Copper-Rich PdxCu1–xAlloy Nanoparticles as Catalyst for Electrochemical Reduction of CO2

Andreas Dueholm Bertelsen; Rebekka Klemmt; Kirstine Nygaard Kolding; Espen Drath Bøjesen; Bo Brummerstedt Iversen

doi:10.1021/acs.chemmater.5c01148

Copper-Rich Pd_xCu_1–xAlloy Nanoparticles as Catalyst for Electrochemical Reduction of CO₂

^*Corresponding author for this work

Research output: Contribution to journal/Conference contribution in journal/Contribution to newspaper › Journal article › Research › peer-review

Abstract

Copper is uniquely able to catalyze the formation of hydrocarbon-derived molecules through the electrochemical carbon dioxide reduction reaction (CO₂RR) in aqueous media. Here, we investigate the change of selectivity and/or activity in CO₂RR by alloying Cu with palladium by using Pd_xCu_1–xnanoparticles as electrocatalysts. In situ powder X-ray diffraction reveals a much lowered reduction temperature of the Cu-precursor upon alloying and establishes the importance of high heating rates during synthesis to ensure homogeneous Pd alloying into copper-rich Pd_xCu_1–xnanoparticles. Two different synthetic approaches were used to obtain Pd_xCu_1–xnanoparticles with a composition range of x = 0.025–0.20, and the complex nanostructures of the particles were highlighted using four-dimensional Scanning Transmission Electron Microscopy (4D-STEM). The activity and selectivity toward electrochemical CO₂RR in 0.1 M KHCO₃were assessed for increasing Pd contents, and a systematic decrease in faradaic efficiency toward hydrocarbon products was found coupled with an increase in faradaic efficiency toward primarily H₂. The results do not support Pd_xCu_1–xalloying as a viable method for increasing selectivity toward specific hydrocarbon products in electrochemical CO₂RR.

Original language	English
Journal	Chemistry of Materials
Volume	37
Issue	17
Pages (from-to)	6619-6628
Number of pages	10
ISSN	0897-4756
DOIs	https://doi.org/10.1021/acs.chemmater.5c01148
Publication status	Published - 9 Sept 2025

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@article{740168df1a614f0bad0a48cdb4be6363,

title = "Copper-Rich PdxCu1–xAlloy Nanoparticles as Catalyst for Electrochemical Reduction of CO2",

abstract = "Copper is uniquely able to catalyze the formation of hydrocarbon-derived molecules through the electrochemical carbon dioxide reduction reaction (CO2RR) in aqueous media. Here, we investigate the change of selectivity and/or activity in CO2RR by alloying Cu with palladium by using PdxCu1–xnanoparticles as electrocatalysts. In situ powder X-ray diffraction reveals a much lowered reduction temperature of the Cu-precursor upon alloying and establishes the importance of high heating rates during synthesis to ensure homogeneous Pd alloying into copper-rich PdxCu1–xnanoparticles. Two different synthetic approaches were used to obtain PdxCu1–xnanoparticles with a composition range of x = 0.025–0.20, and the complex nanostructures of the particles were highlighted using four-dimensional Scanning Transmission Electron Microscopy (4D-STEM). The activity and selectivity toward electrochemical CO2RR in 0.1 M KHCO3were assessed for increasing Pd contents, and a systematic decrease in faradaic efficiency toward hydrocarbon products was found coupled with an increase in faradaic efficiency toward primarily H2. The results do not support PdxCu1–xalloying as a viable method for increasing selectivity toward specific hydrocarbon products in electrochemical CO2RR.",

author = "Bertelsen, \{Andreas Dueholm\} and Rebekka Klemmt and Kolding, \{Kirstine Nygaard\} and B{\o}jesen, \{Espen Drath\} and Iversen, \{Bo Brummerstedt\}",

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doi = "10.1021/acs.chemmater.5c01148",

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Copper-Rich Pd_xCu_1–xAlloy Nanoparticles as Catalyst for Electrochemical Reduction of CO₂. / Bertelsen, Andreas Dueholm ; Klemmt, Rebekka ; Kolding, Kirstine Nygaard et al.
In: Chemistry of Materials, Vol. 37, No. 17, 09.09.2025, p. 6619-6628.

Research output: Contribution to journal/Conference contribution in journal/Contribution to newspaper › Journal article › Research › peer-review

TY - JOUR

T1 - Copper-Rich PdxCu1–xAlloy Nanoparticles as Catalyst for Electrochemical Reduction of CO2

AU - Bertelsen, Andreas Dueholm

AU - Klemmt, Rebekka

AU - Kolding, Kirstine Nygaard

AU - Bøjesen, Espen Drath

AU - Iversen, Bo Brummerstedt

PY - 2025/9/9

Y1 - 2025/9/9

N2 - Copper is uniquely able to catalyze the formation of hydrocarbon-derived molecules through the electrochemical carbon dioxide reduction reaction (CO2RR) in aqueous media. Here, we investigate the change of selectivity and/or activity in CO2RR by alloying Cu with palladium by using PdxCu1–xnanoparticles as electrocatalysts. In situ powder X-ray diffraction reveals a much lowered reduction temperature of the Cu-precursor upon alloying and establishes the importance of high heating rates during synthesis to ensure homogeneous Pd alloying into copper-rich PdxCu1–xnanoparticles. Two different synthetic approaches were used to obtain PdxCu1–xnanoparticles with a composition range of x = 0.025–0.20, and the complex nanostructures of the particles were highlighted using four-dimensional Scanning Transmission Electron Microscopy (4D-STEM). The activity and selectivity toward electrochemical CO2RR in 0.1 M KHCO3were assessed for increasing Pd contents, and a systematic decrease in faradaic efficiency toward hydrocarbon products was found coupled with an increase in faradaic efficiency toward primarily H2. The results do not support PdxCu1–xalloying as a viable method for increasing selectivity toward specific hydrocarbon products in electrochemical CO2RR.

AB - Copper is uniquely able to catalyze the formation of hydrocarbon-derived molecules through the electrochemical carbon dioxide reduction reaction (CO2RR) in aqueous media. Here, we investigate the change of selectivity and/or activity in CO2RR by alloying Cu with palladium by using PdxCu1–xnanoparticles as electrocatalysts. In situ powder X-ray diffraction reveals a much lowered reduction temperature of the Cu-precursor upon alloying and establishes the importance of high heating rates during synthesis to ensure homogeneous Pd alloying into copper-rich PdxCu1–xnanoparticles. Two different synthetic approaches were used to obtain PdxCu1–xnanoparticles with a composition range of x = 0.025–0.20, and the complex nanostructures of the particles were highlighted using four-dimensional Scanning Transmission Electron Microscopy (4D-STEM). The activity and selectivity toward electrochemical CO2RR in 0.1 M KHCO3were assessed for increasing Pd contents, and a systematic decrease in faradaic efficiency toward hydrocarbon products was found coupled with an increase in faradaic efficiency toward primarily H2. The results do not support PdxCu1–xalloying as a viable method for increasing selectivity toward specific hydrocarbon products in electrochemical CO2RR.

UR - https://www.scopus.com/pages/publications/105015512801

U2 - 10.1021/acs.chemmater.5c01148

DO - 10.1021/acs.chemmater.5c01148

M3 - Journal article

AN - SCOPUS:105015512801

SN - 0897-4756

VL - 37

SP - 6619

EP - 6628

JO - Chemistry of Materials

JF - Chemistry of Materials

IS - 17

ER -

Copper-Rich Pd_xCu_1–xAlloy Nanoparticles as Catalyst for Electrochemical Reduction of CO₂

Abstract

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