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Constructing Cu/Cu2O Heterogeneous Interface for Efficient Urea Electrosynthesis
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DOI：10.1002/eem2.70235.png)
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Abstract
En 中文
Electrocatalytic coupling of CO2 and enables urea synthesis under mild conditions while simultaneously converting greenhouse gases/pollutants, yet suffers from sluggish C-N coupling kinetics and low efficiency. To address this, a novel Cu/Cu2O catalyst with a high-density heterogeneous interface and 3D crosslinking network structure was constructed. The high-angle annular dark-field scanning transmission electron microscope reveals the Cu/Cu2O heterogeneous interface at the atomic scale, showing a distinct contrast discontinuity that defines the metal/metal oxides phase boundary. This unique structure exposes a large number of dual active sites. In-situ attenuated total reflection-surface enhanced infrared absorption spectroscopy and density functional theory calculations revealed a space-separated activation mechanism induced by the dual active sites at the heterogeneous interfaces. The electron-deficient Cu site preferentially activates CO2 to produce *CO, while the electron-rich Cu2O site dominates reduction to form *NOH intermediates. The built-in electric field formed at the heterogeneous interface further promotes the efficient C-N coupling of *CO and *NOH, significantly reducing the reaction energy barrier. Electrochemical tests showed Cu/Cu2O outperformed Cu and Cu2O in electrocatalytic coupling of CO2 and for urea synthesis, achieving a record urea yield rate of 1156.63 mmol g-1 h-1 with 29.67% Faradaic efficiency at -1.0 V (vs RHE).
Keywords:
C-N coupling
Cu-based electrocatalysts
electrocatalysis
interfacial engineering
urea synthesis
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E
IF:
14.1
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