| Download | - View final version: Impact of palladium/palladium hydride conversion on electrochemical CO₂ reduction via in-situ transmission electron microscopy and diffraction (PDF, 2.4 MiB)
- View supplementary information part 1: Impact of palladium/palladium hydride conversion on electrochemical CO₂ reduction via in-situ transmission electron microscopy and diffraction (PDF, 2.7 MiB)
- View supplementary information part 2: Impact of palladium/palladium hydride conversion on electrochemical CO₂ reduction via in-situ transmission electron microscopy and diffraction (PDF, 114 KiB)
- View supplementary information part 3: Impact of palladium/palladium hydride conversion on electrochemical CO₂ reduction via in-situ transmission electron microscopy and diffraction (PDF, 4.1 MiB)
|
|---|
| DOI | Resolve DOI: https://doi.org/10.1038/s41467-024-45096-3 |
|---|
| Author | Search for: Abdellah, Ahmed M.; Search for: Ismail, Fatma; Search for: Siig, Oliver W.ORCID identifier: https://orcid.org/0000-0003-4661-4721; Search for: Yang, Jie; Search for: Andrei, Carmen M.; Search for: DiCecco, Liza-Anastasia; Search for: Rakhsha, Amirhossein; Search for: Salem, Kholoud E.; Search for: Grandfield, KathrynORCID identifier: https://orcid.org/0000-0002-0188-9580; Search for: Bassim, NabilORCID identifier: https://orcid.org/0000-0002-9161-5769; Search for: Black, Robert1; Search for: Kastlunger, GeorgORCID identifier: https://orcid.org/0000-0002-3767-8734; Search for: Soleymani, LeylaORCID identifier: https://orcid.org/0000-0003-4915-2999; Search for: Higgins, DrewORCID identifier: https://orcid.org/0000-0002-0585-2670 |
|---|
| Affiliation | - National Research Council of Canada. Clean Energy Innovation
|
|---|
| Format | Text, Article |
|---|
| 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. |
|---|
| Publication date | 2023-01-31 |
|---|
| Publisher | Nature Research |
|---|
| Licence | |
|---|
| In | |
|---|
| Note | Supplementary videos available on publisher's website |
|---|
| Language | English |
|---|
| Peer reviewed | Yes |
|---|
| Export citation | Export as RIS |
|---|
| Report a correction | Report a correction (opens in a new tab) |
|---|
| Record identifier | 8e21e3a0-8a5d-412d-8bac-0cb07f5caca9 |
|---|
| Record created | 2024-04-11 |
|---|
| Record modified | 2024-04-17 |
|---|
