Gardner, Adrian M 
ORCID: 0000-0002-2423-8799, Neri, Gaia, Siritanaratkul, Bhavin ORCID: 0000-0003-0604-7670, Jang, Hansaem ORCID: 0000-0002-1056-9853, Saeed, Khezar H ORCID: 0000-0001-7207-9836, Donaldson, Paul M ORCID: 0000-0002-0305-9142 and Cowan, Alexander J ORCID: 0000-0001-9032-3548
(2024)
Potential Dependent Reorientation Controlling Activity of a Molecular Electrocatalyst.
Journal of the American Chemical Society, 146 (11).
pp. 7130-7134.
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Abstract
The activity of molecular electrocatalysts depends on the interplay of electrolyte composition near the electrode surface, the composition and morphology of the electrode surface, and the electric field at the electrode-electrolyte interface. This interplay is challenging to study and often overlooked when assessing molecular catalyst activity. Here, we use surface specific vibrational sum frequency generation (VSFG) spectroscopy to study the solvent and potential dependent activation of Mo(bpy)(CO)<sub>4</sub>, a CO<sub>2</sub> reduction catalyst, at a polycrystalline Au electrode. We find that the parent complex undergoes potential dependent reorientation at the electrode surface when a small amount of <i>N</i>-methyl-2-pyrrolidone (NMP) is present. This preactivates the complex, resulting in greater yields at less negative potentials, of the active electrocatalyst for CO<sub>2</sub> reduction.
| Item Type: | Article |
|---|---|
| Divisions: | Faculty of Science and Engineering > School of Physical Sciences |
| Depositing User: | Symplectic Admin |
| Date Deposited: | 06 Mar 2024 09:11 |
| Last Modified: | 04 Apr 2024 06:04 |
| DOI: | 10.1021/jacs.3c13076 |
| Related URLs: | |
| URI: | https://livrepository.liverpool.ac.uk/id/eprint/3179137 |
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