Stabilizing the oxidation state of catalysts for effective electrochemical carbon dioxide conversion

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(12), P. 6295 - 6321

Published: Jan. 1, 2024

Developing sophisticated strategies to stabilize oxidative metal catalysts based on the correlation between dynamic oxidation state and product profile is favorable for efficient electrochemical CO 2 conversion.

Language: Английский

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Hierarchical Tandem Catalysis Promotes CO Spillover and Trapping for Efficient CO₂ Reduction to C₂₊ Products

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 27, 2025

The electrochemical CO2 reduction reaction (CO2RR) to produce multicarbon (C2+) hydrocarbons or oxygenate compounds is a promising route obtain renewable fuel valuable chemicals; however, producing C2+ at high current densities still challenge. Herein, we design hierarchically structured tandem catalysis electrode for greatly improved catalytic activity and selectivity products. constructed of sputtered Ag nanoparticle layer on hydrophobic polytetrafluoroethylene (PTFE) membrane nitrogen-doped carbon (NC)-modified Cu nanowire arrays. arrays are in situ grown PTFE by oxidation CuAl alloy, which the chemical etching metal Al induces formation array structure. Within hierarchical configuration, CO can be efficiently generated an active then spillover transfer NC-modified layer, Cu/NC interfaces enhance *CO trapping adsorption. During CO2RR, optimized achieves superior Faradaic efficiencies 53.5% 87.5% ethylene (C2H4) products density 519.0 mA cm–2, respectively, with C2+/C1 ratio 10.42 long-term stability up 50 h. In Raman attenuated total reflection-surface enhanced infrared absorption spectroscopy (ATR-SEIRAS) confirm that Ag–Cu–NC system significantly enhances linear adsorption intermediates dissociation H2O, improves C–C coupling capability, stabilizes key intermediate *OCCOH

Language: Английский

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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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Low‐Coordinated Conductive ZnCu Metal‐Organic Frameworks for Highly Selective H₂O₂ Electrosynthesis

Small, Journal Year: 2024, Volume and Issue: unknown

Published: May 21, 2024

Direct electrosynthesis of hydrogen peroxide (H

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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Enhancing C-C Coupling in CO2 Electroreduction by Engineering Pore Size of Porous Carbon-Supported Cu Catalysts

Catalysts, Journal Year: 2025, Volume and Issue: 15(3), P. 199 - 199

Published: Feb. 20, 2025

The electroreduction of CO2 (CO2RR) is a promising and environmentally sustainable approach to closing the carbon cycle. However, achieving high activity selectivity for multicarbon (C2₊) products remains significant challenge due complexity reaction pathways. In this study, porous carbon-supported copper catalysts (CuHCS) with pore sizes 120 nm (CuHCS120) 500 (CuHCS500) were synthesized tailor microenvironment at electrode–electrolyte interface enhance product selectivity. CuHCS120 achieved maximum faradaic efficiency (FE) C2₊ 46%, double that CuHCS500 (23%). contrast, showed higher FE CO (36%) compared (14%) same potential. In-depth ex situ in investigations revealed smaller pores promote enrichment adsorption *CO intermediates, thereby enhancing C–C coupling formation products. These findings underscore critical role structural confinement modulating catalytic provide valuable insights rational design advanced CO2RR.

Language: Английский

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In-situ characterization technologies and theoretical calculations in carbon dioxide reduction: In-depth understanding of reaction mechanisms and rational design of electrocatalysts

Coordination Chemistry Reviews, Journal Year: 2025, Volume and Issue: 533, P. 216541 - 216541

Published: Feb. 28, 2025

Language: Английский

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Progress in Cu-based electrocatalysts for electrochemical CO₂ reduction to C₂₊ products

Catalysis Science & Technology, Journal Year: 2024, Volume and Issue: 14(10), P. 2697 - 2716

Published: Jan. 1, 2024

Recent progress in Cu-based electrocatalysts for CO 2 RR to C 2+ products, from theoretical and experimental aspects.

Language: Английский

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Interface engineering of Cu2O/In(OH)3 for efficient solar-driven CO2 electrochemical reduction to syngas

Applied Surface Science, Journal Year: 2024, Volume and Issue: 662, P. 160114 - 160114

Published: April 16, 2024

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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