Optimizing C─C Coupling on Cu⁰/Cu⁺/Ga Interfaces by Enhancing Active Hydrogen Absorption for Excellent CO₂‐to‐C₂₊ Electrosynthesis

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

Published: March 5, 2025

The electrocatalytic reduction of CO2 (CO2RR) to high-value chemicals and fuels offers a promising route for clean carbon cycle. However, it often suffers from low catalytic activity poor selectivity. Heterostructure construction has been shown be an effective strategy producing multi-carbon products, but the synergistic mechanisms between multiple active sites resulting reconstruction process remain unclear. In this study, Ga2O3/CuO heterostructure is established via simple sol-gel method produce C2+ products. Experimental results demonstrate that Ga2O3 stabilizes Cu+ form Cu0/Cu+/Ga centers enhances water-splitting ability during reaction. improved hydrogen absorption on Ga site shifts C─C coupling reaction pathway *OCCO asymmetric *OCCHO path with lower energy barrier. As result, catalysts exhibit superior CO2RR performance, achieving 70.1% Faradaic efficiency at -1.2 VRHE in flow cell, ethylene reaching 58.3% remaining stable 10 h.

Language: Английский

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Enhancing Localized Electron Density over Pd_1.4Cu Decorated Oxygen Defective TiO_2‐x Nanoarray for Electrocatalytic Nitrite Reduction to Ammonia

Small, Journal Year: 2024, Volume and Issue: 20(46)

Published: Aug. 6, 2024

Abstract Electrocatalytic nitrite (NO 2 − ) reduction to ammonia (NH 3 is a promising method for reducing pollution and aiding industrial production. However, progress limited by the lack of efficient selective catalysts ambiguous catalytic mechanisms. This study explores loading PdCu alloy onto oxygen defective TiO 2‐x , resulting in significant increase NH yield (from 70.6 366.4 µmol cm −2 h −1 at −0.6 V vs reversible hydrogen electrode) modulating localized electron density. In situ operando studies illustrate that NO involves gradual deoxygenation hydrogenation. The process also demonstrated excellent selectivity stability, with long‐term durability cycling 50 stability tests. Density functional theory (DFT) calculations elucidate introduction alloys further amplified density vacancies (Ovs). Additionally, Ti─O bond strengthened as d ‐band center Ti rising after loading, facilitating adsorption activation * . Moreover, presence Ovs lowers energy barriers hydrogenation, leading high insight controlling offers valuable insights advancing sustainable synthesis methods.

Language: Английский

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Modulating Water Dissociation for Ampere-Level CO2-to-Ethanol Conversion over La(OH)3@Cu Hollow-fiber Penetration Electrode

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125202 - 125202

Published: Feb. 1, 2025

Language: Английский

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Development of catalysts and reactor designs for CO₂ electroreduction towards C₂₊ products

Energy Materials, Journal Year: 2025, Volume and Issue: 5(5)

Published: Feb. 25, 2025

Recent research on the electrocatalytic CO2 reduction reaction (eCO2RR) has garnered significant attention given its capability to address environmental issues associated with emissions while harnessing clean energy produce high-value-added products. Compared C1 products, C2+ products provide greater densities and are highly sought after as chemical feedstocks. However, formation of C-C bond is challenging due competition H-H C-H bonds. Therefore, elevate selectivity yield fuels, it essential develop more advanced electrocatalysts optimize design electrochemical cell configurations. Of materials investigated for CO2RR, Cu-based stand out their wide availability, affordability, compatibility. Moreover, catalysts exhibit promising capabilities in adsorption activation, facilitating compounds via coupling. This review examines recent both cells electroreduction compounds, introducing core principles eCO2RR pathways involved generating A key focus categorization catalyst designs, including defect engineering, surface modification, nanostructure tandem catalysis. By analyzing studies catalysts, we aim elucidate mechanisms behind enhanced compounds. Additionally, various types electrolytic discussed. Lastly, prospects limitations utilizing highlighted future research.

