Potential Dependent Reorientation Controlling Activity of a Molecular Electrocatalyst

Gardner, Adrian M ORCID: 0000-0002-2423-8799, Neri, Gaia, Siritanaratkul, Bhavin ORCID: 0000-0003-0604-7670, Jang, Hansaem, Saeed, Khezar H, Donaldson, Paul M 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. ISSN 0002-7863, 1520-5126

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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)<inf>4</inf>, a CO<inf>2</inf> 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 N-methyl-2-pyrrolidone (NMP) is present. This preactivates the complex, resulting in greater yields at less negative potentials, of the active electrocatalyst for CO<inf>2</inf> reduction.

Item Type:	Article
Uncontrolled Keywords:	34 Chemical Sciences, 3406 Physical Chemistry
Divisions:	Faculty of Science & Engineering > School of Physical Sciences
Depositing User:	Symplectic Admin
Date Deposited:	06 Mar 2024 09:11
Last Modified:	16 Jun 2026 20:05
DOI:	10.1021/jacs.3c13076
Related Websites:	Author Publisher
URI:	https://livrepository.liverpool.ac.uk/id/eprint/3179137
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