Hydroxylation of Cu Sites Enhances Selectivity of Electrosynthesis of Ethanol via Tandem Reduction of CO₂

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

Published: March 31, 2025

Abstract Electrochemical conversion of CO 2 into value‐added multi‐carbon products is highly attractive for utilization using sustainable electricity energy. However, achieving high ethanol selectivity copper‐based catalysts remains challenging due to the competing side reactions such as ethylene formation. Herein, a novel electrocatalyst, PANI‐Ag/Cu‐OH reported, comprising polyaniline‐supported silver single atoms coupled with hydroxyl‐modified copper clusters. Tandem reduction realized by coupling formation on Ag site and further hydroxylated Cu sites. The synergistic approach enables Faradaic efficiency 68.9% current density −263.8 mA cm −2 at −0.78 V versus RHE in alkaline media. CO‐TPD situ infrared spectra studies reveal that strong adsorption + species stabilized hydroxyl groups are crucial asymmetric C–C stabilization intermediates, leading enhanced selectivity.

Language: Английский

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Synergistic Effects in the Electrochemical Carbon Dioxide Reduction Reaction for Multi‐Carbon Product Formation

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

Published: April 1, 2025

Abstract The synergistic effects in electrocatalysis can significantly enhance catalyst performance by improving catalytic activity, selectivity, and stability, optimizing reaction mechanisms electron transfer processes. This review summarizes recent advancements the of electrochemical reduction CO 2 (eCO RR) to multi‐carbon (C 2+ ) products. Starting with fundamental principles eCO RR for C product formation, paper outlines producing , 3 4 5 A comprehensive discussion is provided on critical impact structure–performance relationship production Subsequently, observed are classified various electrocatalysts different properties, including single/dual‐atom catalysts, multi‐centric single‐atom alloys, metal‐organic frameworks, heterojunction catalysts. Finally, challenges achieving selective formation through discussed, along corresponding strategies overcome obstacles.

Language: Английский

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Functional Group Engineering of Single‐Walled Carbon Nanotubes for Anchoring Copper Nanoparticles Toward Selective CO₂ Electroreduction to C₂ Products

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

Published: April 3, 2025

Abstract Electroreduction of carbon dioxide (CO 2 ) is a key strategy for achieving net‐zero emissions. Copper (Cu)‐based electrocatalysts have shown promise CO conversion into valuable chemicals but are hindered by limited C 2+ product selectivity due to competing hydrogen evolution and ineffective dimerization adsorbed intermediate ( * CO). Here, functional‐group‐directed reported enhance using single‐walled nanotubes (SWCNTs) as supports. The catalytic performance Cu nanoparticles strongly influenced the type density functional groups on SWCNTs. Optimized Cu/amine‐functionalized SWCNTs achieved Faradaic efficiency 66.2% partial current −270 mA cm −2 products within flow cell, outperforming Cu/SWCNTs Cu/cyano‐functionalized Density theory calculations revealed that electron‐donating amine can facilitate electron transfer from graphite sheet atoms, thereby shifting d‐band center upward. This shift enhances its hydrogenation derivative adsorption promotes water splitting, leading an increased tendency generation products. In situ infrared Raman spectroscopy confirm enhancement CHO coverage, facilitating C─C coupling. work provides molecular framework exploring interactions between active metals in electrolysis, offering insights designing catalysts broad range electrocatalytic processes.

Language: Английский

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Electrochemical reduction of CO2 to liquid products: Factors influencing production and selectivity

International Journal of Hydrogen Energy, Journal Year: 2025, Volume and Issue: 128, P. 800 - 832

Published: April 25, 2025

Language: Английский

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Recent Advances in Electrocatalytic Conversion of CO2-to-Ethylene: from Reaction Mechanisms to Tuning Strategies

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: unknown, P. 124822 - 124822

Published: Nov. 1, 2024

Language: Английский

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Preferentially Stabilizing the Watershed Intermediates by Adsorbate‐adsorbate Interaction to Accelerate CO₂ Electroreduction to Ethanol

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

Published: Dec. 26, 2024

Abstract Returning CO 2 to liquid ethanol powered by clean energy offers considerable economic benefits and contributes reaching the goal of carbon neutrality, but it remains a formidable challenge achieve high selectivity due inevitable strong competition among various pathways. Herein, an investigation is presented accelerate electroreduction via preferentially stabilizing precarious watershed intermediates ( * CHCOH) creating adsorbate‐adsorbate interaction. The highly ordered CuOx nanoplates (HO‐CuOx NPLs) featuring abundant amorphous‐crystalline interface exhibit exceptional Faradaic efficiency (FE EtOH ) 63.8% ethanol‐to‐ethylene ratio 6.1 at large partial current density j 232.8 mA cm −2 . findings decipher that in‐between nanogaps in enhance adsorption OH, which can strengthen C─O bonds while weakening Cu─C interaction CHCOH through interaction, thereby enabling predilection for conversion. Beyond efficient ethanol‐oriented RR electrocatalyst, investigations provide in‐depth understanding on key steps precise regulation, be extended range conversion technologies.

Language: Английский

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Enhanced CO2 Electroreduction to ethylene on Cu nanocube coated with nitrogen-doped carbon shell in-situ electro-derived from metal-organic framework

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 499, P. 156694 - 156694

Published: Oct. 13, 2024

Language: Английский

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A Stable Copper-based Metal-Azolate Framework for Efficient Electroreduction of CO2 to C2+ Products

Chemical Research in Chinese Universities, Journal Year: 2024, Volume and Issue: unknown

Published: July 6, 2024

Language: Английский

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TM and P dual sites on polymeric carbon nitride enable highly selective CO reduction to C2 products with low potentials: A theoretical perspective

The Journal of Chemical Physics, Journal Year: 2024, Volume and Issue: 161(17)

Published: Nov. 1, 2024

The CO reduction reaction (CORR) for the production of high-value-added multi-carbon (C2+) products is currently being actively investigated, where searching high-efficiency catalysts with moderate intermediate binding strength and low kinetic barrier C–C coupling poses a significant challenge. In this study, we employed density functional theory computations to design four synergistic dual sites CORR C2 products, namely, TM-P@melon, by co-doping transition metals (TM = Mn, Fe, Co, Ni) phosphorus (P) into polymeric carbon nitride (i.e., melon-CN). Mn–P@melon Ni–P@melon exhibit higher selectivity toward C2H5OH C2H6, respectively, limiting potentials (C–C energy barriers) −0.43 V (0.52 eV) −0.17 (0.26 eV), respectively. introduction TM P atoms not only narrows band gap melon-CN but also favors *CHO, providing an active site coupling, thus facilitating catalytic reaction. Our work provides rational insights stable, low-cost, efficient that facilitate sustainable high-value chemicals fuels.

Language: Английский

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Synergistic enhancement of the electrocatalytic reduction of CO2 to hydrocarbons at large-sized Cu@Ag electrode

Materials Chemistry Frontiers, Journal Year: 2024, Volume and Issue: 9(2), P. 271 - 279

Published: Nov. 21, 2024

A large-sized Ag@Cu catalyst was fabricated with the objective of significantly enhancing CO 2 RR while concurrently suppressing HER through synergistic mechanism.

Language: Английский

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