Impact of palladium/palladium hydride conversion on electrochemical CO2 reduction via in-situ transmission electron microscopy and diffraction

Ahmed M. Abdellah, Fatma Ismail, Oliver W. Siig, Jie Yang, Carmen M. Andrei, Liza-Anastasia DiCecco, Amirhossein Rakhsha, Kholoud E. Salem, Kathryn Grandfield, Nabil Bassim, Robert Black, Georg Kastlunger (), Leyla Soleymani and Drew Higgins ()
Additional contact information
Ahmed M. Abdellah: McMaster University
Fatma Ismail: McMaster University
Oliver W. Siig: Technical University of Denmark
Jie Yang: McMaster University
Carmen M. Andrei: McMaster University
Liza-Anastasia DiCecco: McMaster University
Amirhossein Rakhsha: McMaster University
Kholoud E. Salem: McMaster University
Kathryn Grandfield: McMaster University
Nabil Bassim: McMaster University
Robert Black: Energy, Mining, and Environment Research Centre
Georg Kastlunger: Technical University of Denmark
Leyla Soleymani: McMaster University
Drew Higgins: McMaster University

Nature Communications, 2024, vol. 15, issue 1, 1-15

Abstract: Abstract Electrochemical conversion of CO2 offers a sustainable route for producing fuels and chemicals. Pd-based catalysts are effective for converting CO2 into formate at low overpotentials and CO/H2 at high overpotentials, while undergoing poorly understood morphology and phase structure transformations under reaction conditions that impact performance. Herein, in-situ liquid-phase transmission electron microscopy and select area diffraction measurements are applied to track the morphology and Pd/PdHx phase interconversion under reaction conditions as a function of electrode potential. These studies identify the degradation mechanisms, including poisoning and physical structure changes, occurring in PdHx/Pd electrodes. Constant potential density functional theory calculations are used to probe the reaction mechanisms occurring on the PdHx structures observed under reaction conditions. Microkinetic modeling reveals that the intercalation of *H into Pd is essential for formate production. However, the change in electrochemical CO2 conversion selectivity away from formate and towards CO/H2 at increasing overpotentials is due to electrode potential dependent changes in the reaction energetics and not a consequence of morphology or phase structure changes.

Date: 2024
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DOI: 10.1038/s41467-024-45096-3

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