Selective Photoconversion of CO₂ to C₂H₄ on Asymmetrical CeO₂─Cu₂O Interfaces Driven by Oxygen Vacancies

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

Published: March 25, 2025

Abstract Photocatalytic conversion of CO 2 into valuable C H 4 is desirable for achieving a carbon‐neutral future, yet faces sluggish kinetics C─C dimerization and insufficient electron deliverability. Herein, an effective top‐down etching route presented to construct interfacial asymmetric oxygen vacancies (Ov) in CeO ─Cu O supported on the copper foam (CeO O/CF). In situ characterizations theoretical calculations demonstrate that nanointerface‐based heterojunctions serve as rapid electron‐transfer pathways, promoting efficiency without need sacrificial agents. Moreover, sites (Ce‐Ov‐Cu) with different charge distributions can effectuate coupling reaction through stabilization key * COCO intermediates, thus making reduction become more favorable process. Accordingly, optimized O/CF demonstrates remarkable performance 93% selectivity toward generation impressive production rate 26.1 µmol g −1 h . Such strongly coupled heterogeneous catalysts finely tailored structure interaction, containing polarized metal at interface, will provide some inspiration constructing efficient photocatalysts convert high value‐added multi‐carbon products solar energy.

Language: Английский

Strategies for Enhancing Stability in Electrochemical CO₂ Reduction

Chemistry - An Asian Journal, Journal Year: 2025, Volume and Issue: unknown

Published: April 9, 2025

Abstract The electrochemical CO 2 reduction reaction (CO RR) holds significant promise as a sustainable approach to address global energy challenges and reduce carbon emissions. However, achieving long‐term stability in terms of catalytic performance remains critical hurdle for large‐scale commercial deployment. This mini‐review provides comprehensive exploration the key factors influencing RR stability, encompassing catalyst design, electrode architecture, electrolyzer optimization, operational conditions. We examine how degradation occurs through mechanisms such valence changes, elemental dissolution, structural reconfiguration, active site poisoning propose targeted strategies improvement, including doping, alloying, substrate engineering. Additionally, advancements modifications membrane enhancements, are highlighted their role improving stability. Operational parameters temperature, pressure, electrolyte composition also play crucial roles extending lifespan reaction. By addressing these diverse factors, this review aims offer deeper understanding determinants RR, laying groundwork development robust, scalable technologies efficient dioxide conversion.

Language: Английский

Asymmetric CO–CHO Coupling over Pr Single-Atom Alloy Enables Industrial-Level Electrosynthesis of Ethylene

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: April 24, 2025

The electrocatalytic conversion of carbon dioxide (CO2) to ethylene (C2H4) holds great promise for sustainable chemical synthesis, yet achieving industrially relevant production rates remains a significant challenge. Through computational screening, we have identified praseodymium (Pr) single-atom alloy embedded in copper (Cu) catalyst (Pr@Cu) that exhibits superior CO2 activation and remarkably low energy barrier asymmetric *CO-*CHO coupling, primarily by facilitating the *CHO intermediate formation. Our optimized catalyst, Pr@Cu-2 (6 wt % Pr), achieves C2H4 Faradaic efficiency (FE) 64.2% at -1.6 V versus reversible hydrogen electrode (RHE) under high current density 1200 mA cm-2 reduction reaction (CO2RR). Furthermore, when integrated into 100 cm2 membrane assembly (MEA) electrolyzer, demonstrates robust performance, maintaining continuous rate 21.3 mL min-1 20 A over 200 h. This work provides fundamental insights role Pr alloys CO2RR highlights their potential scalable electrosynthesis.

Language: Английский