Establishing Active Cu+–O–Mg2+ Sites at the Cu2O/CuO Interface for Efficient Electroreduction of CO2 to C2+ Products DOI

Qinyuan Ji,

Hu Zang,

Changjiang Liu

et al.

ACS Materials Letters, Journal Year: 2024, Volume and Issue: 7(1), P. 333 - 342

Published: Dec. 20, 2024

Cu-based materials are regarded as effective electrocatalysts for CO2RR; however, Cu+, the active site C–C coupling, is unstable under reduction conditions. Herein, Mg2+ doped into Cu2O/CuO interface and generates high-activity Cu+–O-Mg2+ sites following electrochemical activation. The electron-withdrawing effect of in stabilizes Cu+ optimizes reaction pathway CO2RR. At a partial current density 567.21 ± 5.18 mA cm–2, Faraday efficiency (FE) C2+ products can reach 81.03 0.74%. In situ Raman infrared spectroscopy reveal that significantly enhances coverage stability *CO, which contributes to ultrahigh selectivity CO2 toward products. Density functional theory (DFT) studies indicate *CO2 readily adsorbed on site, facilitating more generation subsequently promotes coupling step accelerates production

Language: Английский

Direct Electrochemical Reduction of CO2 to C2+ Chemicals: Catalysts, Microenvironments, and Mechanistic Understanding DOI
Shichen Guo, J. Wang, Haozhe Zhang

et al.

ACS Energy Letters, Journal Year: 2025, Volume and Issue: 10(1), P. 600 - 619

Published: Jan. 2, 2025

The electrochemical reduction reaction of CO2 (eCO2RR) to chemicals presents a viable solution for addressing climate change and sustainable manufacturing. In this Review, we describe the recent advancements in eCO2RR multicarbon (C2+) production from aspects catalyst structure, microenvironments, mechanistic understanding. We draw experimental theoretical comparisons between systems containing bulk highly dispersed metals, alloys, metal compounds recount new results microenvironmental impacts as well catalytic mechanism. From our own studies, offer some viewpoints on electrocatalytic mechanism during complex multistep proton-coupled electron transfers propose several research directions unlocking full potential scalable industrial CO2-to-C2+ conversion.

Language: Английский

Citations

2
Unraveling the enhanced urea selectivity in electroreduction of CO2 and nitrate over Bimetallic CuZn catalysts DOI
Bo Lv,

Jian Yu,

Fengchen Zhou

et al.

Molecular Catalysis, Journal Year: 2025, Volume and Issue: 578, P. 114978 - 114978

Published: March 6, 2025

Language: Английский

Citations

1
Hierarchical Cavity Cu Nanostructures with Coordinative Microenvironment Engineering for pH‐Universal Electrocatalytic CO2‐to‐C2+ Conversion DOI Open Access

Hu Zang,

Yujie Zhao, Changjiang Liu

et al.

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

Citations

0
Phase engineering Governing reaction pathways in Phosphorus-Doped copper oxide for selective CO2 electroreduction to CH4 and Multicarbon products DOI
Haiyan Lu,

Hu Zang,

Changjiang Liu

et al.

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 162269 - 162269

Published: April 1, 2025

Language: Английский

Citations

0
Establishing Active Cu+–O–Mg2+ Sites at the Cu2O/CuO Interface for Efficient Electroreduction of CO2 to C2+ Products DOI

Qinyuan Ji,

Hu Zang,

Changjiang Liu

et al.

ACS Materials Letters, Journal Year: 2024, Volume and Issue: 7(1), P. 333 - 342

Published: Dec. 20, 2024

Cu-based materials are regarded as effective electrocatalysts for CO2RR; however, Cu+, the active site C–C coupling, is unstable under reduction conditions. Herein, Mg2+ doped into Cu2O/CuO interface and generates high-activity Cu+–O-Mg2+ sites following electrochemical activation. The electron-withdrawing effect of in stabilizes Cu+ optimizes reaction pathway CO2RR. At a partial current density 567.21 ± 5.18 mA cm–2, Faraday efficiency (FE) C2+ products can reach 81.03 0.74%. In situ Raman infrared spectroscopy reveal that significantly enhances coverage stability *CO, which contributes to ultrahigh selectivity CO2 toward products. Density functional theory (DFT) studies indicate *CO2 readily adsorbed on site, facilitating more generation subsequently promotes coupling step accelerates production

Language: Английский

Citations

2