Palladium-enhanced copper nitride anti-perovskite nanocrystals boosting CO2 electroreduction to C2 products

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Palladium-enhanced copper nitride anti-perovskite nanocrystals boosting CO2 electroreduction to C2 products

Year : 2025

Publisher : Elsevier B.V.

Source Title : Chemical Engineering Journal

Document Type :

Abstract

Addressing the dual challenges of energy sustainability and climate change, carbon dioxide electrochemical reduction (CO2 ECR) emerges as a promising technology for converting CO2 into valuable hydrocarbons. This study presents a palladium-enhanced copper nitride (Cu3N) catalyst that significantly boosts the efficiency of CO2 ECR towards multicarbon (C2+) products with only 0.3 % Pd loading. By leveraging the structural stability of anti-perovskite Cu3N, known for its ability to accommodate dopants, we hypothesized that doping in anti-perovskite Cu3N would modulate its electronic structure and improve catalytic activity. Guided by tolerance factor analysis for anti-perovskite Cu3N, we incorporated Pd into anti-perovskite Cu3N in varying amounts to modulate intermediate adsorption during the CO2 ECR reaction. Characterization of the synthesized nanocrystals by transmission electron microscopy and X-ray diffraction confirmed the uniform incorporation of palladium and the preservation of the Cu3N structure. Electrochemical tests and density functional theory (DFT) calculations demonstrated that palladium doping significantly shifts the selectivity towards ethylene and ethanol, with a notable increase in the faradaic efficiency for C2 products at low palladium loadings. These findings underscore the potential of palladium-enhanced Cu3N nanocrystals as a superior catalyst for the sustainable production of high-value chemicals and fuels from CO2. This study not only elucidates the impact of bimetallic interactions in CO2 electroreduction but also showcases the precise control over product selectivity offered by strategically doped electrocatalysts.