Language: Английский

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Progress in Cu‐Based Catalyst Design for Sustained Electrocatalytic CO₂ to C₂₊ Conversion

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

Published: Feb. 27, 2025

Abstract The electrocatalytic conversion of CO 2 into valuable multi‐carbon (C 2+ ) products using Cu‐based catalysts has attracted significant attention. This review provides a comprehensive overview recent advances in catalyst design to improve C selectivity and operational stability. It begins with an analysis the fundamental reaction pathways for formation, encompassing both established emerging mechanisms, which offer critical insights design. In situ techniques, essential validating these by real‐time observation intermediates material evolution, are also introduced. A key focus this is placed on how enhance through manipulation, particularly emphasizing catalytic site construction promote C─C coupling via increasing * coverage optimizing protonation. Additionally, challenge maintaining activity under conditions discussed, highlighting reduction active charged Cu species materials reconstruction as major obstacles. To address these, describes strategies preserve sites control including novel utilization mitigation reconstruction. By presenting developments challenges ahead, aims guide future conversion.

Language: Английский

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Boosting Electrocatalytic CO₂ Reduction to Multi‐Carbon Products via Modulated Asymmetric Cu Sites

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

Published: March 20, 2025

Abstract Electrocatalytic carbon dioxide reduction reaction (CO 2 RR) into high‐value products on Cu‐based catalysts holds promise for achieving neutrality. However, the productivity toward multi‐carbon in CO RR is insufficient practical applications owing to limited * dimerization process, especially under high current operation. Here, Ag‐doped oxide‐derived Cu nanosheets (CuAg x% NSs) are reported via tailoring Ag NSs at an atomic‐level form C 2+ products. The CuAg 0.123% achieved a significant Faradaic efficiency of 77.5% and 71.3% 300 500 mA cm −2 , respectively. Theoretical calculations situ characterizations reveal that single‐atomic facet generates asymmetric CO‐adsorbed sites, stabilizing adsorption further triggering C─C coupling This work emphasizes significance sites fine regulation critical intermediate enhance *CO

Language: Английский

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Hierarchical Cavity Cu Nanostructures with Coordinative Microenvironment Engineering for pH‐Universal Electrocatalytic CO₂‐to‐C₂₊ Conversion

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

Published: March 24, 2025

Abstract The rational design of copper‐based electrocatalysts with optimized *CO intermediate coverage and OH⁻‐enriched microenvironments remain critical yet challenging for achieving efficient CO 2 ‐to‐C 2+ conversion across varied pH conditions. This study presents a Kirkendall effect‐driven synthesis hierarchical copper nanostructures featuring precisely engineered cavity architectures tunable coordination environments. Through systematic number (CN) modulation, it is demonstrated that the d‐band center position Cu sites positively correlated adsorption energy. Specifically, moderate‐coordinated (111) facets in three‐layered structures (3L‐Cu) exhibit optimal dimerization energetics. Benefiting from synergistic effects spatial confinement ionic diffusion gradients, 3L‐Cu catalyst establishes self‐sustaining alkaline microdomains even acidic media (pH 1), as evidenced by situ Raman spectroscopy. unique microenvironment engineering enables state‐of‐the‐art C Faradaic efficiencies 78.74 ± 2.36% (alkaline), 69.33 2.08% (neutral), 58.32 1.75% (acidic) sustained stability, outperforming existing pH‐universal RR catalysts. First‐principles calculations further reveal multilayer effect reduces coupling energy barriers *CO‐*CO *CO‐*COH electrolytes, respectively. work new paradigm designing adaptive through coordinated structural electronic control.

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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Cu supraparticles with enhanced mass transfer and abundant C-C coupling sites achieving ampere-level CO2-to-C2+ electrosynthesis

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

Published: April 10, 2025

The efficient electrochemical CO2 reduction to C2+ products at high current densities remains a significant challenge. Here we show inherently hydrophobic and hierarchically porous Cu supraparticles comprising sub-10 nm constituent particles for ampere-level CO2-to-C2+ electrosynthesis. These feature abundant grain boundaries selectivity, coupled with interconnected mesopores interparticle macropore cavities enhance the accessibility of active sites mass transfer, breaking trade-off between activity transfer in Cu-based catalysts. Moreover, intrinsic hydrophobicity mitigates water-flooding issue catalytic layer flow cells, improving stability densities. Consequently, achieve electrolysis up 3.2 A cm-2 Faradaic efficiency 74.9% (compared 1.21 55.4% nanoparticles) maintain 1 over 100 h. This work provides profound insights into effect coupling reaction under presents corresponding solution by superstructure design.

Language: Английский

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Plasmonic Ag-decorated GaN for efficient photothermal CO2 conversion

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: 373, P. 125366 - 125366

Published: April 14, 2025

Language: Английский

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