Tuning Electrochemical CO₂ Reduction through Variation in Composition of the Cu–Pd Bimetallic Catalyst: Experimental and Theoretical Investigations
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1.
North Carolina Agricultural and Technical State University
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2.
California Institute of Technology
Abstract
In the context of global warming, electrochemical reduction of CO2 (eCO2RR) offers a promising route to achieve net-zero carbon emissions by producing value-added products. This study investigates copper-palladium (Cu-Pd) bimetallic catalysts for the eCO2RR, focusing on product distribution by varying catalyst composition. Cu-Pd catalysts were synthesized and characterized for crystallinity, structure, texture, and morphology. Reactions conducted with Cu-Pd molar ratios (1:1, 2:1, 1:2, 3:1) at -0.6 to -1.6 V vs RHE for 1 h yielded diverse products. A 1:1 Cu-Pd ratio achieved 91% Faradaic efficiency (FE) for formate at -1.6 V, while 2:1 and 1:2 ratios produced acetate with FEs of 58% and 35% at -1.4 V. A 3:1 ratio led to methanol with 38% FE at -1.6 V. XPS analysis revealed the metal oxide/metal interface suppressed hydrogen evolution while facilitating reaction intermediates. Quantum mechanical calculations corroborated experimental results, highlighting potential-dependent product selectivity.
Acknowledgement
The authors of this work gratefully acknowledge the funding received from DOE-BES (Award Number: DE SC0022230) and NSF-SENIC (Award Number: ECCS-2025462). We are thankful to The University of North Carolina at Chapel Hill for performing the FETEM studies.
Supplemental Material
The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpclett.4c03408.
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Materials, methods, and experimental setup; CuPd phase diagram; Cu–Pd 1:1 and 3:1 slab from DFT; Analytical characterization of Cu–Pd nanoparticles; CV and chronoamperometry of Cu–Pd electrodes; 1H NMR spectra of the catholytes; FE of products (PDF)
Copyright and License
Copyright © 2025 American Chemical Society
Contributions
SG and DM contributed equally.
Conflict of Interest
The authors declare no competing financial interest.
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Additional details
Funding
- Office of Basic Energy Sciences
- DE-SC0022230
- Division of Electrical, Communications & Cyber Systems
- ECCS-2025462
Dates
- Available
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2025-02-17Published online