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

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

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