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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Tip carbon encapsulation customizes cationic enrichment and valence stabilization for low K+ acidic CO2 electroreduction

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

Published: Feb. 19, 2025

Abstract Acidic electrochemical CO 2 conversion is a promising alternative to overcome the low utilization. However, over-reliance on highly concentrated K + inhibit hydrogen evolution reaction also causes (bi)carbonate precipitation interfere with catalytic performance. In this work, under screening and guidance of computational simulations, we present carbon coated tip-like O 3 electrocatalyst for stable efficient acidic synthesize formic acid (HCOOH) concentration. The layer protects oxidized species higher intrinsic activity from reductive corrosion, peripherally formulates tip-induced electric field regulate adverse H attraction desirable enrichment. an electrolyte at pH 0.94, only 0.1 M required achieve Faradaic efficiency (FE) 98.9% 300 mA cm −2 HCOOH long-time stability over100 h. By up-scaling electrode into 25 electrolyzer setup, total current 7 A recorded sustain durable production 291.6 mmol L −1 h .

Language: Английский

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Bamboo-like amorphous Ni(OH)2 nanotubes wrapped Cu nanoparticles with a confined geometry for CO2 electroreduction to ethane in a flow cell

Science China Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 2, 2025

Language: Английский

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Establishment of Gas–Liquid–Solid Interface on Multilevel Porous Cu₂O for Potential-Driven Selective CO₂ Electroreduction toward C₁ or C₂ Products

ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 20, 2025

Copper-based catalysts demonstrate distinctive multicarbon product activity in the CO2 electroreduction reaction (CO2RR); however, their low selectivity presents significant challenges for practical applications. Herein, we have developed a multilevel porous spherical Cu2O structure, wherein mesopores are enriched with catalytic active sites and effectively stabilize Cu+, while macropores facilitate formation of "gas–liquid–solid" three-phase interface, thereby creating microenvironment an increasing water concentration gradient from interior to exterior. Potential-driven phase engineering protonation synergistically optimize pathway, facilitating switch between CO C2H4. At current density 100 mA cm–2, faradaic efficiency (FE) reaches impressive 96.97%. When increases 1000 FEC2H4 attains 53.05%. Experiments theoretical calculations indicate that at lower potentials, pure diminishes adsorption *CO intermediates, weak inhibits hydrogen evolution reactions, promoting production. Conversely, more negative Cu0/Cu+ interface strong generate locally elevated concentrations *COOH which enhance C–C coupling deep hydrogenation, ultimately improving toward C2+ products. This study provides novel insights into rational design copper-based customizable

Language: Английский

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Progress of mechanistic pathways involved in electrochemical CO2 reduction

Journal of Energy Chemistry, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 1, 2024

Language: Английский

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Switching CO-to-Acetate Electroreduction on Cu Atomic Ensembles

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 17, 2024

The electrocatalytic reaction pathway is highly dependent on the intrinsic structure of catalyst. CO2/CO electroreduction has recently emerged as a potential approach for obtaining C2+ products, but it challenging to achieve high selectivity single product. Herein, we develop Cu atomic ensemble that satisfies appropriate site distance and coordination environment required CO-to-acetate conversion, which shows outstanding overall performance with an acetate Faradaic efficiency 70.2% partial current density 225 mA cm–2 formation rate 2.1 mmol h–1 cm–2. Moreover, single-pass CO conversion 91% remarkable stability can be also obtained. Detailed experimental theoretical investigations confirm significant advantages ensembles in optimizing C–C coupling, stabilizing key ketene intermediate (*CCO), inhibiting *HOCCOH intermediate, switch reduction from ethanol/ethylene conventional metallic ensembles.

Language: Английский

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Liquid nitrogen quenching for efficient Bifunctional electrocatalysts in water Splitting: Achieving four key objectives in one step

Journal of Colloid and Interface Science, Journal Year: 2025, Volume and Issue: 684, P. 21 - 34

Published: Jan. 4, 2025

Language: Английский

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Nanoscale Cu–Ag Heterostructures for CO₂ Reduction to C₂₊ Products

ACS Applied Nano Materials, Journal Year: 2025, Volume and Issue: 8(4), P. 1893 - 1902

Published: Jan. 17, 2025

The electrochemical reduction of CO2 (CO2RR) to value-added chemicals represents a critical strategy for mitigating carbon emissions and promoting energy sustainability. This study focuses on enhancing the performance copper-based catalysts through silver doping, with specific objective improving C2+ product selectivity suppressing C1 products. We report delicate synthesis three distinct CuAg Janus nanostructures using coreduction method involving metal precursors nucleation growth. Compared Cu NPs, 1:0.02 exhibits significantly superior both C2H4 (∼50%) multicarbon products (∼70%) at −1.2 V vs RHE in CO2RR. X-ray photoelectron spectroscopy (XPS) analysis reveals that nanostructure facilitates an electron transfer process, influencing catalytic activity reaction. In-situ attenuated total reflectance Fourier transform infrared (ATR-FTIR) spectra indicate nanoparticles promote formation *CHO *COCHO, which are key intermediates production enhancement C–C coupling. provides effective designing advanced tandem catalysts, paving way widespread application CO2RR addressing environmental challenges.

Language: Английский

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Catalytic Cu₂O/Cu Site Trades off the Coupling and Etching Reactions of Carbon Intermediates for CO₂‐Assisted Graphene Synthesis

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

Published: Jan. 27, 2025

Abstract In the chemical vapor deposition (CVD) synthesis of graphene, surficial state metal substrate has exerted key roles in all elemental reaction steps determining growth mechanism graphene. Herein, a CO 2 ‐participated annealing procedure is designed to construct catalytic Cu O/Cu sites on foil for graphene CVD with /CH 4 as carbon sources. These species can catalyze CH decomposition and subsequent C─C coupling form C intermediates fast monolayer hexagonal domains diameter ≈30 µm within 0.5 min. The kinetics be bidirectionally regulated merely variation flow rate during stages, association + /Cu 0 ratio, enabling simultaneous control over size shape domains. Density functional theory (DFT) calculations indicate that reduce activation energy by ≈0.13 eV first dehydrogenation , allowing growing driven faster than their etching O‐containing * O OH species. work provides novel insights into heterostructured nano‐catalyst consisting zero valent variably oxide facilitate controllable materials.

Language: Английский

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Eu-Doped Cu2O for Tailored Cu+/Cu0 sites and enhanced C2 selectivity in CO2 electroreduction

Applied Surface Science, Journal Year: 2025, Volume and Issue: unknown, P. 162633 - 162633

Published: Feb. 1, 2025

Language: Английский

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