

Язык: Английский

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Synergistic Effect of Ni/Ni(OH)₂ Core‐Shell Catalyst Boosts Tandem Nitrate Reduction for Ampere‐Level Ammonia Production

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(27)

Опубликована: Апрель 23, 2024

Electrocatalytic reduction of nitrate to ammonia provides a green alternate the Haber-Bosch method, yet it suffers from sluggish kinetics and low yield rate. The follows tandem reaction nitrite subsequent hydrogenation generate ammonia, Faraday efficiency (FE) is limited by competitive hydrogen evolution reaction. Herein, we design heterostructure catalyst remedy above issues, which consists Ni nanosphere core Ni(OH)

Язык: Английский

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Boosting electrochemical oxygen reduction to hydrogen peroxide coupled with organic oxidation

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Июль 19, 2024

Abstract The electrochemical oxygen reduction reaction (ORR) to produce hydrogen peroxide (H 2 O ) is appealing due its sustainability. However, efficiency compromised by the competing 4e − ORR pathway. In this work, we report a hierarchical carbon nanosheet array electrode with single-atom Ni catalyst synthesized using organic molecule-intercalated layered double hydroxides as precursors. exhibits excellent 2e performance under alkaline conditions and achieves H yield rates of 0.73 mol g cat −1 h in H-cell 5.48 flow cell, outperforming most reported catalysts. experimental results show that atoms selectively adsorb , while nanosheets generate reactive species, synergistically enhancing production. Furthermore, coupling system integrating ethylene glycol oxidation significantly enhances rate 7.30 producing valuable glycolic acid. Moreover, convert electrolyte containing directly into downstream product sodium perborate reduce separation cost further. Techno-economic analysis validates economic viability system.

Язык: Английский

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Metal Doped Unconventional Phase IrNi Nanobranches: Tunable Electrochemical Nitrate Reduction Performance and Pollutants Upcycling

Environmental Science & Technology, Год журнала: 2024, Номер 58(24), С. 10863 - 10873

Опубликована: Июнь 6, 2024

Electrochemical nitrate reduction (NO3RR) provides a new option to abate contamination with low carbon footprint. Restricted by competitive hydrogen evolution, achieving satisfied performance in neutral media is still challenge, especially for the regulation of this multielectron multiproton reaction. Herein, facile element doping adopted tune catalytic behavior IrNi alloy nanobranches an unconventional hexagonal close-packed (hcp) phase toward NO3RR. In particular, obtained hcp IrNiCu favor ammonia production and suppress byproduct formation electrolyte indicated situ differential electrochemical mass spectrometry, high Faradaic efficiency (FE) 85.6% large yield rate 1253 μg cm–2 h–1 at −0.4 −0.6 V (vs reversible electrode (RHE)), respectively. contrast, resultant IrNiCo promote nitrite, peak FE 33.1% −0.1 RHE). Furthermore, hybrid electrolysis cell consisting NO3RR formaldehyde oxidation constructed, which are both catalyzed nanobranches. This electrolyzer exhibits lower overpotential holds potential treat polluted air wastewater simultaneously, shedding light on green chemical based contaminate degradation.

Язык: Английский

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Active Hydroxyl‐Mediated Preferential Cleavage of Carbon‐Carbon Bonds in Electrocatalytic Glycerol Oxidation

Angewandte Chemie International Edition, Год журнала: 2025, Номер unknown

Опубликована: Янв. 8, 2025

Electrocatalytic glycerol oxidation reaction (GOR) to produce high-value formic acid (FA) is hindered by high formation potential of active species and sluggish C-C bond cleavage kinetics. Herein, Ni single-atom (NiSA) Co (CoSA) dual sites anchored on nitrogen-doped carbon nanotubes embedded with Ni0.1Co0.9 alloy (Ni0.1Co0.9@NiSACoSA-NCNTs) are constructed for electrochemical GOR. Remarkably, it can reach 10 mA cm-2 at a low 1.15 V versus the reversible hydrogen electrode (vs. RHE) realize formate selectivity 93.27 % even conversion 98.81 1.45 vs. RHE. The GOR mechanism pathway systematically elucidated via experimental analyses theoretical calculations. It revealed that hydroxyl (*OH) be produced during NiSA, CoSA, synergistically optimizes electronic structure CoSA sites, reducing energy barriers *OH-mediated bonds dehydrogenation C1 intermediates. This decreases number intermediates steps GOR-to-FA, thus increasing production efficiency. After coupling evolution in membrane assembly cell, 14.26 g 23.10 L H2 100 108 h.

Язык: Английский

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Unlocking high-current-density nitrate reduction and formaldehyde oxidation synergy for scalable ammonia production and fixation

Energy & Environmental Science, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

Single atom Ag-decorated Cu 2 O nanowires achieve two-ampere-level nitrate-to-ammonia conversion, facilitating further ammonia fixation into ammonium formate at 10 g-scale.

Язык: Английский

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Balancing dynamic evolution of active sites for urea oxidation in practical scenarios

Energy & Environmental Science, Год журнала: 2023, Номер 16(12), С. 6015 - 6025

Опубликована: Янв. 1, 2023

The role of single atomic Ru site for enhanced UOR performance.

Язык: Английский

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Promoting Electrocatalytic Hydrogenation of 5-Hydroxymethylfurfural over a Cooperative Ag/SnO₂ Catalyst in a Wide Potential Window

ACS Catalysis, Год журнала: 2023, Номер 13(20), С. 13528 - 13539

Опубликована: Окт. 6, 2023

Electrochemical reduction of biomass-derived 5-hydroxymethylfurfural (HMF) to produce 2,5-dihydroxymethylfuran (DHMF) is a promising approach for biomass upgrading. The achievement high activity and Faradaic efficiency (FE) in wide potential window critical mature applications considering the significantly varied voltages supplied by different renewable energies. However, it still challenging due multiple reaction pathways competitive hydrogen evolution reaction. Herein, we synthesized cooperative catalyst supporting Ag nanoparticles (AgNPs) on SnO2 nanosheet arrays, which realizes electrochemical HMF DHMF with FE (>95%) (from −0.62 −1.12 V vs reversible electrode). situ measurements reveal that AgNPs promote water splitting generate reactive (H*) species, effectively react via Langmuir–Hinshelwood mechanism. Moreover, accelerate formation oxygen vacancies under conditions, act as electrophilic sites realize selective adsorption hydrogenation carbonyl bond (C═O) yield DHMF. Finally, designed coupling system simultaneously oxidation 2,5-furandicarboxylic acid, showing lower at same current density than traditional cathodic anodic reaction, an economical manner.

Язык: Английский

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